Articles | Volume 14, issue 3
https://doi.org/10.5194/acp-14-1689-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-14-1689-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
14 Feb 2014
Research article |
| 14 Feb 2014
The role of low volatile organics on secondary organic aerosol formation
H. Kokkola
Finnish Meteorological Institute, P.O. Box 1627, 70211, Kuopio, Finland
P. Yli-Pirilä
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
M. Vesterinen
Finnish Meteorological Institute, P.O. Box 1627, 70211, Kuopio, Finland
H. Korhonen
Finnish Meteorological Institute, P.O. Box 503, 00101, Helsinki, Finland
H. Keskinen
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
S. Romakkaniemi
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
L. Hao
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
A. Kortelainen
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
J. Joutsensaari
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
D. R. Worsnop
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
Aerodyne Research Inc., Billerica, MA 01821-3976, USA
A. Virtanen
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
K. E. J. Lehtinen
Finnish Meteorological Institute, P.O. Box 1627, 70211, Kuopio, Finland
University of Eastern Finland, P.O. Box 1627, 70211, Kuopio, Finland
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Silvia M. Calderón, Juha Tonttila, Angela Buchholz, Jorma Joutsensaari, Mika Komppula, Ari Leskinen, Liqing Hao, Dmitri Moisseev, Iida Pullinen, Petri Tiitta, Jian Xu, Annele Virtanen, Harri Kokkola, and Sami Romakkaniemi
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Sini Isokääntä, Paul Kim, Santtu Mikkonen, Thomas Kühn, Harri Kokkola, Taina Yli-Juuti, Liine Heikkinen, Krista Luoma, Tuukka Petäjä, Zak Kipling, Daniel Partridge, and Annele Virtanen
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Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Marje Prank, Juha Tonttila, Jaakko Ahola, Harri Kokkola, Thomas Kühn, Sami Romakkaniemi, and Tomi Raatikainen
Atmos. Chem. Phys., 22, 10971–10992, https://doi.org/10.5194/acp-22-10971-2022, https://doi.org/10.5194/acp-22-10971-2022, 2022
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Aerosols and clouds persist as the dominant sources of uncertainty in climate projections. In this modelling study, we investigate the role of marine aerosols in influencing the lifetime of low-level clouds. Our high resolution simulations show that sea spray can both extend and shorten the lifetime of the cloud layer depending on the model setup. The impact of the primary marine organics is relatively limited while secondary aerosol from monoterpenes can have larger impact.
Jaakko Ahola, Tomi Raatikainen, Muzaffer Ege Alper, Jukka-Pekka Keskinen, Harri Kokkola, Antti Kukkurainen, Antti Lipponen, Jia Liu, Kalle Nordling, Antti-Ilari Partanen, Sami Romakkaniemi, Petri Räisänen, Juha Tonttila, and Hannele Korhonen
Atmos. Chem. Phys., 22, 4523–4537, https://doi.org/10.5194/acp-22-4523-2022, https://doi.org/10.5194/acp-22-4523-2022, 2022
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Tomi Raatikainen, Marje Prank, Jaakko Ahola, Harri Kokkola, Juha Tonttila, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 3763–3778, https://doi.org/10.5194/acp-22-3763-2022, https://doi.org/10.5194/acp-22-3763-2022, 2022
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Atmos. Chem. Phys., 22, 93–118, https://doi.org/10.5194/acp-22-93-2022, https://doi.org/10.5194/acp-22-93-2022, 2022
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Maria Sand, Bjørn H. Samset, Gunnar Myhre, Jonas Gliß, Susanne E. Bauer, Huisheng Bian, Mian Chin, Ramiro Checa-Garcia, Paul Ginoux, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Philippe Le Sager, Marianne T. Lund, Hitoshi Matsui, Twan van Noije, Dirk J. L. Olivié, Samuel Remy, Michael Schulz, Philip Stier, Camilla W. Stjern, Toshihiko Takemura, Kostas Tsigaridis, Svetlana G. Tsyro, and Duncan Watson-Parris
Atmos. Chem. Phys., 21, 15929–15947, https://doi.org/10.5194/acp-21-15929-2021, https://doi.org/10.5194/acp-21-15929-2021, 2021
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Absorption of shortwave radiation by aerosols can modify precipitation and clouds but is poorly constrained in models. A total of 15 different aerosol models from AeroCom phase III have reported total aerosol absorption, and for the first time, 11 of these models have reported in a consistent experiment the contributions to absorption from black carbon, dust, and organic aerosol. Here, we document the model diversity in aerosol absorption.
Antti Ruuskanen, Sami Romakkaniemi, Harri Kokkola, Antti Arola, Santtu Mikkonen, Harri Portin, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, and Ari Leskinen
Atmos. Chem. Phys., 21, 1683–1695, https://doi.org/10.5194/acp-21-1683-2021, https://doi.org/10.5194/acp-21-1683-2021, 2021
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The study focuses mainly on cloud-scavenging efficiency of absorbing particulate matter (mainly black carbon) but additionally covers cloud-scavenging efficiency of scattering particles and statistics of cloud condensation nuclei. The main findings give insight into how black carbon is distributed in different particle sizes and the sensitivity to cloud scavenged. The main findings are useful for large-scale modelling for evaluating cloud scavenging.
Juha Tonttila, Ali Afzalifar, Harri Kokkola, Tomi Raatikainen, Hannele Korhonen, and Sami Romakkaniemi
Atmos. Chem. Phys., 21, 1035–1048, https://doi.org/10.5194/acp-21-1035-2021, https://doi.org/10.5194/acp-21-1035-2021, 2021
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The focus of this study is on rain enhancement by deliberate injection of small particles into clouds (
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Jonas Gliß, Augustin Mortier, Michael Schulz, Elisabeth Andrews, Yves Balkanski, Susanne E. Bauer, Anna M. K. Benedictow, Huisheng Bian, Ramiro Checa-Garcia, Mian Chin, Paul Ginoux, Jan J. Griesfeller, Andreas Heckel, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Paolo Laj, Philippe Le Sager, Marianne Tronstad Lund, Cathrine Lund Myhre, Hitoshi Matsui, Gunnar Myhre, David Neubauer, Twan van Noije, Peter North, Dirk J. L. Olivié, Samuel Rémy, Larisa Sogacheva, Toshihiko Takemura, Kostas Tsigaridis, and Svetlana G. Tsyro
Atmos. Chem. Phys., 21, 87–128, https://doi.org/10.5194/acp-21-87-2021, https://doi.org/10.5194/acp-21-87-2021, 2021
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Simulated aerosol optical properties as well as the aerosol life cycle are investigated for 14 global models participating in the AeroCom initiative. Considerable diversity is found in the simulated aerosol species emissions and lifetimes, also resulting in a large diversity in the simulated aerosol mass, composition, and optical properties. A comparison with observations suggests that, on average, current models underestimate the direct effect of aerosol on the atmosphere radiation budget.
Eemeli Holopainen, Harri Kokkola, Anton Laakso, and Thomas Kühn
Geosci. Model Dev., 13, 6215–6235, https://doi.org/10.5194/gmd-13-6215-2020, https://doi.org/10.5194/gmd-13-6215-2020, 2020
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This paper introduces an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol–climate models. With the default setup, our wet deposition scheme behaves spuriously and better representation can be achieved with this scheme when black carbon is mixed with soluble compounds at emission time. This work is done as many of the global models fail to reproduce the transport of black carbon to the Arctic, which may be due to the poor representation of wet removal in models.
Jaakko Ahola, Hannele Korhonen, Juha Tonttila, Sami Romakkaniemi, Harri Kokkola, and Tomi Raatikainen
Atmos. Chem. Phys., 20, 11639–11654, https://doi.org/10.5194/acp-20-11639-2020, https://doi.org/10.5194/acp-20-11639-2020, 2020
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In this study, we present an improved cloud model that reproduces the behaviour of mixed-phase clouds containing liquid droplets and ice crystals in more detail than before. This model is a convenient computational tool that enables the study of phenomena that cannot fit into a laboratory. These clouds have a significant role in climate, but they are not yet properly understood. Here, we show the advantages of the new model in a case study focusing on Arctic mixed-phase clouds.
Innocent Kudzotsa, Harri Kokkola, Juha Tonttila, Tomi Raatikainen, and Sami Romakkaniemi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-851, https://doi.org/10.5194/acp-2020-851, 2020
Publication in ACP not foreseen
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
Thomas Kühn, Kaarle Kupiainen, Tuuli Miinalainen, Harri Kokkola, Ville-Veikko Paunu, Anton Laakso, Juha Tonttila, Rita Van Dingenen, Kati Kulovesi, Niko Karvosenoja, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 20, 5527–5546, https://doi.org/10.5194/acp-20-5527-2020, https://doi.org/10.5194/acp-20-5527-2020, 2020
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We investigate the effects of black carbon (BC) mitigation on Arctic climate and human health, accounting for the concurrent reduction of other aerosol species. While BC is attributed a net warming effect on climate, most other aerosol species cool the planet. We find that the direct radiative effect of mitigating BC induces cooling, while aerosol–cloud effects offset this cooling and introduce large uncertainties. Furthermore, the reduced aerosol emissions reduce human mortality considerably.
Giulia Saponaro, Moa K. Sporre, David Neubauer, Harri Kokkola, Pekka Kolmonen, Larisa Sogacheva, Antti Arola, Gerrit de Leeuw, Inger H. H. Karset, Ari Laaksonen, and Ulrike Lohmann
Atmos. Chem. Phys., 20, 1607–1626, https://doi.org/10.5194/acp-20-1607-2020, https://doi.org/10.5194/acp-20-1607-2020, 2020
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The understanding of cloud processes is based on the quality of the representation of cloud properties. We compared cloud parameters from three models with satellite observations. We report on the performance of each data source, highlighting strengths and deficiencies, which should be considered when deriving the effect of aerosols on cloud properties.
David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Philip Stier, Daniel G. Partridge, Ina Tegen, Isabelle Bey, Tanja Stanelle, Harri Kokkola, and Ulrike Lohmann
Geosci. Model Dev., 12, 3609–3639, https://doi.org/10.5194/gmd-12-3609-2019, https://doi.org/10.5194/gmd-12-3609-2019, 2019
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The global aerosol–climate model ECHAM6.3–HAM2.3 as well as the previous model versions ECHAM5.5–HAM2.0 and ECHAM6.1–HAM2.2 are evaluated. The simulation of clouds has improved in ECHAM6.3–HAM2.3. This has an impact on effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions and equilibrium climate sensitivity, which are weaker in ECHAM6.3–HAM2.3 than in the previous model versions.
Ina Tegen, David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Isabelle Bey, Nick Schutgens, Philip Stier, Duncan Watson-Parris, Tanja Stanelle, Hauke Schmidt, Sebastian Rast, Harri Kokkola, Martin Schultz, Sabine Schroeder, Nikos Daskalakis, Stefan Barthel, Bernd Heinold, and Ulrike Lohmann
Geosci. Model Dev., 12, 1643–1677, https://doi.org/10.5194/gmd-12-1643-2019, https://doi.org/10.5194/gmd-12-1643-2019, 2019
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We describe a new version of the aerosol–climate model ECHAM–HAM and show tests of the model performance by comparing different aspects of the aerosol distribution with different datasets. The updated version of HAM contains improved descriptions of aerosol processes, including updated emission fields and cloud processes. While there are regional deviations between the model and observations, the model performs well overall.
Mona Kurppa, Antti Hellsten, Pontus Roldin, Harri Kokkola, Juha Tonttila, Mikko Auvinen, Christoph Kent, Prashant Kumar, Björn Maronga, and Leena Järvi
Geosci. Model Dev., 12, 1403–1422, https://doi.org/10.5194/gmd-12-1403-2019, https://doi.org/10.5194/gmd-12-1403-2019, 2019
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This paper describes the implementation of a sectional aerosol module, SALSA, into the PALM model system 6.0. The first evaluation study shows excellent agreements with measurements. Furthermore, we show that ignoring the dry deposition of aerosol particles can overestimate aerosol number concentrations by 20 %, whereas condensation and dissolutional growth increase the total aerosol mass by over 10 % in this specific urban environment.
Harri Kokkola, Thomas Kühn, Anton Laakso, Tommi Bergman, Kari E. J. Lehtinen, Tero Mielonen, Antti Arola, Scarlet Stadtler, Hannele Korhonen, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Ina Tegen, Colombe Siegenthaler-Le Drian, Martin G. Schultz, Isabelle Bey, Philip Stier, Nikos Daskalakis, Colette L. Heald, and Sami Romakkaniemi
Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, https://doi.org/10.5194/gmd-11-3833-2018, 2018
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In this paper we present a global aerosol–chemistry–climate model with the focus on its representation for atmospheric aerosol particles. In the model, aerosols are simulated using the aerosol module SALSA2.0, which in this paper is compared to satellite, ground, and aircraft-based observations of the properties of atmospheric aerosol. Based on this study, the model simulated aerosol properties compare well with the observations.
Scarlet Stadtler, Thomas Kühn, Sabine Schröder, Domenico Taraborrelli, Martin G. Schultz, and Harri Kokkola
Geosci. Model Dev., 11, 3235–3260, https://doi.org/10.5194/gmd-11-3235-2018, https://doi.org/10.5194/gmd-11-3235-2018, 2018
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Atmospheric aerosols interact with our climate system and have adverse health effects. Nevertheless, these particles are a source of uncertainty in climate projections and the formation process of secondary aerosols formed by organic gas-phase precursors is particularly not fully understood. In order to gain a deeper understanding of secondary organic aerosol formation, this model system explicitly represents gas-phase and aerosol formation processes. Finally, this allows for process discussion.
Ian Boutle, Jeremy Price, Innocent Kudzotsa, Harri Kokkola, and Sami Romakkaniemi
Atmos. Chem. Phys., 18, 7827–7840, https://doi.org/10.5194/acp-18-7827-2018, https://doi.org/10.5194/acp-18-7827-2018, 2018
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Aerosol processes are a key mechanism in the development of fog. Poor representation of aerosol–fog interaction can result in large biases in fog forecasts, such as surface temperatures which are too high and fog which is too deep and long lived. A relatively simple representation of aerosol–fog interaction can actually lead to significant improvements in forecasting. Aerosol–fog interaction can have a large effect on the climate system but is poorly represented in climate models.
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
Lukas Pichelstorfer, Dominik Stolzenburg, John Ortega, Thomas Karl, Harri Kokkola, Anton Laakso, Kari E. J. Lehtinen, James N. Smith, Peter H. McMurry, and Paul M. Winkler
Atmos. Chem. Phys., 18, 1307–1323, https://doi.org/10.5194/acp-18-1307-2018, https://doi.org/10.5194/acp-18-1307-2018, 2018
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Quantification of new particle formation as a source of atmospheric aerosol is clearly of importance for climate and health aspects. In our new study we developed two analysis methods that allow retrieval of nanoparticle growth dynamics at much higher precision than it was possible so far. Our results clearly demonstrate that growth rates show much more variation than is currently known and suggest that the Kelvin effect governs growth in the sub-10 nm size range.
Anton Laakso, Hannele Korhonen, Sami Romakkaniemi, and Harri Kokkola
Atmos. Chem. Phys., 17, 6957–6974, https://doi.org/10.5194/acp-17-6957-2017, https://doi.org/10.5194/acp-17-6957-2017, 2017
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Based on simulations, equatorial stratospheric sulfur injections have shown to be an efficient strategy to counteract ongoing global warming. However, equatorial injections would result in relatively larger cooling in low latitudes than in high latitudes. This together with greenhouse-gas-induced warming would lead to cooling in the Equator and warming in the high latitudes. Results of this study show that a more optimal cooling effect is achieved by varying the injection area seasonally.
Antti Arola, Thomas F. Eck, Harri Kokkola, Mikko R. A. Pitkänen, and Sami Romakkaniemi
Atmos. Chem. Phys., 17, 5991–6001, https://doi.org/10.5194/acp-17-5991-2017, https://doi.org/10.5194/acp-17-5991-2017, 2017
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One of the issues that hinder the measurement-based assessment of aerosol–cloud interactions by remote sensing methods is that typically aerosols and clouds cannot be measured simultaneously by passive remote sensing methods. AERONET includes the SDA product that provides the fine-mode AOD also in mixed cloud–aerosol observations. These measurements have not yet been fully exploited in studies of aerosol–cloud interactions. We applied SDA for this kind of analysis.
Juha Tonttila, Zubair Maalick, Tomi Raatikainen, Harri Kokkola, Thomas Kühn, and Sami Romakkaniemi
Geosci. Model Dev., 10, 169–188, https://doi.org/10.5194/gmd-10-169-2017, https://doi.org/10.5194/gmd-10-169-2017, 2017
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Novel techniques for modelling the aerosol–cloud interactions are implemented in a cloud-resolving model. The new methods improve the representation of the poorly constrained effects of cloud processing, precipitation and the wet removal of particles on the aerosol population and the associated feedbacks. The detailed representation of these processes yields more realistic simulation of the evolution of boundary layer clouds and fogs, as compared to results obtained using more simple methods.
Tero Mielonen, Anca Hienola, Thomas Kühn, Joonas Merikanto, Antti Lipponen, Tommi Bergman, Hannele Korhonen, Pekka Kolmonen, Larisa Sogacheva, Darren Ghent, Antti Arola, Gerrit de Leeuw, and Harri Kokkola
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-625, https://doi.org/10.5194/acp-2016-625, 2016
Revised manuscript not accepted
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We studied the temperature dependence of AOD and its radiative effects over the southeastern US. We used spaceborne observations of AOD, LST and tropospheric NO2 with simulations of ECHAM-HAMMOZ. The level of AOD in this region is governed by anthropogenic emissions but the temperature dependency is most likely caused by BVOC emissions. According to the observations and simulations, the regional clear-sky DRE for biogenic aerosols is −0.43 ± 0.88 W/m2/K and −0.86 ± 0.06 W/m2/K, respectively.
Jani Huttunen, Harri Kokkola, Tero Mielonen, Mika Esa Juhani Mononen, Antti Lipponen, Juha Reunanen, Anders Vilhelm Lindfors, Santtu Mikkonen, Kari Erkki Juhani Lehtinen, Natalia Kouremeti, Alkiviadis Bais, Harri Niska, and Antti Arola
Atmos. Chem. Phys., 16, 8181–8191, https://doi.org/10.5194/acp-16-8181-2016, https://doi.org/10.5194/acp-16-8181-2016, 2016
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For a good estimate of the current forcing by anthropogenic aerosols, knowledge in past is needed. One option to lengthen time series is to retrieve aerosol optical depth from solar radiation measurements. We have evaluated several methods for this task. Most of the methods produce aerosol optical depth estimates with a good accuracy. However, machine learning methods seem to be the most applicable not to produce any systematic biases, since they do not need constrain the aerosol properties.
N. I. Kristiansen, A. Stohl, D. J. L. Olivié, B. Croft, O. A. Søvde, H. Klein, T. Christoudias, D. Kunkel, S. J. Leadbetter, Y. H. Lee, K. Zhang, K. Tsigaridis, T. Bergman, N. Evangeliou, H. Wang, P.-L. Ma, R. C. Easter, P. J. Rasch, X. Liu, G. Pitari, G. Di Genova, S. Y. Zhao, Y. Balkanski, S. E. Bauer, G. S. Faluvegi, H. Kokkola, R. V. Martin, J. R. Pierce, M. Schulz, D. Shindell, H. Tost, and H. Zhang
Atmos. Chem. Phys., 16, 3525–3561, https://doi.org/10.5194/acp-16-3525-2016, https://doi.org/10.5194/acp-16-3525-2016, 2016
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Processes affecting aerosol removal from the atmosphere are not fully understood. In this study we investigate to what extent atmospheric transport models can reproduce observed loss of aerosols. We compare measurements of radioactive isotopes, that attached to ambient sulfate aerosols during the 2011 Fukushima nuclear accident, to 19 models using identical emissions. Results indicate aerosol removal that is too fast in most models, and apply to aerosols that have undergone long-range transport.
Zak Kipling, Philip Stier, Colin E. Johnson, Graham W. Mann, Nicolas Bellouin, Susanne E. Bauer, Tommi Bergman, Mian Chin, Thomas Diehl, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Harri Kokkola, Xiaohong Liu, Gan Luo, Twan van Noije, Kirsty J. Pringle, Knut von Salzen, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Toshihiko Takemura, Kostas Tsigaridis, and Kai Zhang
Atmos. Chem. Phys., 16, 2221–2241, https://doi.org/10.5194/acp-16-2221-2016, https://doi.org/10.5194/acp-16-2221-2016, 2016
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The vertical distribution of atmospheric aerosol is an important factor in its effects on climate. In this study we use a sophisticated model of the many interacting processes affecting aerosol in the atmosphere to show that the vertical distribution is typically dominated by only a few of these processes. Constraining these physical processes may help to reduce the large differences between models. However, the important processes are not always the same for different types of aerosol.
A. Laakso, H. Kokkola, A.-I. Partanen, U. Niemeier, C. Timmreck, K. E. J. Lehtinen, H. Hakkarainen, and H. Korhonen
Atmos. Chem. Phys., 16, 305–323, https://doi.org/10.5194/acp-16-305-2016, https://doi.org/10.5194/acp-16-305-2016, 2016
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We have studied the impacts of a volcanic eruption during solar radiation management (SRM) using an aerosol-climate model ECHAM5-HAM-SALSA and an Earth system model MPI-ESM. A volcanic eruption during stratospheric sulfur geoengineering would lead to larger particles and smaller amount of new particles than if an volcano erupts in normal atmospheric conditions. Thus, volcanic eruption during SRM would lead to only a small additional cooling which would last for a significantly shorter period.
A. Arola, G. L. Schuster, M. R. A. Pitkänen, O. Dubovik, H. Kokkola, A. V. Lindfors, T. Mielonen, T. Raatikainen, S. Romakkaniemi, S. N. Tripathi, and H. Lihavainen
Atmos. Chem. Phys., 15, 12731–12740, https://doi.org/10.5194/acp-15-12731-2015, https://doi.org/10.5194/acp-15-12731-2015, 2015
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There have been relatively few measurement-based estimates for the direct radiative effect of brown carbon so far. This is first time that the direct radiative effect of brown carbon is estimated by exploiting the AERONET-retrieved imaginary indices. We estimated it for four sites in the Indo-Gangetic Plain: Karachi, Lahore,
Kanpur and Gandhi College.
M. A. Thomas, M. Kahnert, C. Andersson, H. Kokkola, U. Hansson, C. Jones, J. Langner, and A. Devasthale
Geosci. Model Dev., 8, 1885–1898, https://doi.org/10.5194/gmd-8-1885-2015, https://doi.org/10.5194/gmd-8-1885-2015, 2015
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We have showed that a coupled modelling system is beneficial in the sense that more complex processes can be included to better represent the aerosol processes starting from their formation, their interactions with clouds and provide better estimate of radiative forcing. Using this model set up, we estimated an annual mean 'indirect' radiative forcing of -0.64W/m2. This means that aerosols, solely by their capability of altering the microphysical properties of clouds can cool the Earth system.
C. Andersson, R. Bergström, C. Bennet, L. Robertson, M. Thomas, H. Korhonen, K. E. J. Lehtinen, and H. Kokkola
Geosci. Model Dev., 8, 171–189, https://doi.org/10.5194/gmd-8-171-2015, https://doi.org/10.5194/gmd-8-171-2015, 2015
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We have integrated the sectional aerosol dynamics model SALSA into the European scale chemistry-transport model MATCH. The combined model reproduces observed higher particle number concentration (PNCs) in central Europe and lower concentrations in remote regions; however, the total PNC is underestimated. The low nucleation rate coefficient used in this study is an important reason for the underestimation.
E. M. Dunne, S. Mikkonen, H. Kokkola, and H. Korhonen
Atmos. Chem. Phys., 14, 13631–13642, https://doi.org/10.5194/acp-14-13631-2014, https://doi.org/10.5194/acp-14-13631-2014, 2014
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Marine clouds have a strong effect on the Earth's radiative balance. One proposed climate feedback is that, in a warming climate, marine aerosol emissions will change due to changing wind speeds. We have examined the processes that affect aerosol emissions and removal over 15 years, and high-temporal-resolution output over 2 months. We conclude that wind trends are unlikely to cause a strong feedback in marine regions, but changes in removal processes or transport from continental regions may.
A.-I. Partanen, E. M. Dunne, T. Bergman, A. Laakso, H. Kokkola, J. Ovadnevaite, L. Sogacheva, D. Baisnée, J. Sciare, A. Manders, C. O'Dowd, G. de Leeuw, and H. Korhonen
Atmos. Chem. Phys., 14, 11731–11752, https://doi.org/10.5194/acp-14-11731-2014, https://doi.org/10.5194/acp-14-11731-2014, 2014
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New parameterizations for the sea spray aerosol source flux and its organic fraction were incorporated into a global aerosol-climate model. The emissions of sea salt were considerably less than previous estimates. This study demonstrates that sea spray aerosol may actually decrease the number of cloud droplets, which has a warming effect on climate. Overall, sea spray aerosol was predicted to have a global cooling effect due to the scattering of solar radiation from sea spray aerosol particles.
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
T. Korhola, H. Kokkola, H. Korhonen, A.-I. Partanen, A. Laaksonen, K. E. J. Lehtinen, and S. Romakkaniemi
Geosci. Model Dev., 7, 161–174, https://doi.org/10.5194/gmd-7-161-2014, https://doi.org/10.5194/gmd-7-161-2014, 2014
A. Lipponen, V. Kolehmainen, S. Romakkaniemi, and H. Kokkola
Geosci. Model Dev., 6, 2087–2098, https://doi.org/10.5194/gmd-6-2087-2013, https://doi.org/10.5194/gmd-6-2087-2013, 2013
A. I. Partanen, A. Laakso, A. Schmidt, H. Kokkola, T. Kuokkanen, J.-P. Pietikäinen, V.-M. Kerminen, K. E. J. Lehtinen, L. Laakso, and H. Korhonen
Atmos. Chem. Phys., 13, 12059–12071, https://doi.org/10.5194/acp-13-12059-2013, https://doi.org/10.5194/acp-13-12059-2013, 2013
Kalle Nordling, Jukka-Pekka Keskinen, Sami Romakkaniemi, Harri Kokkola, Petri Räisänen, Antti Lipponen, Antti-Ilari Partanen, Jaakko Ahola, Juha Tonttila, Muzaffer Ege Alper, Hannele Korhonen, and Tomi Raatikainen
EGUsphere, https://doi.org/10.5194/egusphere-2023-912, https://doi.org/10.5194/egusphere-2023-912, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This paper shows how use machine learning methods to for model of small scale atmospherics physics model (large eddy simulation) which cover physics to the 100 m scale and implement that model to global large scale model. Our results shows that the global model is stable and it provides meaningful results. This way we can include physic based presentation of sub-grid (physics which happens in 100 m scale) physics to the global model which resolution is in 100 km scale.
Markku Kulmala, Anna Lintunen, Hanna Lappalainen, Annele Virtanen, Chao Yan, Ekaterina Ezhova, Tuomo Nieminen, Ilona Riipinen, Risto Makkonen, Johanna Tamminen, Anu-Maija Sundström, Antti Arola, Armin Hansel, Kari Lehtinen, Timo Vesala, Tuukka Petäjä, Jaana Bäck, Tom Kokkonen, and Veli-Matti Kerminen
EGUsphere, https://doi.org/10.5194/egusphere-2023-627, https://doi.org/10.5194/egusphere-2023-627, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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To be able to meet global grand challenges, we need comprehensive open data with proper metadata. In this opinion paper, we describe the SMEAR (Station for Measuring Earth surface – Atmosphere Relations) concept and include several examples (cases), such as NPF and growth, feedback loops, the effect of COVID, and what has been learnt from these investigations. The future needs and the potential of comprehensive observations of the environment are summarized.
Tuuli Miinalainen, Harri Kokkola, Antti Lipponen, Antti-Pekka Hyvärinen, Vijay Kumar Soni, Kari E. J. Lehtinen, and Thomas Kühn
Atmos. Chem. Phys., 23, 3471–3491, https://doi.org/10.5194/acp-23-3471-2023, https://doi.org/10.5194/acp-23-3471-2023, 2023
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We simulated the effects of aerosol emission mitigation on both global and regional radiative forcing and city-level air quality with a global-scale climate model. We used a machine learning downscaling approach to bias-correct the PM2.5 values obtained from the global model for the Indian megacity New Delhi. Our results indicate that aerosol mitigation could result in both improved air quality and less radiative heating for India.
Jutta Kesti, Ewan James O'Connor, Anne Hirsikko, John Backman, Heikki Lihavainen, Hannele Korhonen, and Eija Asmi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-811, https://doi.org/10.5194/acp-2022-811, 2023
Preprint under review for ACP
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The study combines aerosol particle measurements at the surface and vertical profiling of the atmosphere with a scanning Doppler lidar to investigate how transport together with boundary layer evolution can affect particle and SO2 concentrations at the surface in the Arabian Peninsula region. The instrumentation enabled us to see elevated nucleation mode particle and SO2 concentrations at the surface when air masses transported from polluted areas are mixed in the boundary layer.
Zijun Li, Angela Buchholz, Luis M. F. Barreira, Arttu Ylisirniö, Liqing Hao, Iida Pullinen, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 23, 203–220, https://doi.org/10.5194/acp-23-203-2023, https://doi.org/10.5194/acp-23-203-2023, 2023
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Interaction between NOx and biogenic emissions can be important in suburban areas. Our study showed that the addition of NOx during α-pinene SOA formation produced considerable amounts of organic nitrates and affected the composition of non-nitrated organic compounds. The compositional difference consequently altered the primary type of aqueous-phase processes during the isothermal particle evaporation.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Silvia M. Calderón, Juha Tonttila, Angela Buchholz, Jorma Joutsensaari, Mika Komppula, Ari Leskinen, Liqing Hao, Dmitri Moisseev, Iida Pullinen, Petri Tiitta, Jian Xu, Annele Virtanen, Harri Kokkola, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 12417–12441, https://doi.org/10.5194/acp-22-12417-2022, https://doi.org/10.5194/acp-22-12417-2022, 2022
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The spatial and temporal restrictions of observations and oversimplified aerosol representation in large eddy simulations (LES) limit our understanding of aerosol–stratocumulus interactions. In this closure study of in situ and remote sensing observations and outputs from UCLALES–SALSA, we have assessed the role of convective overturning and aerosol effects in two cloud events observed at the Puijo SMEAR IV station, Finland, a diurnal-high aerosol case and a nocturnal-low aerosol case.
Sini Isokääntä, Paul Kim, Santtu Mikkonen, Thomas Kühn, Harri Kokkola, Taina Yli-Juuti, Liine Heikkinen, Krista Luoma, Tuukka Petäjä, Zak Kipling, Daniel Partridge, and Annele Virtanen
Atmos. Chem. Phys., 22, 11823–11843, https://doi.org/10.5194/acp-22-11823-2022, https://doi.org/10.5194/acp-22-11823-2022, 2022
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This research employs air mass history analysis and observations to study how clouds and precipitation affect atmospheric aerosols during transport to a boreal forest site. The mass concentrations of studied chemical species showed exponential decrease as a function of accumulated rain along the air mass route. Our analysis revealed in-cloud sulfate formation, while no major changes in organic mass were seen. Most of the in-cloud-formed sulfate could be assigned to particle sizes above 200 nm.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Marje Prank, Juha Tonttila, Jaakko Ahola, Harri Kokkola, Thomas Kühn, Sami Romakkaniemi, and Tomi Raatikainen
Atmos. Chem. Phys., 22, 10971–10992, https://doi.org/10.5194/acp-22-10971-2022, https://doi.org/10.5194/acp-22-10971-2022, 2022
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Aerosols and clouds persist as the dominant sources of uncertainty in climate projections. In this modelling study, we investigate the role of marine aerosols in influencing the lifetime of low-level clouds. Our high resolution simulations show that sea spray can both extend and shorten the lifetime of the cloud layer depending on the model setup. The impact of the primary marine organics is relatively limited while secondary aerosol from monoterpenes can have larger impact.
Petri Tiitta, Ari Leskinen, Ville A. Kaikkonen, Eero O. Molkoselkä, Anssi J. Mäkynen, Jorma Joutsensaari, Silvia Calderon, Sami Romakkaniemi, and Mika Komppula
Atmos. Meas. Tech., 15, 2993–3009, https://doi.org/10.5194/amt-15-2993-2022, https://doi.org/10.5194/amt-15-2993-2022, 2022
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The novel holographic imaging instrument (ICEMET) was adapted to measure the microphysical properties of liquid clouds, and these values were compared with parallel measurements of a cloud droplet spectrometer (FM-120) and particle measurements using a twin-inlet system. When the intercomparison was carried out during isoaxial sampling, our results showed good agreement in terms of variability between the instruments. This agreement was confirmed using Mutual and Pearson correlation analyses.
Zoé Brasseur, Dimitri Castarède, Erik S. Thomson, Michael P. Adams, Saskia Drossaart van Dusseldorp, Paavo Heikkilä, Kimmo Korhonen, Janne Lampilahti, Mikhail Paramonov, Julia Schneider, Franziska Vogel, Yusheng Wu, Jonathan P. D. Abbatt, Nina S. Atanasova, Dennis H. Bamford, Barbara Bertozzi, Matthew Boyer, David Brus, Martin I. Daily, Romy Fösig, Ellen Gute, Alexander D. Harrison, Paula Hietala, Kristina Höhler, Zamin A. Kanji, Jorma Keskinen, Larissa Lacher, Markus Lampimäki, Janne Levula, Antti Manninen, Jens Nadolny, Maija Peltola, Grace C. E. Porter, Pyry Poutanen, Ulrike Proske, Tobias Schorr, Nsikanabasi Silas Umo, János Stenszky, Annele Virtanen, Dmitri Moisseev, Markku Kulmala, Benjamin J. Murray, Tuukka Petäjä, Ottmar Möhler, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 5117–5145, https://doi.org/10.5194/acp-22-5117-2022, https://doi.org/10.5194/acp-22-5117-2022, 2022
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The present measurement report introduces the ice nucleation campaign organized in Hyytiälä, Finland, in 2018 (HyICE-2018). We provide an overview of the campaign settings, and we describe the measurement infrastructure and operating procedures used. In addition, we use results from ice nucleation instrument inter-comparison to show that the suite of these instruments deployed during the campaign reports consistent results.
Jaakko Ahola, Tomi Raatikainen, Muzaffer Ege Alper, Jukka-Pekka Keskinen, Harri Kokkola, Antti Kukkurainen, Antti Lipponen, Jia Liu, Kalle Nordling, Antti-Ilari Partanen, Sami Romakkaniemi, Petri Räisänen, Juha Tonttila, and Hannele Korhonen
Atmos. Chem. Phys., 22, 4523–4537, https://doi.org/10.5194/acp-22-4523-2022, https://doi.org/10.5194/acp-22-4523-2022, 2022
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Clouds are important for the climate, and cloud droplets have a significant role in cloud properties. Cloud droplets form when air rises and cools and water vapour condenses on small particles that can be natural or of anthropogenic origin. Currently, the updraft velocity, meaning how fast the air rises, is poorly represented in global climate models. In our study, we show three methods that will improve the depiction of updraft velocity and which properties are vital to updrafts.
Tomi Raatikainen, Marje Prank, Jaakko Ahola, Harri Kokkola, Juha Tonttila, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 3763–3778, https://doi.org/10.5194/acp-22-3763-2022, https://doi.org/10.5194/acp-22-3763-2022, 2022
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Mineral dust or similar ice-nucleating particles (INPs) are needed to initiate cloud droplet freezing at temperatures common in shallow clouds. In this work we examine how INPs that are released from the sea surface impact marine clouds. Our high-resolution simulations show that turbulent updraughts carry these particles effectively up to the clouds, where they initiate cloud droplet freezing. Sea surface INP emissions become more important with decreasing background dust INP concentrations.
Jessica Slater, Hugh Coe, Gordon McFiggans, Juha Tonttila, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 2937–2953, https://doi.org/10.5194/acp-22-2937-2022, https://doi.org/10.5194/acp-22-2937-2022, 2022
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This paper shows the specific impact of black carbon (BC) on the aerosol–planetary boundary layer (PBL) feedback and its influence on a Beijing haze episode. Overall, this paper shows that strong temperature inversions prevent BC heating within the PBL from significantly increasing PBL height, while BC above the PBL suppresses PBL development significantly through the day. From this we suggest a method by which both locally and regionally emitted BC may impact urban pollution episodes.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
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We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Peifeng Su, Jorma Joutsensaari, Lubna Dada, Martha Arbayani Zaidan, Tuomo Nieminen, Xinyang Li, Yusheng Wu, Stefano Decesari, Sasu Tarkoma, Tuukka Petäjä, Markku Kulmala, and Petri Pellikka
Atmos. Chem. Phys., 22, 1293–1309, https://doi.org/10.5194/acp-22-1293-2022, https://doi.org/10.5194/acp-22-1293-2022, 2022
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We regarded the banana shapes in the surface plots as a special kind of object (similar to cats) and applied an instance segmentation technique to automatically identify the new particle formation (NPF) events (especially the strongest ones), in addition to their growth rates, start times, and end times. The automatic method generalized well on datasets collected in different sites, which is useful for long-term data series analysis and obtaining statistical properties of NPF events.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Jutta Kesti, John Backman, Ewan J. O'Connor, Anne Hirsikko, Eija Asmi, Minna Aurela, Ulla Makkonen, Maria Filioglou, Mika Komppula, Hannele Korhonen, and Heikki Lihavainen
Atmos. Chem. Phys., 22, 481–503, https://doi.org/10.5194/acp-22-481-2022, https://doi.org/10.5194/acp-22-481-2022, 2022
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In this study we combined aerosol particle measurements at the surface with a scanning Doppler lidar providing vertical profiles of the atmosphere to study the effect of different boundary layer conditions on aerosol particle properties in the understudied Arabian Peninsula region. The instrumentation used in this study enabled us to identify periods when pollution from remote sources was mixed down to the surface and initiated new particle formation in the growing boundary layer.
Ian Boutle, Wayne Angevine, Jian-Wen Bao, Thierry Bergot, Ritthik Bhattacharya, Andreas Bott, Leo Ducongé, Richard Forbes, Tobias Goecke, Evelyn Grell, Adrian Hill, Adele L. Igel, Innocent Kudzotsa, Christine Lac, Bjorn Maronga, Sami Romakkaniemi, Juerg Schmidli, Johannes Schwenkel, Gert-Jan Steeneveld, and Benoît Vié
Atmos. Chem. Phys., 22, 319–333, https://doi.org/10.5194/acp-22-319-2022, https://doi.org/10.5194/acp-22-319-2022, 2022
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Fog forecasting is one of the biggest problems for numerical weather prediction. By comparing many models used for fog forecasting with others used for fog research, we hoped to help guide forecast improvements. We show some key processes that, if improved, will help improve fog forecasting, such as how water is deposited on the ground. We also showed that research models were not themselves a suitable baseline for comparison, and we discuss what future observations are required to improve them.
Anton Laakso, Ulrike Niemeier, Daniele Visioni, Simone Tilmes, and Harri Kokkola
Atmos. Chem. Phys., 22, 93–118, https://doi.org/10.5194/acp-22-93-2022, https://doi.org/10.5194/acp-22-93-2022, 2022
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The use of different spatio-temporal sulfur injection strategies with different magnitudes to create an artificial reflective aerosol layer to cool the climate is studied using sectional and modal aerosol schemes in a climate model. There are significant differences in the results depending on the aerosol microphysical module used. Different spatio-temporal injection strategies have a significant impact on the magnitude and zonal distribution of radiative forcing and atmospheric dynamics.
Zijun Li, Angela Buchholz, Arttu Ylisirniö, Luis Barreira, Liqing Hao, Siegfried Schobesberger, Taina Yli-Juuti, and Annele Virtanen
Atmos. Chem. Phys., 21, 18283–18302, https://doi.org/10.5194/acp-21-18283-2021, https://doi.org/10.5194/acp-21-18283-2021, 2021
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We compared the evolution of two types of secondary organic aerosol (SOA) particles during isothermal evaporation. The sesquiterpene SOA particles demonstrated higher resilience to evaporation than α-pinene SOA particles generated under comparable conditions. In-depth analysis showed that under high-relative-humidity conditions, particulate water drove the evolution of particulate constituents by reducing the particle viscosity and initiating chemical aqueous-phase processes.
Maria Sand, Bjørn H. Samset, Gunnar Myhre, Jonas Gliß, Susanne E. Bauer, Huisheng Bian, Mian Chin, Ramiro Checa-Garcia, Paul Ginoux, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Philippe Le Sager, Marianne T. Lund, Hitoshi Matsui, Twan van Noije, Dirk J. L. Olivié, Samuel Remy, Michael Schulz, Philip Stier, Camilla W. Stjern, Toshihiko Takemura, Kostas Tsigaridis, Svetlana G. Tsyro, and Duncan Watson-Parris
Atmos. Chem. Phys., 21, 15929–15947, https://doi.org/10.5194/acp-21-15929-2021, https://doi.org/10.5194/acp-21-15929-2021, 2021
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Absorption of shortwave radiation by aerosols can modify precipitation and clouds but is poorly constrained in models. A total of 15 different aerosol models from AeroCom phase III have reported total aerosol absorption, and for the first time, 11 of these models have reported in a consistent experiment the contributions to absorption from black carbon, dust, and organic aerosol. Here, we document the model diversity in aerosol absorption.
Kalle Nordling, Hannele Korhonen, Jouni Räisänen, Antti-Ilari Partanen, Bjørn H. Samset, and Joonas Merikanto
Atmos. Chem. Phys., 21, 14941–14958, https://doi.org/10.5194/acp-21-14941-2021, https://doi.org/10.5194/acp-21-14941-2021, 2021
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Understanding the temperature responses to different climate forcing agents, such as greenhouse gases and aerosols, is crucial for understanding future regional climate changes. In climate models, the regional temperature responses vary for all forcing agents, but the causes of this variability are poorly understood. For all forcing agents, the main component contributing to variance in regional surface temperature responses between the climate models is the clear-sky longwave emissivity.
Twan van Noije, Tommi Bergman, Philippe Le Sager, Declan O'Donnell, Risto Makkonen, María Gonçalves-Ageitos, Ralf Döscher, Uwe Fladrich, Jost von Hardenberg, Jukka-Pekka Keskinen, Hannele Korhonen, Anton Laakso, Stelios Myriokefalitakis, Pirkka Ollinaho, Carlos Pérez García-Pando, Thomas Reerink, Roland Schrödner, Klaus Wyser, and Shuting Yang
Geosci. Model Dev., 14, 5637–5668, https://doi.org/10.5194/gmd-14-5637-2021, https://doi.org/10.5194/gmd-14-5637-2021, 2021
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This paper documents the global climate model EC-Earth3-AerChem, one of the members of the EC-Earth3 family of models participating in CMIP6. We give an overview of the model and describe in detail how it differs from its predecessor and the other EC-Earth3 configurations. The model's performance is characterized using coupled simulations conducted for CMIP6. The model has an effective equilibrium climate sensitivity of 3.9 °C and a transient climate response of 2.1 °C.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
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Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
Joonas Merikanto, Kalle Nordling, Petri Räisänen, Jouni Räisänen, Declan O'Donnell, Antti-Ilari Partanen, and Hannele Korhonen
Atmos. Chem. Phys., 21, 5865–5881, https://doi.org/10.5194/acp-21-5865-2021, https://doi.org/10.5194/acp-21-5865-2021, 2021
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Human-induced aerosols concentrate around their emission sources, yet their climate effects span far and wide. Here, we use two climate models to robustly identify the mechanisms of how Asian anthropogenic aerosols impact temperatures across the globe. A total removal of Asian anthropogenic aerosols increases the global temperatures by 0.26 ± 0.04 °C in the models, with the strongest warming taking place over the Arctic due to increased atmospheric transport of energy towards the high north.
Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys., 21, 3899–3918, https://doi.org/10.5194/acp-21-3899-2021, https://doi.org/10.5194/acp-21-3899-2021, 2021
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By triggering the formation of ice crystals, ice-nucleating particles (INP) strongly influence cloud formation. Continuous, long-term measurements are needed to characterize the atmospheric INP variability. Here, a first long-term time series of INP spectra measured in the boreal forest for more than 1 year is presented, showing a clear seasonal cycle. It is shown that the seasonal dependency of INP concentrations and prevalent INP types is driven by the abundance of biogenic aerosol.
Antti Ruuskanen, Sami Romakkaniemi, Harri Kokkola, Antti Arola, Santtu Mikkonen, Harri Portin, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, and Ari Leskinen
Atmos. Chem. Phys., 21, 1683–1695, https://doi.org/10.5194/acp-21-1683-2021, https://doi.org/10.5194/acp-21-1683-2021, 2021
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The study focuses mainly on cloud-scavenging efficiency of absorbing particulate matter (mainly black carbon) but additionally covers cloud-scavenging efficiency of scattering particles and statistics of cloud condensation nuclei. The main findings give insight into how black carbon is distributed in different particle sizes and the sensitivity to cloud scavenged. The main findings are useful for large-scale modelling for evaluating cloud scavenging.
Juha Tonttila, Ali Afzalifar, Harri Kokkola, Tomi Raatikainen, Hannele Korhonen, and Sami Romakkaniemi
Atmos. Chem. Phys., 21, 1035–1048, https://doi.org/10.5194/acp-21-1035-2021, https://doi.org/10.5194/acp-21-1035-2021, 2021
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The focus of this study is on rain enhancement by deliberate injection of small particles into clouds (
cloud seeding). The particles, usually released from an aircraft, are expected to enhance cloud droplet growth, but its practical feasibility is somewhat uncertain. To improve upon this, we simulate the seeding effects with a numerical model. The model reproduces the main features seen in field observations, with a strong sensitivity to the total mass of the injected particle material.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Jonas Gliß, Augustin Mortier, Michael Schulz, Elisabeth Andrews, Yves Balkanski, Susanne E. Bauer, Anna M. K. Benedictow, Huisheng Bian, Ramiro Checa-Garcia, Mian Chin, Paul Ginoux, Jan J. Griesfeller, Andreas Heckel, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Paolo Laj, Philippe Le Sager, Marianne Tronstad Lund, Cathrine Lund Myhre, Hitoshi Matsui, Gunnar Myhre, David Neubauer, Twan van Noije, Peter North, Dirk J. L. Olivié, Samuel Rémy, Larisa Sogacheva, Toshihiko Takemura, Kostas Tsigaridis, and Svetlana G. Tsyro
Atmos. Chem. Phys., 21, 87–128, https://doi.org/10.5194/acp-21-87-2021, https://doi.org/10.5194/acp-21-87-2021, 2021
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Simulated aerosol optical properties as well as the aerosol life cycle are investigated for 14 global models participating in the AeroCom initiative. Considerable diversity is found in the simulated aerosol species emissions and lifetimes, also resulting in a large diversity in the simulated aerosol mass, composition, and optical properties. A comparison with observations suggests that, on average, current models underestimate the direct effect of aerosol on the atmosphere radiation budget.
André Welti, Kimmo Korhonen, Pasi Miettinen, Ana A. Piedehierro, Yrjö Viisanen, Annele Virtanen, and Ari Laaksonen
Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, https://doi.org/10.5194/amt-13-7059-2020, 2020
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We describe a modification of the SPectrometer for Ice Nuclei (SPIN) chamber to study ice nucleation at low temperatures, relevant for ice formation in cirrus clouds. Validation experiments of homogeneous freezing of aqueous ammonium sulfate droplets and heterogeneous ice nucleation on silver iodide particles are included to demonstrate the advantages of the modified SPIN chamber for the investigation of ice nucleation in the extended temperature range.
Xiaoxia Shang, Elina Giannakaki, Stephanie Bohlmann, Maria Filioglou, Annika Saarto, Antti Ruuskanen, Ari Leskinen, Sami Romakkaniemi, and Mika Komppula
Atmos. Chem. Phys., 20, 15323–15339, https://doi.org/10.5194/acp-20-15323-2020, https://doi.org/10.5194/acp-20-15323-2020, 2020
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Measurements of the multi-wavelength Raman polarization lidar PollyXT have been combined with measurements of pollen type and concentration using a traditional pollen sampler at a rural forest site in Kuopio, Finland. The depolarization ratio was enhanced when there were pollen grains in the atmosphere, illustrating the potential of lidar to track pollen grains in the atmosphere. The depolarization ratio of pure pollen particles was assessed for birch and pine pollen using a novel algorithm.
Eemeli Holopainen, Harri Kokkola, Anton Laakso, and Thomas Kühn
Geosci. Model Dev., 13, 6215–6235, https://doi.org/10.5194/gmd-13-6215-2020, https://doi.org/10.5194/gmd-13-6215-2020, 2020
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This paper introduces an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol–climate models. With the default setup, our wet deposition scheme behaves spuriously and better representation can be achieved with this scheme when black carbon is mixed with soluble compounds at emission time. This work is done as many of the global models fail to reproduce the transport of black carbon to the Arctic, which may be due to the poor representation of wet removal in models.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
Atmos. Chem. Phys., 20, 11893–11906, https://doi.org/10.5194/acp-20-11893-2020, https://doi.org/10.5194/acp-20-11893-2020, 2020
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The feedback effect between aerosol particles, radiation and meteorology reduces turbulent motion and results in increased surface aerosol concentrations during Beijing haze. Observational analysis and regional modelling studies have examined the feedback effect but these studies are limited. In this work, we set up a high-resolution model for the Beijing environment to examine the sensitivity of the aerosol feedback effect to initial meteorological conditions and aerosol loading.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Jaakko Ahola, Hannele Korhonen, Juha Tonttila, Sami Romakkaniemi, Harri Kokkola, and Tomi Raatikainen
Atmos. Chem. Phys., 20, 11639–11654, https://doi.org/10.5194/acp-20-11639-2020, https://doi.org/10.5194/acp-20-11639-2020, 2020
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In this study, we present an improved cloud model that reproduces the behaviour of mixed-phase clouds containing liquid droplets and ice crystals in more detail than before. This model is a convenient computational tool that enables the study of phenomena that cannot fit into a laboratory. These clouds have a significant role in climate, but they are not yet properly understood. Here, we show the advantages of the new model in a case study focusing on Arctic mixed-phase clouds.
Konstantinos-Matthaios Doulgeris, Mika Komppula, Sami Romakkaniemi, Antti-Pekka Hyvärinen, Veli-Matti Kerminen, and David Brus
Atmos. Meas. Tech., 13, 5129–5147, https://doi.org/10.5194/amt-13-5129-2020, https://doi.org/10.5194/amt-13-5129-2020, 2020
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We intercompared three cloud spectrometers ground setups in conditions with frequently occurring supercooled clouds. The measurements were conducted during the Pallas Cloud Experiment (PaCE) in 2013, in the Finnish sub-Arctic region at Sammaltunturi station. The main meteorological parameters influencing the spectrometers' performance was the wind direction. Final recommendations and our view on the main limitations of each spectrometer ground setup are presented.
Innocent Kudzotsa, Harri Kokkola, Juha Tonttila, Tomi Raatikainen, and Sami Romakkaniemi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-851, https://doi.org/10.5194/acp-2020-851, 2020
Publication in ACP not foreseen
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
Maria Filioglou, Elina Giannakaki, John Backman, Jutta Kesti, Anne Hirsikko, Ronny Engelmann, Ewan O'Connor, Jari T. T. Leskinen, Xiaoxia Shang, Hannele Korhonen, Heikki Lihavainen, Sami Romakkaniemi, and Mika Komppula
Atmos. Chem. Phys., 20, 8909–8922, https://doi.org/10.5194/acp-20-8909-2020, https://doi.org/10.5194/acp-20-8909-2020, 2020
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Dust optical properties are region-dependent. Saharan, Asian, and Arabian dusts do not pose similar optical properties in terms of lidar ratios; thus, a universal lidar ratio for dust particles will lead to biases. The present study analyses observations over the United Arab Emirates, quantifying the optical and geometrical extents of the aerosol layers in the area, providing at the same time the Arabian dust properties along with chemical analysis of dust samples collected in the region.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Sini Isokääntä, Eetu Kari, Angela Buchholz, Liqing Hao, Siegfried Schobesberger, Annele Virtanen, and Santtu Mikkonen
Atmos. Meas. Tech., 13, 2995–3022, https://doi.org/10.5194/amt-13-2995-2020, https://doi.org/10.5194/amt-13-2995-2020, 2020
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Online mass spectrometry produces large amounts of data. These data can be interpreted with statistical methods, enabling scientists to more easily understand the underlying processes. We compared these techniques on car exhaust measurements. We show differences and similarities between the methods and give recommendations on applicability of the methods on certain types of data. We show that applying multiple methods leads to more robust results, thus increasing reliability of the findings.
Mikhail Paramonov, Saskia Drossaart van Dusseldorp, Ellen Gute, Jonathan P. D. Abbatt, Paavo Heikkilä, Jorma Keskinen, Xuemeng Chen, Krista Luoma, Liine Heikkinen, Liqing Hao, Tuukka Petäjä, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 6687–6706, https://doi.org/10.5194/acp-20-6687-2020, https://doi.org/10.5194/acp-20-6687-2020, 2020
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Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland in the winter–spring of 2018. It was found that no single parameter could be used to predict the INP number concentration at the measurement location during the examined time period. It was also not possible to identify physical and chemical properties of ambient INPs despite the complexity of the instrumental set-up. Therefore, this paper addresses the necessity for future INP measurements.
Anni Hartikainen, Petri Tiitta, Mika Ihalainen, Pasi Yli-Pirilä, Jürgen Orasche, Hendryk Czech, Miika Kortelainen, Heikki Lamberg, Heikki Suhonen, Hanna Koponen, Liqing Hao, Ralf Zimmermann, Jorma Jokiniemi, Jarkko Tissari, and Olli Sippula
Atmos. Chem. Phys., 20, 6357–6378, https://doi.org/10.5194/acp-20-6357-2020, https://doi.org/10.5194/acp-20-6357-2020, 2020
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Residential wood combustion emits large amounts of organic compounds, which are transformed in the atmosphere via photochemical ageing reactions. We assessed this organic emission at various stages of exposure with an oxidation flow reactor. Ageing led to major changes in both gaseous and particulate phases including increased acidic compounds and transformation of the polycyclic aromatic compounds. Such changes have serious implications for the health- and climate-related effects of combustion.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Thomas Kühn, Kaarle Kupiainen, Tuuli Miinalainen, Harri Kokkola, Ville-Veikko Paunu, Anton Laakso, Juha Tonttila, Rita Van Dingenen, Kati Kulovesi, Niko Karvosenoja, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 20, 5527–5546, https://doi.org/10.5194/acp-20-5527-2020, https://doi.org/10.5194/acp-20-5527-2020, 2020
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We investigate the effects of black carbon (BC) mitigation on Arctic climate and human health, accounting for the concurrent reduction of other aerosol species. While BC is attributed a net warming effect on climate, most other aerosol species cool the planet. We find that the direct radiative effect of mitigating BC induces cooling, while aerosol–cloud effects offset this cooling and introduce large uncertainties. Furthermore, the reduced aerosol emissions reduce human mortality considerably.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Ricardo Luis Carvalho, Vilhelm Malmborg, Axel Eriksson, Christoffer Boman, Joakim Pagels, Birgitta Svenningsson, Mika Komppula, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 20, 4951–4968, https://doi.org/10.5194/acp-20-4951-2020, https://doi.org/10.5194/acp-20-4951-2020, 2020
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Ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves were studied using a portable ice nuclei counter in an extensive laboratory experiment campaign. We found that even small changes in combustion conditions may affect the ice-nucleating ability of the emissions significantly. Also six different physico-chemical properties of the emissions were studied, but no clear correlation to their ice-nucleating ability was found.
Giulia Saponaro, Moa K. Sporre, David Neubauer, Harri Kokkola, Pekka Kolmonen, Larisa Sogacheva, Antti Arola, Gerrit de Leeuw, Inger H. H. Karset, Ari Laaksonen, and Ulrike Lohmann
Atmos. Chem. Phys., 20, 1607–1626, https://doi.org/10.5194/acp-20-1607-2020, https://doi.org/10.5194/acp-20-1607-2020, 2020
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The understanding of cloud processes is based on the quality of the representation of cloud properties. We compared cloud parameters from three models with satellite observations. We report on the performance of each data source, highlighting strengths and deficiencies, which should be considered when deriving the effect of aerosols on cloud properties.
Eetu Kari, Liqing Hao, Arttu Ylisirniö, Angela Buchholz, Ari Leskinen, Pasi Yli-Pirilä, Ilpo Nuutinen, Kari Kuuspalo, Jorma Jokiniemi, Celia L. Faiola, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 15651–15671, https://doi.org/10.5194/acp-19-15651-2019, https://doi.org/10.5194/acp-19-15651-2019, 2019
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We present, for the first time, the dual effect of GDI-vehicle exhaust on α-pinene SOA mass yield suppression. The first effect is a well-known NOx effect, but the second effect is more complex. Our results imply that this second effect is related to change of reaction pathways of α-pinene in the presence of GDI exhaust. The presence of vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of GDI emissions.
Jianhui Jiang, Sebnem Aksoyoglu, Imad El-Haddad, Giancarlo Ciarelli, Hugo A. C. Denier van der Gon, Francesco Canonaco, Stefania Gilardoni, Marco Paglione, María Cruz Minguillón, Olivier Favez, Yunjiang Zhang, Nicolas Marchand, Liqing Hao, Annele Virtanen, Kalliopi Florou, Colin O'Dowd, Jurgita Ovadnevaite, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, https://doi.org/10.5194/acp-19-15247-2019, 2019
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We use an air quality model with a modified organic aerosol (OA) module based on chamber experiments to identify the OA sources and their contributions in Europe. Comparisons with long-term measurements at nine sites in 2011 show an improvement in OA simulation. Our results suggest that the biomass burning and biogenic emissions are the dominant sources in winter and summer, respectively. Contributions of diesel and gasoline vehicles are relatively small compared to a previous study in the US.
Stephanie Bohlmann, Xiaoxia Shang, Elina Giannakaki, Maria Filioglou, Annika Saarto, Sami Romakkaniemi, and Mika Komppula
Atmos. Chem. Phys., 19, 14559–14569, https://doi.org/10.5194/acp-19-14559-2019, https://doi.org/10.5194/acp-19-14559-2019, 2019
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Measurements of the multiwavelength Raman polarization lidar PollyXT have been combined with measurements of pollen type and concentration using a traditional pollen sampler at the rural forest site in Vehmasmäki, Finland. High particle depolarization ratios were observed during an intense pollination event of birch pollen occasionally mixed with spruce pollen. Our observations illustrate the potential of the particle depolarization ratio to track pollen grains in the atmosphere.
David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Philip Stier, Daniel G. Partridge, Ina Tegen, Isabelle Bey, Tanja Stanelle, Harri Kokkola, and Ulrike Lohmann
Geosci. Model Dev., 12, 3609–3639, https://doi.org/10.5194/gmd-12-3609-2019, https://doi.org/10.5194/gmd-12-3609-2019, 2019
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The global aerosol–climate model ECHAM6.3–HAM2.3 as well as the previous model versions ECHAM5.5–HAM2.0 and ECHAM6.1–HAM2.2 are evaluated. The simulation of clouds has improved in ECHAM6.3–HAM2.3. This has an impact on effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions and equilibrium climate sensitivity, which are weaker in ECHAM6.3–HAM2.3 than in the previous model versions.
Kalle Nordling, Hannele Korhonen, Petri Räisänen, Muzaffer Ege Alper, Petteri Uotila, Declan O'Donnell, and Joonas Merikanto
Atmos. Chem. Phys., 19, 9969–9987, https://doi.org/10.5194/acp-19-9969-2019, https://doi.org/10.5194/acp-19-9969-2019, 2019
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We carry out long equilibrium climate simulations with two modern climate models and show that the climate model dynamic response contributes strongly to the anthropogenic aerosol response. We demonstrate that identical aerosol descriptions do not improve climate model skill to estimate regional anthropogenic aerosol impacts. Our experiment utilized two independent climate models (NorESM and ECHAM6) with an identical description for aerosols optical properties and indirect effect.
Erika Toivonen, Marjo Hippi, Hannele Korhonen, Ari Laaksonen, Markku Kangas, and Joni-Pekka Pietikäinen
Geosci. Model Dev., 12, 3481–3501, https://doi.org/10.5194/gmd-12-3481-2019, https://doi.org/10.5194/gmd-12-3481-2019, 2019
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We evaluated the skill of the road weather model RoadSurf to reproduce present-day road weather conditions in Finland when driven by a high-resolution regional climate model. Simulated road surface temperatures and conditions were compared to observations between 2002 and 2014 at 25 Finnish road weather stations. RoadSurf accurately captured the main characteristics of road weather conditions. Thus, this model can be used to study the future scenarios of road weather in the study area.
Ina Tegen, David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Isabelle Bey, Nick Schutgens, Philip Stier, Duncan Watson-Parris, Tanja Stanelle, Hauke Schmidt, Sebastian Rast, Harri Kokkola, Martin Schultz, Sabine Schroeder, Nikos Daskalakis, Stefan Barthel, Bernd Heinold, and Ulrike Lohmann
Geosci. Model Dev., 12, 1643–1677, https://doi.org/10.5194/gmd-12-1643-2019, https://doi.org/10.5194/gmd-12-1643-2019, 2019
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We describe a new version of the aerosol–climate model ECHAM–HAM and show tests of the model performance by comparing different aspects of the aerosol distribution with different datasets. The updated version of HAM contains improved descriptions of aerosol processes, including updated emission fields and cloud processes. While there are regional deviations between the model and observations, the model performs well overall.
Mona Kurppa, Antti Hellsten, Pontus Roldin, Harri Kokkola, Juha Tonttila, Mikko Auvinen, Christoph Kent, Prashant Kumar, Björn Maronga, and Leena Järvi
Geosci. Model Dev., 12, 1403–1422, https://doi.org/10.5194/gmd-12-1403-2019, https://doi.org/10.5194/gmd-12-1403-2019, 2019
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This paper describes the implementation of a sectional aerosol module, SALSA, into the PALM model system 6.0. The first evaluation study shows excellent agreements with measurements. Furthermore, we show that ignoring the dry deposition of aerosol particles can overestimate aerosol number concentrations by 20 %, whereas condensation and dissolutional growth increase the total aerosol mass by over 10 % in this specific urban environment.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
Juan Hong, Hanbing Xu, Haobo Tan, Changqing Yin, Liqing Hao, Fei Li, Mingfu Cai, Xuejiao Deng, Nan Wang, Hang Su, Yafang Cheng, Lin Wang, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 18, 14079–14094, https://doi.org/10.5194/acp-18-14079-2018, https://doi.org/10.5194/acp-18-14079-2018, 2018
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In this manuscript, we provide the results of the hygroscopicity of a more anthropogenically influenced aerosol in a suburban site in China. Organic material in the current type of aerosols showed moderate hygroscopicity, and it appeared to be less sensitive towards the variation of its oxidation level, which suggests different characteristics of the oxidation products in secondary organic aerosols (SOA) under the suburban/urban atmosphere in China when compared to other background environments.
Harri Kokkola, Thomas Kühn, Anton Laakso, Tommi Bergman, Kari E. J. Lehtinen, Tero Mielonen, Antti Arola, Scarlet Stadtler, Hannele Korhonen, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Ina Tegen, Colombe Siegenthaler-Le Drian, Martin G. Schultz, Isabelle Bey, Philip Stier, Nikos Daskalakis, Colette L. Heald, and Sami Romakkaniemi
Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, https://doi.org/10.5194/gmd-11-3833-2018, 2018
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In this paper we present a global aerosol–chemistry–climate model with the focus on its representation for atmospheric aerosol particles. In the model, aerosols are simulated using the aerosol module SALSA2.0, which in this paper is compared to satellite, ground, and aircraft-based observations of the properties of atmospheric aerosol. Based on this study, the model simulated aerosol properties compare well with the observations.
Maryam Dalirian, Arttu Ylisirniö, Angela Buchholz, Daniel Schlesinger, Johan Ström, Annele Virtanen, and Ilona Riipinen
Atmos. Chem. Phys., 18, 12477–12489, https://doi.org/10.5194/acp-18-12477-2018, https://doi.org/10.5194/acp-18-12477-2018, 2018
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Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect is, however, still uncertain. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC particles, in pure state or coated by various organic species. Our results show that existing theories have potential in describing the CCN activation of atmospheric BC mixed with soluble pollutants.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Scarlet Stadtler, Thomas Kühn, Sabine Schröder, Domenico Taraborrelli, Martin G. Schultz, and Harri Kokkola
Geosci. Model Dev., 11, 3235–3260, https://doi.org/10.5194/gmd-11-3235-2018, https://doi.org/10.5194/gmd-11-3235-2018, 2018
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Atmospheric aerosols interact with our climate system and have adverse health effects. Nevertheless, these particles are a source of uncertainty in climate projections and the formation process of secondary aerosols formed by organic gas-phase precursors is particularly not fully understood. In order to gain a deeper understanding of secondary organic aerosol formation, this model system explicitly represents gas-phase and aerosol formation processes. Finally, this allows for process discussion.
Robin G. Stevens, Katharina Loewe, Christopher Dearden, Antonios Dimitrelos, Anna Possner, Gesa K. Eirund, Tomi Raatikainen, Adrian A. Hill, Benjamin J. Shipway, Jonathan Wilkinson, Sami Romakkaniemi, Juha Tonttila, Ari Laaksonen, Hannele Korhonen, Paul Connolly, Ulrike Lohmann, Corinna Hoose, Annica M. L. Ekman, Ken S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 18, 11041–11071, https://doi.org/10.5194/acp-18-11041-2018, https://doi.org/10.5194/acp-18-11041-2018, 2018
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We perform a model intercomparison of summertime high Arctic clouds. Observed concentrations of aerosol particles necessary for cloud formation fell to extremely low values, coincident with a transition from cloudy to nearly cloud-free conditions. Previous analyses have suggested that at these low concentrations, the radiative properties of the clouds are determined primarily by these particle concentrations. The model results strongly support this hypothesis.
Jorma Joutsensaari, Matthew Ozon, Tuomo Nieminen, Santtu Mikkonen, Timo Lähivaara, Stefano Decesari, M. Cristina Facchini, Ari Laaksonen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 18, 9597–9615, https://doi.org/10.5194/acp-18-9597-2018, https://doi.org/10.5194/acp-18-9597-2018, 2018
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New particle formation (NPF) in the atmosphere is globally an important source of aerosol particles. NPF events are typically identified and analyzed manually by researchers from particle size distribution data day by day, which is time consuming and might be inconsistent. We have developed an automatic analysis method based on deep learning for NPF event identification. The developed method can be easily utilized to analyze any long-term datasets more accurately and consistently.
Wiebke Frey, Dawei Hu, James Dorsey, M. Rami Alfarra, Aki Pajunoja, Annele Virtanen, Paul Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 9393–9409, https://doi.org/10.5194/acp-18-9393-2018, https://doi.org/10.5194/acp-18-9393-2018, 2018
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The coupled system of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber was used to study the ice-forming abilities of secondary
organic aerosol particles under mixed-phase cloud conditions. Given the vast abundance of secondary organic particles in the atmosphere, they
might present an important contribution to ice-nucleating particles. However, we find that in the studied temperature range (20 to 28 °C)
the secondary organic particles do not nucleate ice particles.
Ian Boutle, Jeremy Price, Innocent Kudzotsa, Harri Kokkola, and Sami Romakkaniemi
Atmos. Chem. Phys., 18, 7827–7840, https://doi.org/10.5194/acp-18-7827-2018, https://doi.org/10.5194/acp-18-7827-2018, 2018
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Aerosol processes are a key mechanism in the development of fog. Poor representation of aerosol–fog interaction can result in large biases in fog forecasts, such as surface temperatures which are too high and fog which is too deep and long lived. A relatively simple representation of aerosol–fog interaction can actually lead to significant improvements in forecasting. Aerosol–fog interaction can have a large effect on the climate system but is poorly represented in climate models.
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
Joni-Pekka Pietikäinen, Tiina Markkanen, Kevin Sieck, Daniela Jacob, Johanna Korhonen, Petri Räisänen, Yao Gao, Jaakko Ahola, Hannele Korhonen, Ari Laaksonen, and Jussi Kaurola
Geosci. Model Dev., 11, 1321–1342, https://doi.org/10.5194/gmd-11-1321-2018, https://doi.org/10.5194/gmd-11-1321-2018, 2018
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The regional climate model REMO was coupled with the FLake lake model to include an interactive treatment of lakes. Using this new version, the Fenno-Scandinavian climate and lake characteristics were studied. Our results show that overall the new model version improves the representation of the Fenno-Scandinavian climate in terms of 2 m temperature and precipitation and that the model can reproduce surface water temperature, ice depth and ice season length with reasonably high accuracy.
Antti Lipponen, Tero Mielonen, Mikko R. A. Pitkänen, Robert C. Levy, Virginia R. Sawyer, Sami Romakkaniemi, Ville Kolehmainen, and Antti Arola
Atmos. Meas. Tech., 11, 1529–1547, https://doi.org/10.5194/amt-11-1529-2018, https://doi.org/10.5194/amt-11-1529-2018, 2018
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Atmospheric aerosols are small solid or liquid particles suspended in the atmosphere and they have a significant effect on the climate. Satellite data are used to get global estimates of atmospheric aerosols. In this work, a statistics-based Bayesian aerosol retrieval algorithm was developed to improve the accuracy and quantify the uncertainties related to the aerosol estimates. The algorithm is tested with NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) satellite data.
Wei Huang, Harald Saathoff, Aki Pajunoja, Xiaoli Shen, Karl-Heinz Naumann, Robert Wagner, Annele Virtanen, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, https://doi.org/10.5194/acp-18-2883-2018, 2018
Lukas Pichelstorfer, Dominik Stolzenburg, John Ortega, Thomas Karl, Harri Kokkola, Anton Laakso, Kari E. J. Lehtinen, James N. Smith, Peter H. McMurry, and Paul M. Winkler
Atmos. Chem. Phys., 18, 1307–1323, https://doi.org/10.5194/acp-18-1307-2018, https://doi.org/10.5194/acp-18-1307-2018, 2018
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Quantification of new particle formation as a source of atmospheric aerosol is clearly of importance for climate and health aspects. In our new study we developed two analysis methods that allow retrieval of nanoparticle growth dynamics at much higher precision than it was possible so far. Our results clearly demonstrate that growth rates show much more variation than is currently known and suggest that the Kelvin effect governs growth in the sub-10 nm size range.
Maria Filioglou, Anna Nikandrova, Sami Niemelä, Holger Baars, Tero Mielonen, Ari Leskinen, David Brus, Sami Romakkaniemi, Elina Giannakaki, and Mika Komppula
Atmos. Meas. Tech., 10, 4303–4316, https://doi.org/10.5194/amt-10-4303-2017, https://doi.org/10.5194/amt-10-4303-2017, 2017
Sami Romakkaniemi, Zubair Maalick, Antti Hellsten, Antti Ruuskanen, Olli Väisänen, Irshad Ahmad, Juha Tonttila, Santtu Mikkonen, Mika Komppula, and Thomas Kühn
Atmos. Chem. Phys., 17, 7955–7964, https://doi.org/10.5194/acp-17-7955-2017, https://doi.org/10.5194/acp-17-7955-2017, 2017
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Surface topography affects aerosol–cloud interactions in boundary layer clouds. Local topography effects should be screened out from in situ observations before results can be generalised into a larger scale. Here we present modelling and observational results from a measurement station residing in a 75 m tower on top of a 150 m hill, and analyse how landscape affects the cloud formation, and which factors should be taken into account when aerosol effect on cloud droplet formation is studied.
Changjin Hu, Qiao Ma, Zhi Liu, Yue Cheng, Liqing Hao, Nana Wei, Yanbo Gai, Xiaoxiao Lin, Xuejun Gu, Weixiong Zhao, Mingqiang Huang, Zhenya Wang, and Weijun Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-433, https://doi.org/10.5194/acp-2017-433, 2017
Revised manuscript not accepted
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The effect of NO2 on SOA formation from oxidation of limonene is found to be related to the competition between O3- and NO3-initiated oxidation as well as the competition between RO2 + HO2 and RO2 + NO2 (or NO3) following the initial ozonolysis, and organic nitrates is believed to play an important role in aerosol particle formation. It is suggested that SOA formation in the regions with substantial anthropogenic-biogenic interactions should be evaluated more systematically than before.
Anton Laakso, Hannele Korhonen, Sami Romakkaniemi, and Harri Kokkola
Atmos. Chem. Phys., 17, 6957–6974, https://doi.org/10.5194/acp-17-6957-2017, https://doi.org/10.5194/acp-17-6957-2017, 2017
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Based on simulations, equatorial stratospheric sulfur injections have shown to be an efficient strategy to counteract ongoing global warming. However, equatorial injections would result in relatively larger cooling in low latitudes than in high latitudes. This together with greenhouse-gas-induced warming would lead to cooling in the Equator and warming in the high latitudes. Results of this study show that a more optimal cooling effect is achieved by varying the injection area seasonally.
Antti Arola, Thomas F. Eck, Harri Kokkola, Mikko R. A. Pitkänen, and Sami Romakkaniemi
Atmos. Chem. Phys., 17, 5991–6001, https://doi.org/10.5194/acp-17-5991-2017, https://doi.org/10.5194/acp-17-5991-2017, 2017
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One of the issues that hinder the measurement-based assessment of aerosol–cloud interactions by remote sensing methods is that typically aerosols and clouds cannot be measured simultaneously by passive remote sensing methods. AERONET includes the SDA product that provides the fine-mode AOD also in mixed cloud–aerosol observations. These measurements have not yet been fully exploited in studies of aerosol–cloud interactions. We applied SDA for this kind of analysis.
Juan Hong, Mikko Äijälä, Silja A. K. Häme, Liqing Hao, Jonathan Duplissy, Liine M. Heikkinen, Wei Nie, Jyri Mikkilä, Markku Kulmala, Nønne L. Prisle, Annele Virtanen, Mikael Ehn, Pauli Paasonen, Douglas R. Worsnop, Ilona Riipinen, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 17, 4387–4399, https://doi.org/10.5194/acp-17-4387-2017, https://doi.org/10.5194/acp-17-4387-2017, 2017
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Estimates of volatility of secondary organic aerosols was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model and by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer data. About 16 % of the variation can be explained by the linear regression between the results from these two methods.
Wei Nie, Juan Hong, Silja A. K. Häme, Aijun Ding, Yugen Li, Chao Yan, Liqing Hao, Jyri Mikkilä, Longfei Zheng, Yuning Xie, Caijun Zhu, Zheng Xu, Xuguang Chi, Xin Huang, Yang Zhou, Peng Lin, Annele Virtanen, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, Jianzhen Yu, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 3659–3672, https://doi.org/10.5194/acp-17-3659-2017, https://doi.org/10.5194/acp-17-3659-2017, 2017
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HULIS are demonstrated to be important low-volatility, or even extremely low volatility, compounds in the organic aerosol phase. This sheds new light on the connection between atmospheric HULIS and ELVOCs. The interaction between HULIS and ammonium sulfate was found to decrease the volatility of the HULIS part in HULIS-AS mixed samples, indicating multiphase processes have the potential to lower the volatility of organic compounds in the aerosol phase.
Juha Tonttila, Zubair Maalick, Tomi Raatikainen, Harri Kokkola, Thomas Kühn, and Sami Romakkaniemi
Geosci. Model Dev., 10, 169–188, https://doi.org/10.5194/gmd-10-169-2017, https://doi.org/10.5194/gmd-10-169-2017, 2017
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Novel techniques for modelling the aerosol–cloud interactions are implemented in a cloud-resolving model. The new methods improve the representation of the poorly constrained effects of cloud processing, precipitation and the wet removal of particles on the aerosol population and the associated feedbacks. The detailed representation of these processes yields more realistic simulation of the evolution of boundary layer clouds and fogs, as compared to results obtained using more simple methods.
Lei Yao, Ming-Yi Wang, Xin-Ke Wang, Yi-Jun Liu, Hang-Fei Chen, Jun Zheng, Wei Nie, Ai-Jun Ding, Fu-Hai Geng, Dong-Fang Wang, Jian-Min Chen, Douglas R. Worsnop, and Lin Wang
Atmos. Chem. Phys., 16, 14527–14543, https://doi.org/10.5194/acp-16-14527-2016, https://doi.org/10.5194/acp-16-14527-2016, 2016
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We present the development of a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) method, utilizing protonated ethanol as reagent ions to simultaneously detect atmospheric gaseous amines (C1 to C6) and amides (C1 to C6). Deployment of this ethanol HR-ToF-CIMS has been demonstrated in a field campaign in urban Shanghai, China, detecting amines (from a few pptv to hundreds of pptv) and amides (from tens of pptv to a few ppbv).
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Olli Väisänen, Antti Ruuskanen, Arttu Ylisirniö, Pasi Miettinen, Harri Portin, Liqing Hao, Ari Leskinen, Mika Komppula, Sami Romakkaniemi, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 16, 10385–10398, https://doi.org/10.5194/acp-16-10385-2016, https://doi.org/10.5194/acp-16-10385-2016, 2016
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In-cloud measurements of aerosol hygroscopicity and cloud droplet activation were conducted in Kuopio, Finland. According to the observations, the less hygroscopic accumulation mode particles were present in the non-activated aerosol, whereas the more hygroscopic particles were scavenged into cloud droplets. The results illustrate the sensitivity of cloud droplet formation to varying chemical composition and highlight the need for proper treatment of anthropogenic aerosols in CCN predictions.
Hilkka Timonen, Mike Cubison, Minna Aurela, David Brus, Heikki Lihavainen, Risto Hillamo, Manjula Canagaratna, Bettina Nekat, Rolf Weller, Douglas Worsnop, and Sanna Saarikoski
Atmos. Meas. Tech., 9, 3263–3281, https://doi.org/10.5194/amt-9-3263-2016, https://doi.org/10.5194/amt-9-3263-2016, 2016
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The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power (m∕Δm50 ∼ 500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements and ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results.
Jordan E. Krechmer, Michael Groessl, Xuan Zhang, Heikki Junninen, Paola Massoli, Andrew T. Lambe, Joel R. Kimmel, Michael J. Cubison, Stephan Graf, Ying-Hsuan Lin, Sri H. Budisulistiorini, Haofei Zhang, Jason D. Surratt, Richard Knochenmuss, John T. Jayne, Douglas R. Worsnop, Jose-Luis Jimenez, and Manjula R. Canagaratna
Atmos. Meas. Tech., 9, 3245–3262, https://doi.org/10.5194/amt-9-3245-2016, https://doi.org/10.5194/amt-9-3245-2016, 2016
Tero Mielonen, Anca Hienola, Thomas Kühn, Joonas Merikanto, Antti Lipponen, Tommi Bergman, Hannele Korhonen, Pekka Kolmonen, Larisa Sogacheva, Darren Ghent, Antti Arola, Gerrit de Leeuw, and Harri Kokkola
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-625, https://doi.org/10.5194/acp-2016-625, 2016
Revised manuscript not accepted
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We studied the temperature dependence of AOD and its radiative effects over the southeastern US. We used spaceborne observations of AOD, LST and tropospheric NO2 with simulations of ECHAM-HAMMOZ. The level of AOD in this region is governed by anthropogenic emissions but the temperature dependency is most likely caused by BVOC emissions. According to the observations and simulations, the regional clear-sky DRE for biogenic aerosols is −0.43 ± 0.88 W/m2/K and −0.86 ± 0.06 W/m2/K, respectively.
Yele Sun, Wei Du, Pingqing Fu, Qingqing Wang, Jie Li, Xinlei Ge, Qi Zhang, Chunmao Zhu, Lujie Ren, Weiqi Xu, Jian Zhao, Tingting Han, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 16, 8309–8329, https://doi.org/10.5194/acp-16-8309-2016, https://doi.org/10.5194/acp-16-8309-2016, 2016
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We have a comprehensive characterization of the sources, variations and processes of submicron aerosols in Beijing in winter using HR-AMS and GC/MS measurements. The primary sources including traffic, cooking, biomass burning and coal combustion emissions, and secondary components were separated and quantified with PMF. Our results elucidated the important roles of primary emissions, particularly coal combustion, and aqueous-phase processing in the formation of severe air pollution in winter.
Jani Huttunen, Harri Kokkola, Tero Mielonen, Mika Esa Juhani Mononen, Antti Lipponen, Juha Reunanen, Anders Vilhelm Lindfors, Santtu Mikkonen, Kari Erkki Juhani Lehtinen, Natalia Kouremeti, Alkiviadis Bais, Harri Niska, and Antti Arola
Atmos. Chem. Phys., 16, 8181–8191, https://doi.org/10.5194/acp-16-8181-2016, https://doi.org/10.5194/acp-16-8181-2016, 2016
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For a good estimate of the current forcing by anthropogenic aerosols, knowledge in past is needed. One option to lengthen time series is to retrieve aerosol optical depth from solar radiation measurements. We have evaluated several methods for this task. Most of the methods produce aerosol optical depth estimates with a good accuracy. However, machine learning methods seem to be the most applicable not to produce any systematic biases, since they do not need constrain the aerosol properties.
Bernadette Rosati, Martin Gysel, Florian Rubach, Thomas F. Mentel, Brigitta Goger, Laurent Poulain, Patrick Schlag, Pasi Miettinen, Aki Pajunoja, Annele Virtanen, Henk Klein Baltink, J. S. Bas Henzing, Johannes Größ, Gian Paolo Gobbi, Alfred Wiedensohler, Astrid Kiendler-Scharr, Stefano Decesari, Maria Cristina Facchini, Ernest Weingartner, and Urs Baltensperger
Atmos. Chem. Phys., 16, 7295–7315, https://doi.org/10.5194/acp-16-7295-2016, https://doi.org/10.5194/acp-16-7295-2016, 2016
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This study presents PEGASOS project data from field campaigns in the Po Valley, Italy and the Netherlands. Vertical profiles of aerosol hygroscopicity and chemical composition were investigated with airborne measurements on board a Zeppelin NT airship. A special focus was on the evolution of different mixing layers within the PBL as a function of daytime. A closure study showed that variations in aerosol hygroscopicity can well be explained by the variations in chemical composition.
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
Bernadette Rosati, Erik Herrmann, Silvia Bucci, Federico Fierli, Francesco Cairo, Martin Gysel, Ralf Tillmann, Johannes Größ, Gian Paolo Gobbi, Luca Di Liberto, Guido Di Donfrancesco, Alfred Wiedensohler, Ernest Weingartner, Annele Virtanen, Thomas F. Mentel, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4539–4554, https://doi.org/10.5194/acp-16-4539-2016, https://doi.org/10.5194/acp-16-4539-2016, 2016
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We present vertical profiles of aerosol optical properties, which were explored within the planetary boundary layer in a case study in 2012 in the Po Valley region. A comparison of in situ measurements recorded aboard a Zeppelin NT and ground-based remote-sensing data was performed yielding good agreement. Additionally, the role of ambient relative humidity for the aerosol particles' optical properties was investigated.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
N. I. Kristiansen, A. Stohl, D. J. L. Olivié, B. Croft, O. A. Søvde, H. Klein, T. Christoudias, D. Kunkel, S. J. Leadbetter, Y. H. Lee, K. Zhang, K. Tsigaridis, T. Bergman, N. Evangeliou, H. Wang, P.-L. Ma, R. C. Easter, P. J. Rasch, X. Liu, G. Pitari, G. Di Genova, S. Y. Zhao, Y. Balkanski, S. E. Bauer, G. S. Faluvegi, H. Kokkola, R. V. Martin, J. R. Pierce, M. Schulz, D. Shindell, H. Tost, and H. Zhang
Atmos. Chem. Phys., 16, 3525–3561, https://doi.org/10.5194/acp-16-3525-2016, https://doi.org/10.5194/acp-16-3525-2016, 2016
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Processes affecting aerosol removal from the atmosphere are not fully understood. In this study we investigate to what extent atmospheric transport models can reproduce observed loss of aerosols. We compare measurements of radioactive isotopes, that attached to ambient sulfate aerosols during the 2011 Fukushima nuclear accident, to 19 models using identical emissions. Results indicate aerosol removal that is too fast in most models, and apply to aerosols that have undergone long-range transport.
Zak Kipling, Philip Stier, Colin E. Johnson, Graham W. Mann, Nicolas Bellouin, Susanne E. Bauer, Tommi Bergman, Mian Chin, Thomas Diehl, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Harri Kokkola, Xiaohong Liu, Gan Luo, Twan van Noije, Kirsty J. Pringle, Knut von Salzen, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Toshihiko Takemura, Kostas Tsigaridis, and Kai Zhang
Atmos. Chem. Phys., 16, 2221–2241, https://doi.org/10.5194/acp-16-2221-2016, https://doi.org/10.5194/acp-16-2221-2016, 2016
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The vertical distribution of atmospheric aerosol is an important factor in its effects on climate. In this study we use a sophisticated model of the many interacting processes affecting aerosol in the atmosphere to show that the vertical distribution is typically dominated by only a few of these processes. Constraining these physical processes may help to reduce the large differences between models. However, the important processes are not always the same for different types of aerosol.
M. Dal Maso, L. Liao, J. Wildt, A. Kiendler-Scharr, E. Kleist, R. Tillmann, M. Sipilä, J. Hakala, K. Lehtipalo, M. Ehn, V.-M. Kerminen, M. Kulmala, D. Worsnop, and T. Mentel
Atmos. Chem. Phys., 16, 1955–1970, https://doi.org/10.5194/acp-16-1955-2016, https://doi.org/10.5194/acp-16-1955-2016, 2016
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In this paper, we present the first direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We found that the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength, and that the formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
A. Laakso, H. Kokkola, A.-I. Partanen, U. Niemeier, C. Timmreck, K. E. J. Lehtinen, H. Hakkarainen, and H. Korhonen
Atmos. Chem. Phys., 16, 305–323, https://doi.org/10.5194/acp-16-305-2016, https://doi.org/10.5194/acp-16-305-2016, 2016
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We have studied the impacts of a volcanic eruption during solar radiation management (SRM) using an aerosol-climate model ECHAM5-HAM-SALSA and an Earth system model MPI-ESM. A volcanic eruption during stratospheric sulfur geoengineering would lead to larger particles and smaller amount of new particles than if an volcano erupts in normal atmospheric conditions. Thus, volcanic eruption during SRM would lead to only a small additional cooling which would last for a significantly shorter period.
A. M. K. Hansen, J. Hong, T. Raatikainen, K. Kristensen, A. Ylisirniö, A. Virtanen, T. Petäjä, M. Glasius, and N. L. Prisle
Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, https://doi.org/10.5194/acp-15-14071-2015, 2015
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This paper presents the first study of the hygroscopic properties of limonene derived organosulfates (L-OS 250). The results showed that L-OS 250 particles are weakly hygroscopic and able to activate into cloud droplets. Particles of L-OS 250 mixed with ammonium sulfate were much more hygroscopic than expected from model parametrizations and the ZSR mixing rule, indicating that solubility and non-ideal droplet interactions could be important for the hygroscopic properties of the mixed particles.
W. Q. Xu, Y. L. Sun, C. Chen, W. Du, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, X. J. Zhao, L. B. Zhou, D. S. Ji, P. C. Wang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 13681–13698, https://doi.org/10.5194/acp-15-13681-2015, https://doi.org/10.5194/acp-15-13681-2015, 2015
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We have investigated the response of aerosol composition, size distributions, and oxidation properties to emission controls during the 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing. Our results showed substantial changes of aerosol bulk composition during APEC with the most reductions in secondary aerosols in large accumulation modes, demonstrating that that emission controls over regional scales can substantially reduce secondary particulates.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
C. Chen, Y. L. Sun, W. Q. Xu, W. Du, L. B. Zhou, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, Z. Q. Gao, Q. Zhang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 12879–12895, https://doi.org/10.5194/acp-15-12879-2015, https://doi.org/10.5194/acp-15-12879-2015, 2015
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A comprehensive characterization of submicron aerosol composition and sources at 260m in urban Beijing during APEC 2014 is presented. Aerosol species were shown to decrease substantially by 40–80% during APEC, whereas the bulk composition was relatively similar to the result of synergetic controls of secondary precursors. Our results elucidated that the good air quality during APEC was the combined result of emission controls and meteorological effects, with the former playing the dominant role.
S. Carbone, T. Onasch, S. Saarikoski, H. Timonen, K. Saarnio, D. Sueper, T. Rönkkö, L. Pirjola, A. Häyrinen, D. Worsnop, and R. Hillamo
Atmos. Meas. Tech., 8, 4803–4815, https://doi.org/10.5194/amt-8-4803-2015, https://doi.org/10.5194/amt-8-4803-2015, 2015
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The purpose of this study was to develop a method for the quantification of trace metal content in black carbon aerosol in real time, such as combustion-related emissions, by using the SP-AMS. The properties of 13 different trace metals (Na, Al, Ca, V, Cr, Fe, Mn, Ni, Cu, Zn, Rb, Sr and Ba) were investigated in a controlled laboratory experiment. The results from the laboratory tests were applied to study fine particles in emissions of a heavy-fuel-oil-fired heating station.
A. Arola, G. L. Schuster, M. R. A. Pitkänen, O. Dubovik, H. Kokkola, A. V. Lindfors, T. Mielonen, T. Raatikainen, S. Romakkaniemi, S. N. Tripathi, and H. Lihavainen
Atmos. Chem. Phys., 15, 12731–12740, https://doi.org/10.5194/acp-15-12731-2015, https://doi.org/10.5194/acp-15-12731-2015, 2015
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There have been relatively few measurement-based estimates for the direct radiative effect of brown carbon so far. This is first time that the direct radiative effect of brown carbon is estimated by exploiting the AERONET-retrieved imaginary indices. We estimated it for four sites in the Indo-Gangetic Plain: Karachi, Lahore,
Kanpur and Gandhi College.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
J. C. Corbin, A. Othman, J. D. Allan, D. R. Worsnop, J. D. Haskins, B. Sierau, U. Lohmann, and A. A. Mensah
Atmos. Meas. Tech., 8, 4615–4636, https://doi.org/10.5194/amt-8-4615-2015, https://doi.org/10.5194/amt-8-4615-2015, 2015
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Peak-integration uncertainties in the Aerodyne high-resolution aerosol mass spectrometer (AMS) are analyzed in detail using a combination of empirical data analysis and Monte Carlo approaches. The most general conclusion, applicable to any mass spectrometer, is that non-zero mass accuracy leads to a percentage error in constrained peak fits, even for well-resolved peaks. For overlapping peaks, this mass-accuracy effect may be viewed as a reduction in the effective m/z-calibration precision.
J. Joutsensaari, P. Yli-Pirilä, H. Korhonen, A. Arola, J. D. Blande, J. Heijari, M. Kivimäenpää, S. Mikkonen, L. Hao, P. Miettinen, P. Lyytikäinen-Saarenmaa, C. L. Faiola, A. Laaksonen, and J. K. Holopainen
Atmos. Chem. Phys., 15, 12139–12157, https://doi.org/10.5194/acp-15-12139-2015, https://doi.org/10.5194/acp-15-12139-2015, 2015
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Global warming will induce large-scale insect outbreaks in boreal forests. Our results from field and laboratory experiments, satellite observations and global-scale modelling suggest that more frequent insect outbreaks, in addition to temperature-dependent increases in VOC emissions, could result in substantial increases in biogenic SOA formation and therefore affect both aerosol direct and indirect forcing of climate at regional scales. This should be considered in future climate predictions.
J. Hong, J. Kim, T. Nieminen, J. Duplissy, M. Ehn, M. Äijälä, L. Q. Hao, W. Nie, N. Sarnela, N. L. Prisle, M. Kulmala, A. Virtanen, T. Petäjä, and V.-M. Kerminen
Atmos. Chem. Phys., 15, 11999–12009, https://doi.org/10.5194/acp-15-11999-2015, https://doi.org/10.5194/acp-15-11999-2015, 2015
R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, F. Canonaco, P. L. Croteau, M. Gysel, S. Henne, E. Herrmann, J. T. Jayne, M. Steinbacher, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11373–11398, https://doi.org/10.5194/acp-15-11373-2015, https://doi.org/10.5194/acp-15-11373-2015, 2015
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This manuscript presents the first long-term (14-month) and highly time-resolved (10 min) measurements of NR-PM1 aerosol chemical composition at a high-altitude site (JFJ, Switzerland, 3580m a.s.l.). The elevated location allowed the investigation of free tropospheric aerosol year round. Total and relative mass loadings, diurnal variations as well as seasonal variations are discussed together with geographical origin, organic aerosol sources and the influence of the planetary boundary layer.
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
Y. L. Sun, Z. F. Wang, W. Du, Q. Zhang, Q. Q. Wang, P. Q. Fu, X. L. Pan, J. Li, J. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 10149–10165, https://doi.org/10.5194/acp-15-10149-2015, https://doi.org/10.5194/acp-15-10149-2015, 2015
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We conducted the first long-term real-time measurement of submicron aerosol composition in Beijing using an ACSM for 1 year. The seasonal variations of mass concentrations and chemical composition of submicron aerosol were investigated in detail, and the meteorological effects on aerosol chemistry, particularly temperature and relative humidity, were elucidated. Finally, the potential source areas of aerosol species during four seasons were identified.
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
M. A. Thomas, M. Kahnert, C. Andersson, H. Kokkola, U. Hansson, C. Jones, J. Langner, and A. Devasthale
Geosci. Model Dev., 8, 1885–1898, https://doi.org/10.5194/gmd-8-1885-2015, https://doi.org/10.5194/gmd-8-1885-2015, 2015
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We have showed that a coupled modelling system is beneficial in the sense that more complex processes can be included to better represent the aerosol processes starting from their formation, their interactions with clouds and provide better estimate of radiative forcing. Using this model set up, we estimated an annual mean 'indirect' radiative forcing of -0.64W/m2. This means that aerosols, solely by their capability of altering the microphysical properties of clouds can cool the Earth system.
A. Leskinen, P. Yli-Pirilä, K. Kuuspalo, O. Sippula, P. Jalava, M.-R. Hirvonen, J. Jokiniemi, A. Virtanen, M. Komppula, and K. E. J. Lehtinen
Atmos. Meas. Tech., 8, 2267–2278, https://doi.org/10.5194/amt-8-2267-2015, https://doi.org/10.5194/amt-8-2267-2015, 2015
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A 29 m3 Teflon chamber was characterized and tested with oxidation experiments of toluene. Secondary organic aerosol yields of 12-42 % were obtained. These yields are comparable to those obtained in other laboratories.
J.-P. Pietikäinen, K. Kupiainen, Z. Klimont, R. Makkonen, H. Korhonen, R. Karinkanta, A.-P. Hyvärinen, N. Karvosenoja, A. Laaksonen, H. Lihavainen, and V.-M. Kerminen
Atmos. Chem. Phys., 15, 5501–5519, https://doi.org/10.5194/acp-15-5501-2015, https://doi.org/10.5194/acp-15-5501-2015, 2015
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The global aerosol--climate model ECHAM-HAMMOZ is used to study the aerosol burden and forcing changes in the coming decades. We show that aerosol burdens overall can have a decreasing trend leading to reductions in the direct aerosol effect being globally 0.06--0.4W/m2 by 2030, whereas the aerosol indirect radiative effect could decline 0.25--0.82W/m2. We also show that the targeted emission reduction measures can be a much better choice for the climate than overall high reductions globally.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
M. Dalirian, H. Keskinen, L. Ahlm, A. Ylisirniö, S. Romakkaniemi, A. Laaksonen, A. Virtanen, and I. Riipinen
Atmos. Chem. Phys., 15, 3815–3829, https://doi.org/10.5194/acp-15-3815-2015, https://doi.org/10.5194/acp-15-3815-2015, 2015
A. T. Lambe, P. S. Chhabra, T. B. Onasch, W. H. Brune, J. F. Hunter, J. H. Kroll, M. J. Cummings, J. F. Brogan, Y. Parmar, D. R. Worsnop, C. E. Kolb, and P. Davidovits
Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, https://doi.org/10.5194/acp-15-3063-2015, 2015
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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
S. Xiao, M. Y. Wang, L. Yao, M. Kulmala, B. Zhou, X. Yang, J. M. Chen, D. F. Wang, Q. Y. Fu, D. R. Worsnop, and L. Wang
Atmos. Chem. Phys., 15, 1769–1781, https://doi.org/10.5194/acp-15-1769-2015, https://doi.org/10.5194/acp-15-1769-2015, 2015
C. Andersson, R. Bergström, C. Bennet, L. Robertson, M. Thomas, H. Korhonen, K. E. J. Lehtinen, and H. Kokkola
Geosci. Model Dev., 8, 171–189, https://doi.org/10.5194/gmd-8-171-2015, https://doi.org/10.5194/gmd-8-171-2015, 2015
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We have integrated the sectional aerosol dynamics model SALSA into the European scale chemistry-transport model MATCH. The combined model reproduces observed higher particle number concentration (PNCs) in central Europe and lower concentrations in remote regions; however, the total PNC is underestimated. The low nucleation rate coefficient used in this study is an important reason for the underestimation.
I. Nuaaman, S.-M. Li, K. L. Hayden, T. B. Onasch, P. Massoli, D. Sueper, D. R. Worsnop, T. S. Bates, P. K. Quinn, and R. McLaren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-2085-2015, https://doi.org/10.5194/acpd-15-2085-2015, 2015
Revised manuscript has not been submitted
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In this paper, we focus on the measurement and reporting of mass concentrations of particulate chloride and sea salt in a marine area off the coast of California using a High Resolution Aerosol Mass Spectrometer. We outline a method of deconvolving the total aerosol chloride mass into refractory and non-refractory components, previously not reported in the literature. This can be important in regions where refractory sea salt aerosols can contribute to the aerosol chloride signal measured with t
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
S. Schobesberger, A. Franchin, F. Bianchi, L. Rondo, J. Duplissy, A. Kürten, I. K. Ortega, A. Metzger, R. Schnitzhofer, J. Almeida, A. Amorim, J. Dommen, E. M. Dunne, M. Ehn, S. Gagné, L. Ickes, H. Junninen, A. Hansel, V.-M. Kerminen, J. Kirkby, A. Kupc, A. Laaksonen, K. Lehtipalo, S. Mathot, A. Onnela, T. Petäjä, F. Riccobono, F. D. Santos, M. Sipilä, A. Tomé, G. Tsagkogeorgas, Y. Viisanen, P. E. Wagner, D. Wimmer, J. Curtius, N. M. Donahue, U. Baltensperger, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 55–78, https://doi.org/10.5194/acp-15-55-2015, https://doi.org/10.5194/acp-15-55-2015, 2015
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We used an ion mass spectrometer at CERN's CLOUD chamber to investigate the detailed composition of ammonia--sulfuric acid ion clusters (of both polarities) as they initially form and then grow into aerosol particles, at atmospherically relevant conditions. We found that these clusters’ composition is mainly determined by the ratio of the precursor vapors and ranges from ammonia-free clusters to clusters containing > 1 ammonia per sulfuric acid. Acid--base bindings are a key formation mechanism.
P. S. Chhabra, A. T. Lambe, M. R. Canagaratna, H. Stark, J. T. Jayne, T. B. Onasch, P. Davidovits, J. R. Kimmel, and D. R. Worsnop
Atmos. Meas. Tech., 8, 1–18, https://doi.org/10.5194/amt-8-1-2015, https://doi.org/10.5194/amt-8-1-2015, 2015
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Authors of this publication used acetate chemical ionization mass spectrometry (acetate-CIMS) to measure experimental products of alpha-pinene and naphthalene oxidation formed in a flow reactor. Acetate-CIMS instrumentation is selective toward carboxylic acid compounds which are readily formed in atmospheric photooxidation processes. Spectral information was used to identify previously measured products of both systems and to estimate their volatilities.
J.-E. Petit, O. Favez, J. Sciare, F. Canonaco, P. Croteau, G. Močnik, J. Jayne, D. Worsnop, and E. Leoz-Garziandia
Atmos. Chem. Phys., 14, 13773–13787, https://doi.org/10.5194/acp-14-13773-2014, https://doi.org/10.5194/acp-14-13773-2014, 2014
E. M. Dunne, S. Mikkonen, H. Kokkola, and H. Korhonen
Atmos. Chem. Phys., 14, 13631–13642, https://doi.org/10.5194/acp-14-13631-2014, https://doi.org/10.5194/acp-14-13631-2014, 2014
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Marine clouds have a strong effect on the Earth's radiative balance. One proposed climate feedback is that, in a warming climate, marine aerosol emissions will change due to changing wind speeds. We have examined the processes that affect aerosol emissions and removal over 15 years, and high-temporal-resolution output over 2 months. We conclude that wind trends are unlikely to cause a strong feedback in marine regions, but changes in removal processes or transport from continental regions may.
L. Q. Hao, A. Kortelainen, S. Romakkaniemi, H. Portin, A. Jaatinen, A. Leskinen, M. Komppula, P. Miettinen, D. Sueper, A. Pajunoja, J. N. Smith, K. E. J. Lehtinen, D. R. Worsnop, A. Laaksonen, and A. Virtanen
Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, https://doi.org/10.5194/acp-14-13483-2014, 2014
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Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions from the measurement in a mixed region between the boreal forestland and the urban area. The PMF analysis succeeded in separating the mixed spectra into three distinct organic factors and one inorganic factor. The particulate organic nitrate was distinguished by PMF for the first time, with a contribution of one-third of the total nitrate mass.
M. D. Willis, A. K. Y. Lee, T. B. Onasch, E. C. Fortner, L. R. Williams, A. T. Lambe, D. R. Worsnop, and J. P. D. Abbatt
Atmos. Meas. Tech., 7, 4507–4516, https://doi.org/10.5194/amt-7-4507-2014, https://doi.org/10.5194/amt-7-4507-2014, 2014
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
L. Rondo, A. Kürten, S. Ehrhart, S. Schobesberger, A. Franchin, H. Junninen, T. Petäjä, M. Sipilä, D. R. Worsnop, and J. Curtius
Atmos. Meas. Tech., 7, 3849–3859, https://doi.org/10.5194/amt-7-3849-2014, https://doi.org/10.5194/amt-7-3849-2014, 2014
S. Decesari, J. Allan, C. Plass-Duelmer, B. J. Williams, M. Paglione, M. C. Facchini, C. O'Dowd, R. M. Harrison, J. K. Gietl, H. Coe, L. Giulianelli, G. P. Gobbi, C. Lanconelli, C. Carbone, D. Worsnop, A. T. Lambe, A. T. Ahern, F. Moretti, E. Tagliavini, T. Elste, S. Gilge, Y. Zhang, and M. Dall'Osto
Atmos. Chem. Phys., 14, 12109–12132, https://doi.org/10.5194/acp-14-12109-2014, https://doi.org/10.5194/acp-14-12109-2014, 2014
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We made use of multiple spectrometric techniques for characterizing the aerosol chemical composition and mixing in the Po Valley in the summer.
The oxygenated organic aerosol (OOA) concentrations were correlated with simple tracers for recirculated planetary boundary layer air.
A full internal mixing between black carbon (BC) and the non-refractory aerosol components was never observed. Local sources in the Po Valley were responsible for the production of organic particles unmixed with BC.
A.-I. Partanen, E. M. Dunne, T. Bergman, A. Laakso, H. Kokkola, J. Ovadnevaite, L. Sogacheva, D. Baisnée, J. Sciare, A. Manders, C. O'Dowd, G. de Leeuw, and H. Korhonen
Atmos. Chem. Phys., 14, 11731–11752, https://doi.org/10.5194/acp-14-11731-2014, https://doi.org/10.5194/acp-14-11731-2014, 2014
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New parameterizations for the sea spray aerosol source flux and its organic fraction were incorporated into a global aerosol-climate model. The emissions of sea salt were considerably less than previous estimates. This study demonstrates that sea spray aerosol may actually decrease the number of cloud droplets, which has a warming effect on climate. Overall, sea spray aerosol was predicted to have a global cooling effect due to the scattering of solar radiation from sea spray aerosol particles.
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
T. R. Dallmann, T. B. Onasch, T. W. Kirchstetter, D. R. Worton, E. C. Fortner, S. C. Herndon, E. C. Wood, J. P. Franklin, D. R. Worsnop, A. H. Goldstein, and R. A. Harley
Atmos. Chem. Phys., 14, 7585–7599, https://doi.org/10.5194/acp-14-7585-2014, https://doi.org/10.5194/acp-14-7585-2014, 2014
S. Saarikoski, S. Carbone, M. J. Cubison, R. Hillamo, P. Keronen, C. Sioutas, D. R. Worsnop, and J. L. Jimenez
Atmos. Meas. Tech., 7, 2121–2135, https://doi.org/10.5194/amt-7-2121-2014, https://doi.org/10.5194/amt-7-2121-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, and Q. Zhang
Atmos. Chem. Phys., 14, 6477–6494, https://doi.org/10.5194/acp-14-6477-2014, https://doi.org/10.5194/acp-14-6477-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
J. Huttunen, A. Arola, G. Myhre, A. V. Lindfors, T. Mielonen, S. Mikkonen, J. S. Schafer, S. N. Tripathi, M. Wild, M. Komppula, and K. E. J. Lehtinen
Atmos. Chem. Phys., 14, 6103–6110, https://doi.org/10.5194/acp-14-6103-2014, https://doi.org/10.5194/acp-14-6103-2014, 2014
H. Portin, A. Leskinen, L. Hao, A. Kortelainen, P. Miettinen, A. Jaatinen, A. Laaksonen, K. E. J. Lehtinen, S. Romakkaniemi, and M. Komppula
Atmos. Chem. Phys., 14, 6021–6034, https://doi.org/10.5194/acp-14-6021-2014, https://doi.org/10.5194/acp-14-6021-2014, 2014
M. Paglione, S. Saarikoski, S. Carbone, R. Hillamo, M. C. Facchini, E. Finessi, L. Giulianelli, C. Carbone, S. Fuzzi, F. Moretti, E. Tagliavini, E. Swietlicki, K. Eriksson Stenström, A. S. H. Prévôt, P. Massoli, M. Canaragatna, D. Worsnop, and S. Decesari
Atmos. Chem. Phys., 14, 5089–5110, https://doi.org/10.5194/acp-14-5089-2014, https://doi.org/10.5194/acp-14-5089-2014, 2014
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384, https://doi.org/10.5194/amt-7-1377-2014, https://doi.org/10.5194/amt-7-1377-2014, 2014
A. Hirsikko, E. J. O'Connor, M. Komppula, K. Korhonen, A. Pfüller, E. Giannakaki, C. R. Wood, M. Bauer-Pfundstein, A. Poikonen, T. Karppinen, H. Lonka, M. Kurri, J. Heinonen, D. Moisseev, E. Asmi, V. Aaltonen, A. Nordbo, E. Rodriguez, H. Lihavainen, A. Laaksonen, K. E. J. Lehtinen, T. Laurila, T. Petäjä, M. Kulmala, and Y. Viisanen
Atmos. Meas. Tech., 7, 1351–1375, https://doi.org/10.5194/amt-7-1351-2014, https://doi.org/10.5194/amt-7-1351-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä
Atmos. Meas. Tech., 7, 689–700, https://doi.org/10.5194/amt-7-689-2014, https://doi.org/10.5194/amt-7-689-2014, 2014
P. Tiitta, V. Vakkari, P. Croteau, J. P. Beukes, P. G. van Zyl, M. Josipovic, A. D. Venter, K. Jaars, J. J. Pienaar, N. L. Ng, M. R. Canagaratna, J. T. Jayne, V.-M. Kerminen, H. Kokkola, M. Kulmala, A. Laaksonen, D. R. Worsnop, and L. Laakso
Atmos. Chem. Phys., 14, 1909–1927, https://doi.org/10.5194/acp-14-1909-2014, https://doi.org/10.5194/acp-14-1909-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
T. Korhola, H. Kokkola, H. Korhonen, A.-I. Partanen, A. Laaksonen, K. E. J. Lehtinen, and S. Romakkaniemi
Geosci. Model Dev., 7, 161–174, https://doi.org/10.5194/gmd-7-161-2014, https://doi.org/10.5194/gmd-7-161-2014, 2014
V. Cesnulyte, A. V. Lindfors, M. R. A. Pitkänen, K. E. J. Lehtinen, J.-J. Morcrette, and A. Arola
Atmos. Chem. Phys., 14, 593–608, https://doi.org/10.5194/acp-14-593-2014, https://doi.org/10.5194/acp-14-593-2014, 2014
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
A. Lipponen, V. Kolehmainen, S. Romakkaniemi, and H. Kokkola
Geosci. Model Dev., 6, 2087–2098, https://doi.org/10.5194/gmd-6-2087-2013, https://doi.org/10.5194/gmd-6-2087-2013, 2013
A. I. Partanen, A. Laakso, A. Schmidt, H. Kokkola, T. Kuokkanen, J.-P. Pietikäinen, V.-M. Kerminen, K. E. J. Lehtinen, L. Laakso, and H. Korhonen
Atmos. Chem. Phys., 13, 12059–12071, https://doi.org/10.5194/acp-13-12059-2013, https://doi.org/10.5194/acp-13-12059-2013, 2013
L. R. Williams, L. A. Gonzalez, J. Peck, D. Trimborn, J. McInnis, M. R. Farrar, K. D. Moore, J. T. Jayne, W. A. Robinson, D. K. Lewis, T. B. Onasch, M. R. Canagaratna, A. Trimborn, M. T. Timko, G. Magoon, R. Deng, D. Tang, E. de la Rosa Blanco, A. S. H. Prévôt, K. A. Smith, and D. R. Worsnop
Atmos. Meas. Tech., 6, 3271–3280, https://doi.org/10.5194/amt-6-3271-2013, https://doi.org/10.5194/amt-6-3271-2013, 2013
R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, A. S. H. Prévôt, U. Baltensperger, J. Schneider, J. R. Kimmel, M. Gonin, U. Rohner, D. R. Worsnop, and J. T. Jayne
Atmos. Meas. Tech., 6, 3225–3241, https://doi.org/10.5194/amt-6-3225-2013, https://doi.org/10.5194/amt-6-3225-2013, 2013
J. Kontkanen, K. E. J. Lehtinen, T. Nieminen, H. E. Manninen, K. Lehtipalo, V.-M. Kerminen, and M. Kulmala
Atmos. Chem. Phys., 13, 11391–11401, https://doi.org/10.5194/acp-13-11391-2013, https://doi.org/10.5194/acp-13-11391-2013, 2013
G. S. Stuart, R. G. Stevens, A.-I. Partanen, A. K. L. Jenkins, H. Korhonen, P. M. Forster, D. V. Spracklen, and J. R. Pierce
Atmos. Chem. Phys., 13, 10385–10396, https://doi.org/10.5194/acp-13-10385-2013, https://doi.org/10.5194/acp-13-10385-2013, 2013
M. R. Pennington, B. R. Bzdek, J. W. DePalma, J. N. Smith, A.-M. Kortelainen, L. Hildebrandt Ruiz, T. Petäjä, M. Kulmala, D. R. Worsnop, and M. V. Johnston
Atmos. Chem. Phys., 13, 10215–10225, https://doi.org/10.5194/acp-13-10215-2013, https://doi.org/10.5194/acp-13-10215-2013, 2013
M. Dall'Osto, X. Querol, A. Alastuey, M. C. Minguillon, M. Alier, F. Amato, M. Brines, M. Cusack, J. O. Grimalt, A. Karanasiou, T. Moreno, M. Pandolfi, J. Pey, C. Reche, A. Ripoll, R. Tauler, B. L. Van Drooge, M. Viana, R. M. Harrison, J. Gietl, D. Beddows, W. Bloss, C. O'Dowd, D. Ceburnis, G. Martucci, N. L. Ng, D. Worsnop, J. Wenger, E. Mc Gillicuddy, J. Sodeau, R. Healy, F. Lucarelli, S. Nava, J. L. Jimenez, F. Gomez Moreno, B. Artinano, A. S. H. Prévôt, L. Pfaffenberger, S. Frey, F. Wilsenack, D. Casabona, P. Jiménez-Guerrero, D. Gross, and N. Cots
Atmos. Chem. Phys., 13, 8991–9019, https://doi.org/10.5194/acp-13-8991-2013, https://doi.org/10.5194/acp-13-8991-2013, 2013
A. Arola, T. F. Eck, J. Huttunen, K. E. J. Lehtinen, A. V. Lindfors, G. Myhre, A. Smirnov, S. N. Tripathi, and H. Yu
Atmos. Chem. Phys., 13, 7895–7901, https://doi.org/10.5194/acp-13-7895-2013, https://doi.org/10.5194/acp-13-7895-2013, 2013
H. Keskinen, A. Virtanen, J. Joutsensaari, G. Tsagkogeorgas, J. Duplissy, S. Schobesberger, M. Gysel, F. Riccobono, J. G. Slowik, F. Bianchi, T. Yli-Juuti, K. Lehtipalo, L. Rondo, M. Breitenlechner, A. Kupc, J. Almeida, A. Amorim, E. M. Dunne, A. J. Downard, S. Ehrhart, A. Franchin, M.K. Kajos, J. Kirkby, A. Kürten, T. Nieminen, V. Makhmutov, S. Mathot, P. Miettinen, A. Onnela, T. Petäjä, A. Praplan, F. D. Santos, S. Schallhart, M. Sipilä, Y. Stozhkov, A. Tomé, P. Vaattovaara, D. Wimmer, A. Prevot, J. Dommen, N. M. Donahue, R.C. Flagan, E. Weingartner, Y. Viisanen, I. Riipinen, A. Hansel, J. Curtius, M. Kulmala, D. R. Worsnop, U. Baltensperger, H. Wex, F. Stratmann, and A. Laaksonen
Atmos. Chem. Phys., 13, 5587–5600, https://doi.org/10.5194/acp-13-5587-2013, https://doi.org/10.5194/acp-13-5587-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
J. E. Shilling, R. A. Zaveri, J. D. Fast, L. Kleinman, M. L. Alexander, M. R. Canagaratna, E. Fortner, J. M. Hubbe, J. T. Jayne, A. Sedlacek, A. Setyan, S. Springston, D. R. Worsnop, and Q. Zhang
Atmos. Chem. Phys., 13, 2091–2113, https://doi.org/10.5194/acp-13-2091-2013, https://doi.org/10.5194/acp-13-2091-2013, 2013
J. Leppä, S. Gagné, L. Laakso, H. E. Manninen, K. E. J. Lehtinen, M. Kulmala, and V.-M. Kerminen
Atmos. Chem. Phys., 13, 463–486, https://doi.org/10.5194/acp-13-463-2013, https://doi.org/10.5194/acp-13-463-2013, 2013
V.-M. Kerminen, M. Paramonov, T. Anttila, I. Riipinen, C. Fountoukis, H. Korhonen, E. Asmi, L. Laakso, H. Lihavainen, E. Swietlicki, B. Svenningsson, A. Asmi, S. N. Pandis, M. Kulmala, and T. Petäjä
Atmos. Chem. Phys., 12, 12037–12059, https://doi.org/10.5194/acp-12-12037-2012, https://doi.org/10.5194/acp-12-12037-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Photo-induced shrinking of aqueous glycine aerosol droplets
Sulfate formation via aerosol-phase SO2 oxidation by model biomass burning photosensitizers: 3,4-dimethoxybenzaldehyde, vanillin and syringaldehyde using single-particle mixing-state analysis
Yields and molecular composition of gas-phase and secondary organic aerosol from the photooxidation of the volatile consumer product benzyl alcohol: formation of highly oxygenated and hydroxy nitro-aromatic compounds
A combined gas- and particle-phase analysis of highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis
Photoaging of Phenolic Secondary Organic Aerosol in the Aqueous Phase: Evolution of Chemical and Optical Properties and Effects of Oxidants
Comparison of aqueous secondary organic aerosol (aqSOA) product distributions from guaiacol oxidation by non-phenolic and phenolic methoxybenzaldehydes as photosensitizers in the absence and presence of ammonium nitrate
Technical note: Chemical composition and source identification of fluorescent components in atmospheric water-soluble brown carbon by excitation–emission matrix spectroscopy with parallel factor analysis – potential limitations and applications
Insoluble lipid film mediates transfer of soluble saccharides from the sea to the atmosphere: the role of hydrogen bonding
Simultaneous Formation of Sulfate and Nitrate via Co-uptake of SO2 and NO2 by Aqueous NaCl Droplets: Combined Effect of Nitrate Photolysis and Chlorine Chemistry
Measurement Report: Atmospheric aging of combustion-derived particles: impact on stable free radical concentration and its ability to produce reactive oxygen species in aqueous media
Magnetic fraction of the atmospheric dust in Kraków – physicochemical characteristics and possible environmental impact
Modeling daytime and nighttime secondary organic aerosol formation via multiphase reactions of biogenic hydrocarbons
SO2 enhances aerosol formation from anthropogenic volatile organic compound ozonolysis by producing sulfur-containing compounds
Isothermal evaporation of α-pinene secondary organic aerosol particles formed under low NOx and high NOx conditions
Chemical characterization of organic compounds involved in iodine-initiated new particle formation from coastal macroalgal emission
The Urmia playa as a source of airborne dust and ice-nucleating particles – Part 2: Unraveling the relationship between soil dust composition and ice nucleation activity
Winter brown carbon over six of China's megacities: light absorption, molecular characterization, and improved source apportionment revealed by multilayer perceptron neural network
Chamber investigation of the formation and transformation of secondary organic aerosol in mixtures of biogenic and anthropogenic volatile organic compounds
Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types
Comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) from heavy-duty diesel vehicles using two-dimensional gas chromatography time-of-flight mass spectrometry
Measurement report: Investigation of pH- and particle-size-dependent chemical and optical properties of water-soluble organic carbon: implications for its sources and aging processes
The influence of the addition of isoprene on the volatility of particles formed from the photo-oxidation of anthropogenic–biogenic mixtures
Significant formation of sulfate aerosols contributed by the heterogeneous drivers of dust surface
Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime
Particle-phase processing of α-pinene NO3 secondary organic aerosol in the dark
Chemical characteristics and sources of PM2.5 in Hohhot, a semi-arid city in northern China: insight from the COVID-19 lockdown
The positive effect of formaldehyde on the photocatalytic renoxification of nitrate on TiO2 particles
Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical
A comprehensive study on hygroscopic behaviour and nitrate depletion of NaNO3 and dicarboxylic acid mixtures: implications for nitrate depletion in tropospheric aerosols
Secondary organic aerosols from OH oxidation of cyclic volatile methyl siloxanes as an important Si source in the atmosphere
An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles
Effects of OH radical and SO2 concentrations on photochemical reactions of mixed anthropogenic organic gases
Chemically distinct particle phase emissions from highly controlled pyrolysis of three wood types
Effects of the sample matrix on the photobleaching and photodegradation of toluene-derived secondary organic aerosol compounds
Functionality-based formation of secondary organic aerosol from m-xylene photooxidation
Chemical composition of secondary organic aerosol particles formed from mixtures of anthropogenic and biogenic precursors
A novel pathway of atmospheric sulfate formation through carbonate radicals
A sulfuric acid nucleation potential model for the atmosphere
Optical and chemical properties and oxidative potential of aqueous-phase products from OH and 3C∗-initiated photooxidation of eugenol
The relationship between PM2.5 and anticyclonic wave activity during summer over the United States
Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions
Cellulose in atmospheric particulate matter at rural and urban sites across France and Switzerland
Kinetics, SOA yields, and chemical composition of secondary organic aerosol from β-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K
Chemical transformation of α-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates
Aqueous chemical bleaching of 4-nitrophenol brown carbon by hydroxyl radicals; products, mechanism, and light absorption
Secondary organic aerosol formation from camphene oxidation: measurements and modeling
Technical note: Real-time diagnosis of the hygroscopic growth micro-dynamics of nanoparticles with Fourier transform infrared spectroscopy
Single-particle Raman spectroscopy for studying physical and chemical processes of atmospheric particles
Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?
Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates
Shinnosuke Ishizuka, Oliver Reich, Grégory David, and Ruth Signorell
Atmos. Chem. Phys., 23, 5393–5402, https://doi.org/10.5194/acp-23-5393-2023, https://doi.org/10.5194/acp-23-5393-2023, 2023
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Photosensitizers play an important role in the photochemistry of atmospheric aerosols. Our study provides evidence that mesoscopic glycine clusters forming in aqueous droplets act as unconventional photosensitizers in the visible light spectrum. We observed the influence of these photoactive molecular aggregates in single optically trapped aqueous droplets. Such mesoscopic photosensitizers might be more important for aerosol photochemistry than previously anticipated.
Liyuan Zhou, Zhancong Liang, Beatrix Rosette Go Mabato, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, and Chak K. Chan
Atmos. Chem. Phys., 23, 5251–5261, https://doi.org/10.5194/acp-23-5251-2023, https://doi.org/10.5194/acp-23-5251-2023, 2023
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This study reveals the sulfate formation in photosensitized particles from biomass burning under UV and SO2, of which the relative atmospheric importance in sulfate production was qualitatively compared to nitrate photolysis. On the basis of single-particle aerosol mass spectrometry measurements, the number percentage of sulfate-containing particles and relative peak area of sulfate in single-particle spectra exhibited a descending order of 3,4-dimethoxybenzaldehyde > vanillin > syringaldehyde.
Mohammed Jaoui, Kenneth S. Docherty, Michael Lewandowski, and Tadeusz E. Kleindienst
Atmos. Chem. Phys., 23, 4637–4661, https://doi.org/10.5194/acp-23-4637-2023, https://doi.org/10.5194/acp-23-4637-2023, 2023
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VCPs are a class of chemicals widely used in industrial and consumer products (e.g., coatings, adhesives, inks, personal care products) and are an important component of total VOCs in urban atmospheres. This study provides SOA yields and detailed chemical analysis of the gas- and aerosol-phase products of the photooxidation of one of these VCPs, benzyl alcohol. These results will allow better links between characterized sources and their resulting criteria for pollutant formation.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Wenqing Jiang, Christopher Niedek, Cort Anastasio, and Qi Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-443, https://doi.org/10.5194/egusphere-2023-443, 2023
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Aqueous-phase aging can affect the composition and properties of secondary organic aerosol (SOA). Our photochemical aging experiments of phenolic aqSOA show that fragmentation and evaporation of volatile products dominate the aqSOA aging, leading to significant loss of aqSOA mass and photobleaching. Elevated oxidant concentration can accelerate the evolution of the aqSOA during photoaging.
Beatrix Rosette Go Mabato, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak K. Chan
Atmos. Chem. Phys., 23, 2859–2875, https://doi.org/10.5194/acp-23-2859-2023, https://doi.org/10.5194/acp-23-2859-2023, 2023
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We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud and fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings are useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA predictive models.
Tao Cao, Meiju Li, Cuncun Xu, Jianzhong Song, Xingjun Fan, Jun Li, Wanglu Jia, and Ping'an Peng
Atmos. Chem. Phys., 23, 2613–2625, https://doi.org/10.5194/acp-23-2613-2023, https://doi.org/10.5194/acp-23-2613-2023, 2023
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This work comprehensively investigated the fluorescence data of light-absorbing organic compounds, water-soluble organic matter in different types of aerosol samples, soil dust, and fulvic and humic acids using an excitation–emission matrix (EEM) method and parallel factor modeling. The results revealed which light-absorbing species can be detected by EEM and also provided important information for identifying the chemical composition and possible sources of these species in atmospheric samples.
Minglan Xu, Narcisse Tsona Tchinda, Jianlong Li, and Lin Du
Atmos. Chem. Phys., 23, 2235–2249, https://doi.org/10.5194/acp-23-2235-2023, https://doi.org/10.5194/acp-23-2235-2023, 2023
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The promotion of soluble saccharides on sea spray aerosol (SSA) generation and the changes in particle morphology were observed. On the contrary, the coexistence of surface insoluble fatty acid film and soluble saccharides significantly inhibited the production of SSA. This is the first demonstration that hydrogen bonding mediated by surface-insoluble fatty acids contributes to saccharide transfer in seawater, providing a new mechanism for saccharide enrichment in SSA.
Ruifeng Zhang and Chak Keung Chan
EGUsphere, https://doi.org/10.5194/egusphere-2023-223, https://doi.org/10.5194/egusphere-2023-223, 2023
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Research in sulfate and nitrate formation from co-uptake of NO2 and SO2, especially under irradiation, is rare. We studied the co-uptake of NO2 and SO2 by NaCl droplets under various conditions, including irradiation/dark and different RHs, using Raman spectroscopy/Flow cell and kinetic model simulation. A significant nitrate from NO2 hydrolysis can be photolyzed to generate OH radicals that can further react with chloride to produce reactive chlorine species and promote sulfate formation.
Heather L. Runberg and Brian J. Majestic
EGUsphere, https://doi.org/10.5194/egusphere-2023-4, https://doi.org/10.5194/egusphere-2023-4, 2023
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Environmentally persistent free radicals (EPFR) are an emerging pollutant found in soot particles. Understanding how these change as they move through the atmosphere is important to human health. Here, soot was generated in the laboratory and exposed to simulated sunlight. The concentrations and characteristics of EPFR in the soot was measured and found to be unchanged. However, it was also found that the ability of soot to form hydroxyl radicals was stronger for fresh soot.
Jan M. Michalik, Wanda Wilczyńska-Michalik, Łukasz Gondek, Waldemar Tokarz, Jan Żukrowski, Marta Gajewska, and Marek Michalik
Atmos. Chem. Phys., 23, 1449–1464, https://doi.org/10.5194/acp-23-1449-2023, https://doi.org/10.5194/acp-23-1449-2023, 2023
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The magnetic fraction of the aerosols in Kraków was collected and analysed using scanning and transmission electron microscopy with energy-dispersive spectrometry, X-ray diffraction, Mössbauer spectrometry, and magnetometry. It contains metallic Fe or Fe-rich alloy and Fe oxides. The occurrence of nanometre-scale Fe3O4 particles (predominantly of anthropogenic origin) is shown. Our results can help to determine the sources and transport of pollutants, potential harmful effects, etc.
Sanghee Han and Myoseon Jang
Atmos. Chem. Phys., 23, 1209–1226, https://doi.org/10.5194/acp-23-1209-2023, https://doi.org/10.5194/acp-23-1209-2023, 2023
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The diurnal pattern in biogenic secondary organic aerosol (SOA) formation is simulated by using the UNIPAR model, which predicts SOA growth via multiphase reactions of hydrocarbons under varying NOx levels, aerosol acidity, humidity, and temperature. The simulation suggests that nighttime SOA formation, even in urban environments, where anthropogenic emission is high, is dominated by products from ozonolysis and NO3-initiated oxidation of biogenic hydrocarbons.
Zhaomin Yang, Kun Li, Narcisse T. Tsona, Xin Luo, and Lin Du
Atmos. Chem. Phys., 23, 417–430, https://doi.org/10.5194/acp-23-417-2023, https://doi.org/10.5194/acp-23-417-2023, 2023
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SO2 significantly promotes particle formation during cyclooctene ozonolysis. Carboxylic acids and their dimers were major products in particles formed in the absence of SO2. SO2 can induce production of organosulfates with stronger particle formation ability than their precursors, leading to the enhancement in particle formation. Formation mechanisms and structures of organosulfates were proposed, which is helpful for better understanding how SO2 perturbs the formation and fate of particles.
Zijun Li, Angela Buchholz, Luis M. F. Barreira, Arttu Ylisirniö, Liqing Hao, Iida Pullinen, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 23, 203–220, https://doi.org/10.5194/acp-23-203-2023, https://doi.org/10.5194/acp-23-203-2023, 2023
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Interaction between NOx and biogenic emissions can be important in suburban areas. Our study showed that the addition of NOx during α-pinene SOA formation produced considerable amounts of organic nitrates and affected the composition of non-nitrated organic compounds. The compositional difference consequently altered the primary type of aqueous-phase processes during the isothermal particle evaporation.
Yibei Wan, Xiangpeng Huang, Chong Xing, Qiongqiong Wang, Xinlei Ge, and Huan Yu
Atmos. Chem. Phys., 22, 15413–15423, https://doi.org/10.5194/acp-22-15413-2022, https://doi.org/10.5194/acp-22-15413-2022, 2022
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The organic compounds involved in continental new particle formation have been investigated in depth in the last 2 decades. In contrast, no prior work has studied the exact chemical composition of organic compounds and their role in coastal new particle formation. We present a complementary study to the ongoing laboratory and field research on iodine nucleation in the coastal atmosphere. This study provided a more complete story of coastal I-NPF from low-tide macroalgal emission.
Nikou Hamzehpour, Claudia Marcolli, Kristian Klumpp, Debora Thöny, and Thomas Peter
Atmos. Chem. Phys., 22, 14931–14956, https://doi.org/10.5194/acp-22-14931-2022, https://doi.org/10.5194/acp-22-14931-2022, 2022
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Dust aerosols from dried lakebeds contain mineral particles, as well as soluble salts and (bio-)organic compounds. Here, we investigate ice nucleation (IN) activity of dust samples from Lake Urmia playa, Iran. We find high IN activity of the untreated samples that decreases after organic matter removal but increases after removing soluble salts and carbonates, evidencing inhibiting effects of soluble salts and carbonates on the IN activity of organic matter and minerals, especially microcline.
Diwei Wang, Zhenxing Shen, Qian Zhang, Yali Lei, Tian Zhang, Shasha Huang, Jian Sun, Hongmei Xu, and Junji Cao
Atmos. Chem. Phys., 22, 14893–14904, https://doi.org/10.5194/acp-22-14893-2022, https://doi.org/10.5194/acp-22-14893-2022, 2022
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The optical properties and molecular structure of atmospheric brown carbon (BrC) in winter of several megacities in China were analyzed, and the source contribution of brown carbon was improved by using positive matrix factorization coupled with a multilayer perceptron neural network. These results can provide a basis for the more effective control of BrC to reduce its impacts on regional climates and human health.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 22, 14147–14175, https://doi.org/10.5194/acp-22-14147-2022, https://doi.org/10.5194/acp-22-14147-2022, 2022
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Mixing experiments are crucial and highly beneficial for our understanding of atmospheric chemical interactions. However, interpretation quickly becomes complex, and both the experimental design and evaluation need to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in SOA formed from mixtures of VOCs.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys., 22, 13783–13796, https://doi.org/10.5194/acp-22-13783-2022, https://doi.org/10.5194/acp-22-13783-2022, 2022
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The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types that are internally mixed within individual particles.
Xiao He, Xuan Zheng, Shaojun Zhang, Xuan Wang, Ting Chen, Xiao Zhang, Guanghan Huang, Yihuan Cao, Liqiang He, Xubing Cao, Yuan Cheng, Shuxiao Wang, and Ye Wu
Atmos. Chem. Phys., 22, 13935–13947, https://doi.org/10.5194/acp-22-13935-2022, https://doi.org/10.5194/acp-22-13935-2022, 2022
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With the use of two-dimensional gas chromatography time-of-flight mass spectrometry (GC × GC ToF-MS), we successfully give a comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emitted from heavy-duty diesel vehicles. I/SVOCs are speciated, identified, and quantified based on the patterns of the mass spectrum, and the gas–particle partitioning is fully addressed.
Yuanyuan Qin, Juanjuan Qin, Xiaobo Wang, Kang Xiao, Ting Qi, Yuwei Gao, Xueming Zhou, Shaoxuan Shi, Jingnan Li, Jingsi Gao, Ziyin Zhang, Jihua Tan, Yang Zhang, and Rongzhi Chen
Atmos. Chem. Phys., 22, 13845–13859, https://doi.org/10.5194/acp-22-13845-2022, https://doi.org/10.5194/acp-22-13845-2022, 2022
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Deep interrogation of water-soluble organic carbon (WSOC) in aerosols is critical and challenging considering its involvement in many key aerosol-associated chemical reactions. This work examined how the chemical structures (functional groups) and optical properties (UV/fluorescence properties) of WSOC were affected by pH and particle size. We found that the pH- and particle-size-dependent behaviors could be used to reveal the structures, sources, and aging of aerosol WSOC.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Tao Wang, Yangyang Liu, Hanyun Cheng, Zhenzhen Wang, Hongbo Fu, Jianmin Chen, and Liwu Zhang
Atmos. Chem. Phys., 22, 13467–13493, https://doi.org/10.5194/acp-22-13467-2022, https://doi.org/10.5194/acp-22-13467-2022, 2022
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This study compared the gas-phase, aqueous-phase, and heterogeneous SO2 oxidation pathways by combining laboratory work with a modelling study. The heterogeneous oxidation, particularly that induced by the dust surface drivers, presents positive implications for the removal of airborne SO2 and formation of sulfate aerosols. This work highlighted the atmospheric significance of heterogeneous oxidation and suggested a comparison model to evaluate the following heterogeneous laboratory research.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-658, https://doi.org/10.5194/acp-2022-658, 2022
Revised manuscript accepted for ACP
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Haijun Zhou, Tao Liu, Bing Sun, Yongli Tian, Xingjun Zhou, Feng Hao, Xi Chun, Zhiqiang Wan, Peng Liu, Jingwen Wang, and Dagula Du
Atmos. Chem. Phys., 22, 12153–12166, https://doi.org/10.5194/acp-22-12153-2022, https://doi.org/10.5194/acp-22-12153-2022, 2022
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A single year’s offline measurement was conducted in Hohhot to reveal the chemical characteristics and sources of PM2.5 in a semi-arid region. We believe that our study makes a significant contribution to the literature because relatively few studies have focused on the chemical composition and sources of PM2.5 with offline measurements. A knowledge gap exists concerning how chemical composition and sources respond to implemented control measures for aerosols, particularly in a semi-arid region.
Yuhan Liu, Xuejiao Wang, Jing Shang, Weiwei Xu, Mengshuang Sheng, and Chunxiang Ye
Atmos. Chem. Phys., 22, 11347–11358, https://doi.org/10.5194/acp-22-11347-2022, https://doi.org/10.5194/acp-22-11347-2022, 2022
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In this study, the influence of HCHO on renoxification on nitrate-doped TiO2 particles is investigated by using an experimental chamber. Mass NOx release is suggested to follow the NO−3-NO3·-HNO3-NOx pathway, with HCHO involved in the transformation of NO3· to HNO3 through hydrogen abstraction. Our proposed reaction mechanism by which HCHO promotes photocatalytic renoxification is helpful for deeply understanding the atmospheric photochemical processes and nitrogen cycling.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, https://doi.org/10.5194/acp-22-11323-2022, 2022
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The oxidation of limonene, a common volatile emitted by trees and chemical products, by NO3, a nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10-30 compounds. Most of the HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted for a major fraction. Their formation can be explained by chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
Shuaishuai Ma, Qiong Li, and Yunhong Zhang
Atmos. Chem. Phys., 22, 10955–10970, https://doi.org/10.5194/acp-22-10955-2022, https://doi.org/10.5194/acp-22-10955-2022, 2022
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The nitrate phase state can play a critical role in determining the occurrence and extent of nitrate depletion in internally mixed NaNO3–DCA particles, which may be instructive for relevant aerosol reaction systems. Besides, organic acids have a potential to deplete nitrate based on the comprehensive consideration of acidity, particle-phase state, droplet water activity, and HNO3 gas-phase diffusion.
Chong Han, Hongxing Yang, Kun Li, Patrick Lee, John Liggio, Amy Leithead, and Shao-Meng Li
Atmos. Chem. Phys., 22, 10827–10839, https://doi.org/10.5194/acp-22-10827-2022, https://doi.org/10.5194/acp-22-10827-2022, 2022
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We presented yields and compositions of Si-containing SOAs generated from the reaction of cVMSs (D3–D6) with OH radicals. NOx played a negative role in cVMS SOA formation, while ammonium sulfate seeds enhanced D3–D5 SOA yields at short photochemical ages under high-NOx conditions. The aerosol mass spectra confirmed that the components of cVMS SOAs significantly relied on OH exposure. A global cVMS-derived SOA source strength was estimated in order to understand SOA formation potentials of cVMSs.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-498, https://doi.org/10.5194/acp-2022-498, 2022
Revised manuscript accepted for ACP
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In this study, we present an intercomparison study of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Junling Li, Kun Li, Hao Zhang, Xin Zhang, Yuanyuan Ji, Wanghui Chu, Yuxue Kong, Yangxi Chu, Yanqin Ren, Yujie Zhang, Haijie Zhang, Rui Gao, Zhenhai Wu, Fang Bi, Xuan Chen, Xuezhong Wang, Weigang Wang, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 22, 10489–10504, https://doi.org/10.5194/acp-22-10489-2022, https://doi.org/10.5194/acp-22-10489-2022, 2022
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Ozone formation is enhanced by higher OH concentration and higher temperature but is influenced little by SO2. SO2 can largely enhance the particle formation. Organo-sulfates and organo-nitrates are detected in the formed particles, and the presence of SO2 can promote the formation of organo-sulfates. The results provide a scientific basis for systematically evaluating the effects of SO2, OH concentration, and temperature on the oxidation of mixed organic gases in the atmosphere.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-535, https://doi.org/10.5194/acp-2022-535, 2022
Revised manuscript accepted for ACP
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Pyrolysis is the thermal decomposition of fuels like wood, which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to inform both the uncombusted emissions from wild fires, and the fuel that participates in combustion.
Alexandra L. Klodt, Marley Adamek, Monica Dibley, Sergey A. Nizkorodov, and Rachel E. O'Brien
Atmos. Chem. Phys., 22, 10155–10171, https://doi.org/10.5194/acp-22-10155-2022, https://doi.org/10.5194/acp-22-10155-2022, 2022
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We investigated photochemistry of a secondary organic aerosol under three different conditions: in a dilute aqueous solution mimicking cloud droplets, in a solution of concentrated ammonium sulfate mimicking deliquesced aerosol, and in an organic matrix mimicking dry organic aerosol. We find that rate and mechanisms of photochemistry depend sensitively on these conditions, suggesting that the same organic aerosol compounds will degrade at different rates depending on their local environment.
Yixin Li, Jiayun Zhao, Mario Gomez-Hernandez, Michael Lavallee, Natalie M. Johnson, and Renyi Zhang
Atmos. Chem. Phys., 22, 9843–9857, https://doi.org/10.5194/acp-22-9843-2022, https://doi.org/10.5194/acp-22-9843-2022, 2022
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Here we elucidate the production of COOs and their roles in SOA and brown carbon formation from m-xylene oxidation by simultaneously monitoring the evolution of gas-phase products and aerosol properties in an environmental chamber. A kinetic framework is developed to predict SOA production from the concentrations and uptake coefficients for COOs. This functionality-based approach reproduces SOA formation from m-xylene oxidation well and is applicable to VOC oxidation for other species.
Yunqi Shao, Aristeidis Voliotis, Mao Du, Yu Wang, Kelly Pereira, Jacqueline Hamilton, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 9799–9826, https://doi.org/10.5194/acp-22-9799-2022, https://doi.org/10.5194/acp-22-9799-2022, 2022
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This study explored the chemical properties of secondary organic aerosol (SOA) that formed from photo-oxidation of single and mixed biogenic and anthropogenic precursors. We showed that SOA chemical properties in a mixed vapour system are mainly affected by the
higher-yield precursor's oxidation products and products from
cross-product formation. This study also identifies potential tracer compounds in a mixed vapour system that might be used in SOA source attribution in future ambient studies.
Yangyang Liu, Yue Deng, Jiarong Liu, Xiaozhong Fang, Tao Wang, Kejian Li, Kedong Gong, Aziz U. Bacha, Iqra Nabi, Qiuyue Ge, Xiuhui Zhang, Christian George, and Liwu Zhang
Atmos. Chem. Phys., 22, 9175–9197, https://doi.org/10.5194/acp-22-9175-2022, https://doi.org/10.5194/acp-22-9175-2022, 2022
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Both CO2 and carbonate salt work as the precursor of carbonate radicals, which largely promotes sulfate formation during the daytime. This study provides the first indication that the carbonate radical not only plays a role as an intermediate in tropospheric anion chemistry but also as a strong oxidant for the surface processing of trace gas in the atmosphere. CO2, carbponate radicals, and sulfate receive attention from those looking at the environment, atmosphere, aerosol, and photochemistry.
Jack S. Johnson and Coty N. Jen
Atmos. Chem. Phys., 22, 8287–8297, https://doi.org/10.5194/acp-22-8287-2022, https://doi.org/10.5194/acp-22-8287-2022, 2022
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Sulfuric acid nucleation forms particles in Earth's atmosphere that influence cloud formation and climate. This study introduces the Nucleation Potential Model, which simplifies the diverse reactions between sulfuric acid and numerous precursor gases to predict nucleation rates. Results show that the model is capable of estimating the potency and concentration of mixtures of precursor gases from laboratory and field observations and can be used to model nucleation across diverse environments.
Xudong Li, Ye Tao, Longwei Zhu, Shuaishuai Ma, Shipeng Luo, Zhuzi Zhao, Ning Sun, Xinlei Ge, and Zhaolian Ye
Atmos. Chem. Phys., 22, 7793–7814, https://doi.org/10.5194/acp-22-7793-2022, https://doi.org/10.5194/acp-22-7793-2022, 2022
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This work has, for the first time, investigated the optical and chemical properties and oxidative potential of aqueous-phase photooxidation products of eugenol (a biomass-burning-emitted compound) and elucidated the interplay among these properties. Large mass yields exceeding 100 % were found, and the aqueous processing is a source of BrC (likely relevant with humic-like substances). We also show that aqueous processing can produce species that are more toxic than that of its precursor.
Ye Wang, Natalie Mahowald, Peter Hess, Wenxiu Sun, and Gang Chen
Atmos. Chem. Phys., 22, 7575–7592, https://doi.org/10.5194/acp-22-7575-2022, https://doi.org/10.5194/acp-22-7575-2022, 2022
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PM2.5 is positively related to anticyclonic wave activity (AWA) changes close to the observing sites. Changes between current and future climates in AWA can explain up to 75 % of PM2.5 variability at some stations using a linear regression model. Our analysis indicates that higher PM2.5 concentrations occur when a positive AWA anomaly is prominent, which could be critical for understanding how pollutants respond to changing atmospheric circulation and for developing robust pollution projections.
Clarissa Baldo, Akinori Ito, Michael D. Krom, Weijun Li, Tim Jones, Nick Drake, Konstantin Ignatyev, Nicholas Davidson, and Zongbo Shi
Atmos. Chem. Phys., 22, 6045–6066, https://doi.org/10.5194/acp-22-6045-2022, https://doi.org/10.5194/acp-22-6045-2022, 2022
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High ionic strength relevant to the aerosol-water enhanced proton-promoted dissolution of iron in coal fly ash (up to 7 times) but suppressed oxalate-promoted dissolution at low pH (< 3). Fe in coal fly ash dissolved up to 7 times faster than in Saharan dust at low pH. A global model with the updated dissolution rates of iron in coal fly ash suggested a larger contribution of pyrogenic dissolved Fe over regions with a strong impact from fossil fuel combustions.
Adam Brighty, Véronique Jacob, Gaëlle Uzu, Lucille Borlaza, Sébastien Conil, Christoph Hueglin, Stuart K. Grange, Olivier Favez, Cécile Trébuchon, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 6021–6043, https://doi.org/10.5194/acp-22-6021-2022, https://doi.org/10.5194/acp-22-6021-2022, 2022
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With an revised analytical method and long-term sampling strategy, we have been able to elucidate much more information about atmospheric plant debris, a poorly understood class of particulate matter. We found weaker seasonal patterns at urban locations compared to rural locations and significant interannual variability in concentrations between previous years and 2020, during the COVID-19 pandemic. This suggests a possible man-made influence on plant debris concentration and source strength.
Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
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We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
Rongshuang Xu, Sze In Madeleine Ng, Wing Sze Chow, Yee Ka Wong, Yuchen Wang, Donger Lai, Zhongping Yao, Pui-Kin So, Jian Zhen Yu, and Man Nin Chan
Atmos. Chem. Phys., 22, 5685–5700, https://doi.org/10.5194/acp-22-5685-2022, https://doi.org/10.5194/acp-22-5685-2022, 2022
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To date, while over a hundred organosulfates (OSs) have been detected in atmospheric aerosols, many of them are still unidentified, with unknown precursors and formation processes. We found the heterogeneous OH oxidation of an α-pinene-derived organosulfate (C10H17O5SNa, αpOS-249, αpOS-249) can proceed at an efficient rate and transform into more oxygenated OSs, which have been commonly detected in atmospheric aerosols and α-pinene-derived SOA in chamber studies.
Bartłomiej Witkowski, Priyanka Jain, and Tomasz Gierczak
Atmos. Chem. Phys., 22, 5651–5663, https://doi.org/10.5194/acp-22-5651-2022, https://doi.org/10.5194/acp-22-5651-2022, 2022
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This article describes a comprehensive investigation of the aqueous oxidation of 4-nitrophenol (4NP) by hydroxyl radicals (OH). The reaction was carried out in a laboratory photoreactor. We report the formation of key intermediates under different pH conditions and the evolution of the light absorption of the reaction solution. The results provide new insights into the formation and removal (chemical bleaching) of light-absorbing organic aerosols (atmospheric brown carbon).
Qi Li, Jia Jiang, Isaac K. Afreh, Kelley C. Barsanti, and David R. Cocker III
Atmos. Chem. Phys., 22, 3131–3147, https://doi.org/10.5194/acp-22-3131-2022, https://doi.org/10.5194/acp-22-3131-2022, 2022
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Chamber-derived secondary organic aerosol (SOA) yields from camphene are reported for the first time. The role of peroxy radicals (RO2) was investigated using chemically detailed box models. We observed higher SOA yields (up to 64 %) in the experiments with added NOx than without due to the formation of highly oxygenated organic molecules (HOMs) when
NOx is present. This work can improve the representation of camphene in air quality models and provide insights into other monoterpene studies.
Xiuli Wei, Haosheng Dai, Huaqiao Gui, Jiaoshi Zhang, Yin Cheng, Jie Wang, Yixin Yang, Youwen Sun, and Jianguo Liu
Atmos. Chem. Phys., 22, 3097–3109, https://doi.org/10.5194/acp-22-3097-2022, https://doi.org/10.5194/acp-22-3097-2022, 2022
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We demonstrated the usage of the Fourier transform infrared (FTIR) spectroscopic technique to characterize in real time the hygroscopic growth properties of nanoparticles and their phase transition micro-dynamics at the molecular level. We first realize real-time measurements of water content and dry nanoparticle mass to characterize hygroscopic growth factors. We then identify in real time the hydration interactions and the dynamic hygroscopic growth process of the functional groups.
Zhancong Liang, Yangxi Chu, Masao Gen, and Chak K. Chan
Atmos. Chem. Phys., 22, 3017–3044, https://doi.org/10.5194/acp-22-3017-2022, https://doi.org/10.5194/acp-22-3017-2022, 2022
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The properties and fate of individual airborne particles can be significantly different, leading to distinct environmental impacts (e.g., climate and human health). While many instruments only analyze an ensemble of these particles, single-particle Raman spectroscopy enables unambiguous characterization of individual particles. This paper comprehensively reviews the applications of such a technique in studying atmospheric particles, especially for their physicochemical processing.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Short summary
Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
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