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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Jaakko Ahola, Hannele Korhonen, Juha Tonttila, Sami Romakkaniemi, Harri Kokkola, and Tomi Raatikainen
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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
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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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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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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
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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
Jutta Kesti, Ewan J. O'Connor, Anne Hirsikko, John Backman, Maria Filioglou, Anu-Maija Sundström, Juha Tonttila, Heikki Lihavainen, Hannele Korhonen, and Eija Asmi
Atmos. Chem. Phys., 24, 9369–9386, https://doi.org/10.5194/acp-24-9369-2024, https://doi.org/10.5194/acp-24-9369-2024, 2024
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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 particle transportation 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.
Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
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We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Harri Kokkola, Juha Tonttila, Silvia Calderón, Sami Romakkaniemi, Antti Lipponen, Aapo Peräkorpi, Tero Mielonen, Edward Gryspeerdt, Timo H. Virtanen, Pekka Kolmonen, and Antti Arola
EGUsphere, https://doi.org/10.5194/egusphere-2024-1964, https://doi.org/10.5194/egusphere-2024-1964, 2024
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Understanding how atmospheric aerosols affect clouds is a scientific challenge. One question is how aerosols affects the amount cloud water. We used a cloud-scale model to study these effects on marine clouds. The study showed that variations in cloud properties and instrument noise can cause bias in satellite derived cloud water content. However, our results suggest that for similar weather conditions with well-defined aerosol concentrations, satellite data can reliably track these effects.
Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-15, https://doi.org/10.5194/ar-2024-15, 2024
Revised manuscript accepted for AR
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This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto-La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes Kaiser, Zak Kipling, Harri Kokkola, Xiaohong Liu, Keren Mezuman, Tero Mielonen, Gunnar Myhre, Xiaohua Pan, Anna Protonotariou, Samuel Remy, Ragnhild Bieltvedt Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Hailong Wang, Duncan Watson-Parris, and Kai Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1487, https://doi.org/10.5194/egusphere-2024-1487, 2024
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We compared smoke plume simulations from 11 global models to each other and to satellite smoke-amount observations, aimed at constraining smoke source strength. In regions where plumes are thick and background aerosol is low, models and satellites compare well. However, the input emission inventory tends to underestimate in many places, and particle property and loss-rate assumptions vary enormously among models, causing uncertainties that require systematic in-situ measurements to resolve.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yi Yuan, Junchen Guo, Yuyang Li, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1325, https://doi.org/10.5194/egusphere-2024-1325, 2024
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Online Vocus-PTR measurements show the compositions and seasonal variations of organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various sub-ppt level species and organics with multiple oxygens (≥3) were discovered. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens. While in other seasons, the variations of them could be influenced by primary emissions.
Marje Prank, Juha Tonttila, Xiaoxia Shang, Sami Romakkaniemi, and Tomi Raatikainen
EGUsphere, https://doi.org/10.5194/egusphere-2024-876, https://doi.org/10.5194/egusphere-2024-876, 2024
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Large primary bioparticles such as pollen can be abundant in the atmosphere. In humid conditions pollens can rupture and release a large number of fine sub-pollen particles (SPPs). The paper investigates what kind of birch pollen concentrations are needed for the pollen and SPPs to start playing a noticeable role in cloud processes and alter precipitation formation. In the studied cases only the largest observed pollen concentrations were able to noticeably alter the precipitation formation.
Anton Laakso, Daniele Visioni, Ulrike Niemeier, Simone Tilmes, and Harri Kokkola
Earth Syst. Dynam., 15, 405–427, https://doi.org/10.5194/esd-15-405-2024, https://doi.org/10.5194/esd-15-405-2024, 2024
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This study is the second in a two-part series in which we explore the dependency of the impacts of stratospheric sulfur injections on both the model employed and the strategy of injection utilized. The study uncovers uncertainties associated with these techniques to cool climate, highlighting how the simulated climate impacts are dependent on both the selected model and the magnitude of the injections. We also show that estimating precipitation impacts of aerosol injection is a complex task.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
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The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Mahen Konwar, Benjamin Werden, Edward C. Fortner, Sudarsan Bera, Mercy Varghese, Subharthi Chowdhuri, Kurt Hibert, Philip Croteau, John Jayne, Manjula Canagaratna, Neelam Malap, Sandeep Jayakumar, Shivsai A. Dixit, Palani Murugavel, Duncan Axisa, Darrel Baumgardner, Peter F. DeCarlo, Doug R. Worsnop, and Thara Prabhakaran
Atmos. Meas. Tech., 17, 2387–2400, https://doi.org/10.5194/amt-17-2387-2024, https://doi.org/10.5194/amt-17-2387-2024, 2024
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In a warm cloud seeding experiment hygroscopic particles are released to alter cloud processes to induce early raindrops. During the Cloud–Aerosol Interaction and Precipitation Enhancement Experiment, airborne mini aerosol mass spectrometers analyse the particles on which clouds form. The seeded clouds showed higher concentrations of chlorine and potassium, the oxidizing agents of flares. Small cloud droplet concentrations increased, and seeding particles were detected in deep cloud depths.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
Atmos. Chem. Phys., 24, 4591–4610, https://doi.org/10.5194/acp-24-4591-2024, https://doi.org/10.5194/acp-24-4591-2024, 2024
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We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass burning plumes.
Markku Kulmala, Diego Aliaga, Santeri Tuovinen, Runlong Cai, Heikki Junninen, Chao Yan, Federico Bianchi, Yafang Cheng, Aijun Ding, Douglas R. Worsnop, Tuukka Petäjä, Katrianne Lehtipalo, Pauli Paasonen, and Veli-Matti Kerminen
Aerosol Research, 2, 49–58, https://doi.org/10.5194/ar-2-49-2024, https://doi.org/10.5194/ar-2-49-2024, 2024
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Atmospheric new particle formation (NPF), together with secondary production of particulate matter in the atmosphere, dominates aerosol particle number concentrations and submicron particle mass loads in many environments globally. In this opinion paper, we describe the paradigm shift to understand NPF in a continuous way instead of using traditional binary event–non-event analysis.
Satish Basnet, Anni Hartikainen, Aki Virkkula, Pasi Yli-Pirilä, Miika Kortelainen, Heikki Suhonen, Laura Kilpeläinen, Mika Ihalainen, Sampsa Väätäinen, Juho Louhisalmi, Markus Somero, Jarkko Tissari, Gert Jakobi, Ralf Zimmermann, Antti Kilpeläinen, and Olli Sippula
Atmos. Chem. Phys., 24, 3197–3215, https://doi.org/10.5194/acp-24-3197-2024, https://doi.org/10.5194/acp-24-3197-2024, 2024
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Brown carbon (BrC) emissions were estimated, for residential wood combustion (RWC) from various northern European appliances, utilizing an extensive seven-wavelength aethalometer dataset and thermal–optical carbon analysis. The contribution of BrC370–950 to the absorption of visible light varied between 1 % and 21 %, and was linked with fuel moisture content and combustion efficiency. This study provides important information required for assessing the climate effects of RWC emissions.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
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Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
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Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
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
Atmos. Chem. Phys., 24, 869–890, https://doi.org/10.5194/acp-24-869-2024, https://doi.org/10.5194/acp-24-869-2024, 2024
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Our results show that the global model is stable and it provides meaningful results. This way we can include a physics-based presentation of sub-grid physics (physics which happens on a 100 m scale) in the global model, whose resolution is on a 100 km scale.
Diego Aliaga, Santeri Tuovinen, Tinghan Zhang, Janne Lampilahti, Xinyang Li, Lauri Ahonen, Tom Kokkonen, Tuomo Nieminen, Simo Hakala, Pauli Paasonen, Federico Bianchi, Doug Worsnop, Veli-Matti Kerminen, and Markku Kulmala
Aerosol Research, 1, 81–92, https://doi.org/10.5194/ar-1-81-2023, https://doi.org/10.5194/ar-1-81-2023, 2023
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We introduce a novel method for evaluating days when small particles are formed in the atmosphere. Instead of the traditional binary division between event and non-event days, our method, known as "nano ranking analysis", provides a continuous, non-categorical metric for each day. By utilizing data from Hyytiälä, Finland, we show that our approach effectively quantifies these events. This innovative method paves the way for a deeper understanding of the factors influencing particle formation.
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
Atmos. Chem. Phys., 23, 14949–14971, https://doi.org/10.5194/acp-23-14949-2023, https://doi.org/10.5194/acp-23-14949-2023, 2023
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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 new particle formation and growth, feedback loops and the effect of COVID-19, and what has been learned from these investigations. The future needs and the potential of comprehensive observations of the environment are summarized.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Jonas Elm, Aladár Czitrovszky, Andreas Held, Annele Virtanen, Astrid Kiendler-Scharr, Benjamin J. Murray, Daniel McCluskey, Daniele Contini, David Broday, Eirini Goudeli, Hilkka Timonen, Joan Rosell-Llompart, Jose L. Castillo, Evangelia Diapouli, Mar Viana, Maria E. Messing, Markku Kulmala, Naděžda Zíková, and Sebastian H. Schmitt
Aerosol Research, 1, 13–16, https://doi.org/10.5194/ar-1-13-2023, https://doi.org/10.5194/ar-1-13-2023, 2023
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., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison 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.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
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Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
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Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
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.
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.
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.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
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.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
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.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
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.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
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.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
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.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
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.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
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.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
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.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
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.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
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.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
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.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
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.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
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.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
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.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 5945–5961, https://doi.org/10.5194/acp-20-5945-2020, https://doi.org/10.5194/acp-20-5945-2020, 2020
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By utilizing a new analysis approach, we investigated atmospheric oxidation of biogenic volatile emissions in a Finnish forest, measured by chemical ionization mass spectrometry. We identified several new compound groups, including low-volatility accretion products and their formation pathways. Results from this study are important for understanding atmospheric aerosol formation, as well as providing new perspectives on future lab studies and data analysis of short-lived species.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
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.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807, https://doi.org/10.5194/acp-20-3793-2020, https://doi.org/10.5194/acp-20-3793-2020, 2020
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We characterized secondary aerosol formation in Beijing. Our results showed that relative humidity (RH) and Ox have opposite effects on sulfate and nitrate formation in summer and winter. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC). Meanwhile, the dependence of less-oxidized OOA (LO-OOA) and the mass ratio of LO-OOA to MO-OOA in Ox both degraded when RH > 60 %, suggesting that RH or ALWC may also affect LO-OOA formation.
Liine Heikkinen, Mikko Äijälä, Matthieu Riva, Krista Luoma, Kaspar Dällenbach, Juho Aalto, Pasi Aalto, Diego Aliaga, Minna Aurela, Helmi Keskinen, Ulla Makkonen, Pekka Rantala, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 3151–3180, https://doi.org/10.5194/acp-20-3151-2020, https://doi.org/10.5194/acp-20-3151-2020, 2020
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Atmospheric aerosols are solid or liquid particles suspended in the air. They are known as a health risk, but they also influence the Earth's climate. The composition of aerosols becomes important when predicting their effect on climate. We show both seasonal and year-to-year variability of aerosol chemical composition in the boreal forest of Finland. We observed a consistent bimodal seasonal trend: a biogenic summertime maximum and an anthropogenic wintertime maximum in the mass concentration.
Lu Lei, Conghui Xie, Dawei Wang, Yao He, Qingqing Wang, Wei Zhou, Wei Hu, Pingqing Fu, Yong Chen, Xiaole Pan, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 20, 2877–2890, https://doi.org/10.5194/acp-20-2877-2020, https://doi.org/10.5194/acp-20-2877-2020, 2020
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We characterized aerosol composition and sources near two steel plants in a coastal region in fall and spring seasons. Our results showed substantially different aerosol composition and sources between the two seasons. We observed significant impacts of steel plant emissions on aerosol chemistry nearby, and we found that aerosol particles emitted from the steel plants were dominated by ammonium sulfate/bisulfate; NOx/CO and NOx/SO2 were distinct from those in the absence of industrial plumes.
Haiyan Li, Matthieu Riva, Pekka Rantala, Liine Heikkinen, Kaspar Daellenbach, Jordan E. Krechmer, Pierre-Marie Flaud, Douglas Worsnop, Markku Kulmala, Eric Villenave, Emilie Perraudin, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 20, 1941–1959, https://doi.org/10.5194/acp-20-1941-2020, https://doi.org/10.5194/acp-20-1941-2020, 2020
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We deployed the recently developed Vocus PTR-TOF in the French Landes forest during summertime to gain insights into terpene chemistry. In addition to isoprene, monoterpenes, sesquiterpenes, and the low-volatility diterpenes, various terpene reaction products are characterized. Through the analysis of terpene chemistry, we demonstrate the capability of the Vocus PTR-TOF for the detection of oxidized reaction products, highlighting its importance in investigating atmospheric oxidation processes.
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.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
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.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545, https://doi.org/10.5194/amt-12-5535-2019, https://doi.org/10.5194/amt-12-5535-2019, 2019
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We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
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.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
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.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920, https://doi.org/10.5194/amt-12-3907-2019, https://doi.org/10.5194/amt-12-3907-2019, 2019
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An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 3761–3776, https://doi.org/10.5194/amt-12-3761-2019, https://doi.org/10.5194/amt-12-3761-2019, 2019
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Recent advancements in atmospheric mass spectrometry provide large amounts of new information but at the same time present considerable challenges for the data analysis, for example, in high-resolution peak identification and separation. To address these problems, this study presents a simple and novel method, which succeeds in analyzing both synthetic and ambient datasets. We believe it will become a powerful approach in the data analysis of mass spectra.
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.
Matthieu Riva, Pekka Rantala, Jordan E. Krechmer, Otso Peräkylä, Yanjun Zhang, Liine Heikkinen, Olga Garmash, Chao Yan, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 2403–2421, https://doi.org/10.5194/amt-12-2403-2019, https://doi.org/10.5194/amt-12-2403-2019, 2019
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The impact of aerosol particles on climate and air quality remains poorly understood due to multiple factors. One of the current limitations is the incomplete understanding of the contribution of oxygenated species, formed from the oxidation of volatile organic compounds (VOCs) to aerosol formation. Taking advantage of recent mass spectrometric developments, we have evaluated and compared the capability of multiple state-of-the-art mass spectrometers to detect a wide variety of oxygenated VOCs.
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.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
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.
Qiaozhi Zha, Chao Yan, Heikki Junninen, Matthieu Riva, Nina Sarnela, Juho Aalto, Lauriane Quéléver, Simon Schallhart, Lubna Dada, Liine Heikkinen, Otso Peräkylä, Jun Zou, Clémence Rose, Yonghong Wang, Ivan Mammarella, Gabriel Katul, Timo Vesala, Douglas R. Worsnop, Markku Kulmala, Tuukka Petäjä, Federico Bianchi, and Mikael Ehn
Atmos. Chem. Phys., 18, 17437–17450, https://doi.org/10.5194/acp-18-17437-2018, https://doi.org/10.5194/acp-18-17437-2018, 2018
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Vertical measurements of highly oxygenated molecules (HOMs) below and above the forest canopy were performed for the first time in a boreal forest during September 2016. Our results highlight that near-ground HOM measurements may only be representative of a small fraction of the entire nocturnal boundary layer, which may sequentially influence the growth of newly formed particles and SOA formation close to ground surface, where the majority of measurements are conducted.
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.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
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.
Yue Zhang, Shachi Katira, Andrew Lee, Andrew T. Lambe, Timothy B. Onasch, Wen Xu, William A. Brooks, Manjula R. Canagaratna, Andrew Freedman, John T. Jayne, Doug R. Worsnop, Paul Davidovits, David Chandler, and Charles E. Kolb
Atmos. Meas. Tech., 11, 3479–3490, https://doi.org/10.5194/amt-11-3479-2018, https://doi.org/10.5194/amt-11-3479-2018, 2018
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We have adopted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols at submicron sizes and relatively low mass concentrations. Aerosol particles are deposited in the form of a thin film with interdigitated electrodes using electrostatic precipitation. Broadband dielectric spectroscopy is used to measure the kinetically controlled glass transition temperatures of glycerol and citric acid aerosols with three atmospheric relevant cooling rates.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
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.
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
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
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
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.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
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
Eben S. Cross, Leah R. Williams, David K. Lewis, Gregory R. Magoon, Timothy B. Onasch, Michael L. Kaminsky, Douglas R. Worsnop, and John T. Jayne
Atmos. Meas. Tech., 10, 3575–3588, https://doi.org/10.5194/amt-10-3575-2017, https://doi.org/10.5194/amt-10-3575-2017, 2017
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Low-cost air quality sensor technologies offer new opportunities for fast and distributed measurements of air pollution, but a persistent characterization gap remains when it comes to evaluating sensor performance under realistic environmental sampling conditions. We present results from a newly developed integrated AQ-sensor system (ARISense) and demonstrate the utility of using high-dimensional model representation to improve the conversion of raw sensor signal to ambient concentration.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
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.
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
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.
Hilkka Timonen, Panu Karjalainen, Erkka Saukko, Sanna Saarikoski, Päivi Aakko-Saksa, Pauli Simonen, Timo Murtonen, Miikka Dal Maso, Heino Kuuluvainen, Matthew Bloss, Erik Ahlberg, Birgitta Svenningsson, Joakim Pagels, William H. Brune, Jorma Keskinen, Douglas R. Worsnop, Risto Hillamo, and Topi Rönkkö
Atmos. Chem. Phys., 17, 5311–5329, https://doi.org/10.5194/acp-17-5311-2017, https://doi.org/10.5194/acp-17-5311-2017, 2017
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The effect of fuel ethanol content (10–100 %) on primary emissions and the subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. The emissions were characterized during the New European Driving Cycle (NEDC) using high time-resolution instruments. The chemical composition of the exhaust particulate matter was studied using a soot particle aerosol mass spectrometer (SP-AMS), and the secondary aerosol formation was studied with an oxidation chamber.
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.
Ellis Shipley Robinson, Timothy B. Onasch, Douglas Worsnop, and Neil M. Donahue
Atmos. Meas. Tech., 10, 1139–1154, https://doi.org/10.5194/amt-10-1139-2017, https://doi.org/10.5194/amt-10-1139-2017, 2017
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.
Mikko Äijälä, Liine Heikkinen, Roman Fröhlich, Francesco Canonaco, André S. H. Prévôt, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 17, 3165–3197, https://doi.org/10.5194/acp-17-3165-2017, https://doi.org/10.5194/acp-17-3165-2017, 2017
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Mass spectrometric measurements commonly yield data on hundreds of variables over thousands of points in time. Refining and synthesising this “raw” data into chemical information necessitates the use of advanced, statistics-based data analysis techniques. Here we present an example of combining data dimensionality reduction (factorisation) with exploratory classification (clustering) and show that the results complement and broaden our current perspectives on aerosol chemical classification.
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.