Articles | Volume 19, issue 24
Atmos. Chem. Phys., 19, 15545–15567, 2019
https://doi.org/10.5194/acp-19-15545-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 19, 15545–15567, 2019
https://doi.org/10.5194/acp-19-15545-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
19 Dec 2019
Research article
| 19 Dec 2019
Impact of isolated atmospheric aging processes on the cloud condensation nuclei activation of soot particles
Franz Friebel et al.
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Kunfeng Gao, Franz Friebel, Chong-Wen Zhou, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 4985–5016, https://doi.org/10.5194/acp-22-4985-2022, https://doi.org/10.5194/acp-22-4985-2022, 2022
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Soot particles impact cloud formation and radiative properties in the upper atmosphere where aircraft emit carbonaceous particles. We use cloud chambers to mimic the upper atmosphere temperature and humidity to test the influence of the morphology of the soot particles on ice cloud formation. For particles larger than 200 nm, the compacted (densified) samples have a higher affinity for ice crystal formation in the cirrus regime than the fluffy (un-compacted) soot particles of the same sample.
Franz Friebel and Amewu A. Mensah
Atmos. Meas. Tech., 12, 2647–2663, https://doi.org/10.5194/amt-12-2647-2019, https://doi.org/10.5194/amt-12-2647-2019, 2019
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Simulating atmospheric aging processes in the laboratory under atmospheric conditions is a challenging task. The main obstacle is achieving long observation times with a reasonable amount of technical and financial input. We adapted the concept of the continuous-flow stirred tank reactor in order to achieve long observation times (up to 16 h) in small chamber volumes (3m3). We successfully tested this concept by oxidation of soot particles with ozone.
Julie Thérèse Pasquier, Jan Henneberger, Fabiola Ramelli, Annika Lauber, Robert Oscar David, Jörg Wieder, Tim Carlsen, Rosa Gierens, Marion Maturilli, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 15579–15601, https://doi.org/10.5194/acp-22-15579-2022, https://doi.org/10.5194/acp-22-15579-2022, 2022
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It is important to understand how ice crystals and cloud droplets form in clouds, as their concentrations and sizes determine the exact radiative properties of the clouds. Normally, ice crystals form from aerosols, but we found evidence for the formation of additional ice crystals from the original ones over a large temperature range within Arctic clouds. In particular, additional ice crystals were formed during collisions of several ice crystals or during the freezing of large cloud droplets.
Bernhard Markus Enz, Jan Paul Engelmann, and Ulrike Lohmann
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-279, https://doi.org/10.5194/gmd-2022-279, 2022
Preprint under review for GMD
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An algorithm to track tropical cyclones in model simulation data has been developed. The algorithm uses many combinations of varying parameter thresholds to detect weaker phases of tropical cyclones while still being resilient to false positives. It is shown that the algorithm performs well, and adequately represents the tropical cyclone activity of the underlying simulation data. The impact of false positives on overall tropical cyclone activity is shown to be insignificant.
Colin Tully, David Neubauer, Diego Villanueva, and Ulrike Lohmann
EGUsphere, https://doi.org/10.5194/egusphere-2022-1238, https://doi.org/10.5194/egusphere-2022-1238, 2022
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This study details the first attempt with a GCM to simulate a fully prognostic aerosol species specifically for cirrus climate intervention. The new approach is in line with the real-world delivery mechanism via aircraft. However, to achieve an appreciable signal from seeding, smaller particles were needed, and their mass emissions needed to be scaled by at least a factor of 100. These biases contributed to either overseeding, or small and insignificant effects in response to seeding cirrus.
Colin Tully, David Neubauer, and Ulrike Lohmann
EGUsphere, https://doi.org/10.5194/egusphere-2022-1057, https://doi.org/10.5194/egusphere-2022-1057, 2022
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A new method to simulate deterministic ice nucleation processes based on the differential activated fraction was evaluated against a cumulative approach. Box model simulations of heterogeneous-only ice nucleation within cirrus suggest that the latter approach likely underpredicts the ice crystal number concentration. Longer simulations with a GCM show that choosing between these two approaches impacts ice nucleation competition within cirrus but leads to small and insignificant climate effects.
Florin N. Isenrich, Nadia Shardt, Michael Rösch, Julia Nette, Stavros Stavrakis, Claudia Marcolli, Zamin A. Kanji, Andrew J. deMello, and Ulrike Lohmann
Atmos. Meas. Tech., 15, 5367–5381, https://doi.org/10.5194/amt-15-5367-2022, https://doi.org/10.5194/amt-15-5367-2022, 2022
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Ice nucleation in the atmosphere influences cloud properties and lifetimes. Microfluidic instruments have recently been used to investigate ice nucleation, but these instruments are typically made out of a polymer that contributes to droplet instability over extended timescales and relatively high temperature uncertainty. To address these drawbacks, we develop and validate a new microfluidic instrument that uses fluoropolymer tubing to extend droplet stability and improve temperature accuracy.
Colin Tully, David Neubauer, Nadja Omanovic, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 11455–11484, https://doi.org/10.5194/acp-22-11455-2022, https://doi.org/10.5194/acp-22-11455-2022, 2022
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The proposed geoengineering method, cirrus cloud thinning, was evaluated using a more physically based microphysics scheme coupled to a more realistic approach for calculating ice cloud fractions in the ECHAM-HAM GCM. Sensitivity tests reveal that using the new ice cloud fraction approach and increasing the critical ice saturation ratio for ice nucleation on seeding particles reduces warming from overseeding. However, this geoengineering method is unlikely to be feasible on a global scale.
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.
Jörg Wieder, Nikola Ihn, Claudia Mignani, Moritz Haarig, Johannes Bühl, Patric Seifert, Ronny Engelmann, Fabiola Ramelli, Zamin A. Kanji, Ulrike Lohmann, and Jan Henneberger
Atmos. Chem. Phys., 22, 9767–9797, https://doi.org/10.5194/acp-22-9767-2022, https://doi.org/10.5194/acp-22-9767-2022, 2022
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Ice formation and its evolution in mixed-phase clouds are still uncertain. We evaluate the lidar retrieval of ice-nucleating particle concentration in dust-dominated and continental air masses over the Swiss Alps with in situ observations. A calibration factor to improve the retrieval from continental air masses is proposed. Ice multiplication factors are obtained with a new method utilizing remote sensing. Our results indicate that secondary ice production occurs at temperatures down to −30 °C.
Zane Dedekind, Jacopo Grazioli, Philip H. Austin, and Ulrike Lohmann
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-429, https://doi.org/10.5194/acp-2022-429, 2022
Revised manuscript under review for ACP
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Simulations allowing ice particles to collide with one another producing more ice particles represented surface observations of ice particles accurately. An increase in ice particles formed through collisions was related to sharp changes in the wind direction and speed with height. Changes in wind speed and direction can therefore cause more enhanced collisions between ice particles and alter how fast and how much precipitation forms. Simulations were conducted with an atmospheric model COSMO.
Joel C. Corbin, Tobias Schripp, Bruce E. Anderson, Greg J. Smallwood, Patrick LeClercq, Ewan C. Crosbie, Steven Achterberg, Philip D. Whitefield, Richard C. Miake-Lye, Zhenhong Yu, Andrew Freedman, Max Trueblood, David Satterfield, Wenyan Liu, Patrick Oßwald, Claire Robinson, Michael A. Shook, Richard H. Moore, and Prem Lobo
Atmos. Meas. Tech., 15, 3223–3242, https://doi.org/10.5194/amt-15-3223-2022, https://doi.org/10.5194/amt-15-3223-2022, 2022
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The combustion of sustainable aviation fuels in aircraft engines produces particulate matter (PM) emissions with different properties than conventional fuels due to changes in fuel composition. Consequently, the response of various diagnostic instruments to PM emissions may be impacted. We found no significant instrument biases in terms of particle mass, number, and size measurements for conventional and sustainable aviation fuel blends despite large differences in the magnitude of emissions.
Kunfeng Gao, Franz Friebel, Chong-Wen Zhou, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 4985–5016, https://doi.org/10.5194/acp-22-4985-2022, https://doi.org/10.5194/acp-22-4985-2022, 2022
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Soot particles impact cloud formation and radiative properties in the upper atmosphere where aircraft emit carbonaceous particles. We use cloud chambers to mimic the upper atmosphere temperature and humidity to test the influence of the morphology of the soot particles on ice cloud formation. For particles larger than 200 nm, the compacted (densified) samples have a higher affinity for ice crystal formation in the cirrus regime than the fluffy (un-compacted) soot particles of the same sample.
Ulrike Proske, Sylvaine Ferrachat, David Neubauer, Martin Staab, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 4737–4762, https://doi.org/10.5194/acp-22-4737-2022, https://doi.org/10.5194/acp-22-4737-2022, 2022
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Cloud microphysical processes shape cloud properties and are therefore important to represent in climate models. Their parameterization has grown more complex, making the model results more difficult to interpret. Using sensitivity analysis we test how the global aerosol–climate model ECHAM-HAM reacts to changes to these parameterizations. The model is sensitive to the parameterization of ice crystal autoconversion but not to, e.g., self-collection, suggesting that it may be simplified.
Jörg Wieder, Claudia Mignani, Mario Schär, Lucie Roth, Michael Sprenger, Jan Henneberger, Ulrike Lohmann, Cyril Brunner, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 3111–3130, https://doi.org/10.5194/acp-22-3111-2022, https://doi.org/10.5194/acp-22-3111-2022, 2022
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We investigate the variation in ice-nucleating particles (INPs) relevant for primary ice formation in mixed-phased clouds over the Alps based on simultaneous in situ observations at a mountaintop and a nearby high valley (1060 m height difference). In most cases, advection from the surrounding lower regions was responsible for changes in INP concentration, causing a diurnal cycle at the mountaintop. Our study underlines the importance of the planetary boundary layer as an INP reserve.
Ruoyang Yuan, Prem Lobo, Greg J. Smallwood, Mark P. Johnson, Matthew C. Parker, Daniel Butcher, and Adrian Spencer
Atmos. Meas. Tech., 15, 241–259, https://doi.org/10.5194/amt-15-241-2022, https://doi.org/10.5194/amt-15-241-2022, 2022
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The relationship between the non-volatile particulate matter (nvPM) mass emissions produced by different engine sources and the response of the LII 300 instrument, used for regulatory measurements of nvPM mass emissions in aircraft engine certification tests, was investigated for different sources and operating conditions. Laser fluence optimisation was required for real-time nvPM mass concentration measurements. These results will inform the development of updated calibration protocols.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182, https://doi.org/10.5194/acp-21-16161-2021, https://doi.org/10.5194/acp-21-16161-2021, 2021
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Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
Zane Dedekind, Annika Lauber, Sylvaine Ferrachat, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 15115–15134, https://doi.org/10.5194/acp-21-15115-2021, https://doi.org/10.5194/acp-21-15115-2021, 2021
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The RACLETS campaign combined cloud and snow research to improve the understanding of precipitation formation in clouds. A numerical weather prediction model, COSMO, was used to assess the importance of ice crystal enhancement by ice–ice collisions for cloud properties. We found that the number of ice crystals increased by 1 to 3 orders of magnitude when ice–ice collisions were permitted to occur, reducing localized regions of high precipitation and, thereby, improving the model performance.
Paolo Pelucchi, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 14, 5413–5434, https://doi.org/10.5194/gmd-14-5413-2021, https://doi.org/10.5194/gmd-14-5413-2021, 2021
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Stratocumulus are thin clouds whose cloud cover is underestimated in climate models partly due to overly low vertical resolution. We develop a scheme that locally refines the vertical grid based on a physical constraint for the cloud top. Global simulations show that the scheme, implemented only in the radiation routine, can increase stratocumulus cloud cover. However, this effect is poorly propagated to the simulated cloud cover. The scheme's limitations and possible ways forward are discussed.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Fabiola Ramelli, Jan Henneberger, Robert O. David, Johannes Bühl, Martin Radenz, Patric Seifert, Jörg Wieder, Annika Lauber, Julie T. Pasquier, Ronny Engelmann, Claudia Mignani, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 6681–6706, https://doi.org/10.5194/acp-21-6681-2021, https://doi.org/10.5194/acp-21-6681-2021, 2021
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Orographic mixed-phase clouds are an important source of precipitation, but the ice formation processes within them remain uncertain. Here we investigate the origin of ice crystals in a mixed-phase cloud in the Swiss Alps using aerosol and cloud data from in situ and remote sensing observations. We found that ice formation primarily occurs in cloud top generating cells. Our results indicate that secondary ice processes are active in the feeder region, which can enhance orographic precipitation.
Fabiola Ramelli, Jan Henneberger, Robert O. David, Annika Lauber, Julie T. Pasquier, Jörg Wieder, Johannes Bühl, Patric Seifert, Ronny Engelmann, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 5151–5172, https://doi.org/10.5194/acp-21-5151-2021, https://doi.org/10.5194/acp-21-5151-2021, 2021
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Interactions between dynamics, microphysics and orography can enhance precipitation. Yet the exact role of these interactions is still uncertain. Here we investigate the role of low-level blocking and turbulence for precipitation by combining remote sensing and in situ observations. The observations show that blocked flow can induce the formation of feeder clouds and that turbulence can enhance hydrometeor growth, demonstrating the importance of local flow effects for orographic precipitation.
Ulrike Proske, Verena Bessenbacher, Zane Dedekind, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 21, 5195–5216, https://doi.org/10.5194/acp-21-5195-2021, https://doi.org/10.5194/acp-21-5195-2021, 2021
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Ice crystals falling out of one cloud can initiate freezing in a second cloud below. We estimate the occurrence frequency of this natural cloud seeding over Switzerland from satellite data and sublimation calculations. We find that such situations with an ice cloud above another cloud are frequent and that the falling crystals survive the fall between two clouds in a significant number of cases, suggesting that natural cloud seeding is an important phenomenon over Switzerland.
Annika Lauber, Jan Henneberger, Claudia Mignani, Fabiola Ramelli, Julie T. Pasquier, Jörg Wieder, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 3855–3870, https://doi.org/10.5194/acp-21-3855-2021, https://doi.org/10.5194/acp-21-3855-2021, 2021
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An accurate prediction of the ice crystal number concentration (ICNC) is important to determine the radiation budget, lifetime, and precipitation formation of clouds. Even though secondary-ice processes can increase the ICNC by several orders of magnitude, they are poorly constrained and lack a well-founded quantification. During measurements on a mountain slope, a high ICNC of small ice crystals was observed just below 0 °C, attributed to a secondary-ice process and parametrized in this study.
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.
Steven T. Turnock, Robert J. Allen, Martin Andrews, Susanne E. Bauer, Makoto Deushi, Louisa Emmons, Peter Good, Larry Horowitz, Jasmin G. John, Martine Michou, Pierre Nabat, Vaishali Naik, David Neubauer, Fiona M. O'Connor, Dirk Olivié, Naga Oshima, Michael Schulz, Alistair Sellar, Sungbo Shim, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 20, 14547–14579, https://doi.org/10.5194/acp-20-14547-2020, https://doi.org/10.5194/acp-20-14547-2020, 2020
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A first assessment is made of the historical and future changes in air pollutants from models participating in the 6th Coupled Model Intercomparison Project (CMIP6). Substantial benefits to future air quality can be achieved in future scenarios that implement measures to mitigate climate and involve reductions in air pollutant emissions, particularly methane. However, important differences are shown between models in the future regional projection of air pollutants under the same scenario.
Augustin Mortier, Jonas Gliß, Michael Schulz, Wenche Aas, Elisabeth Andrews, Huisheng Bian, Mian Chin, Paul Ginoux, Jenny Hand, Brent Holben, Hua Zhang, Zak Kipling, Alf Kirkevåg, Paolo Laj, Thibault Lurton, Gunnar Myhre, David Neubauer, Dirk Olivié, Knut von Salzen, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 20, 13355–13378, https://doi.org/10.5194/acp-20-13355-2020, https://doi.org/10.5194/acp-20-13355-2020, 2020
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We present a multiparameter analysis of the aerosol trends over the last 2 decades in the different regions of the world. In most of the regions, ground-based observations show a decrease in aerosol content in both the total atmospheric column and at the surface. The use of climate models, assessed against these observations, reveals however an increase in the total aerosol load, which is not seen with the sole use of observation due to partial coverage in space and time.
Robert J. Allen, Steven Turnock, Pierre Nabat, David Neubauer, Ulrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, Jie Zhang, Toshihiko Takemura, Michael Schulz, Kostas Tsigaridis, Susanne E. Bauer, Louisa Emmons, Larry Horowitz, Vaishali Naik, Twan van Noije, Tommi Bergman, Jean-Francois Lamarque, Prodromos Zanis, Ina Tegen, Daniel M. Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona O'Connor, Dimitris Akritidis, Aristeidis K. Georgoulias, Makoto Deushi, Lori T. Sentman, Jasmin G. John, Shinichiro Fujimori, and William J. Collins
Atmos. Chem. Phys., 20, 9641–9663, https://doi.org/10.5194/acp-20-9641-2020, https://doi.org/10.5194/acp-20-9641-2020, 2020
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.
Mattia Righi, Johannes Hendricks, Ulrike Lohmann, Christof Gerhard Beer, Valerian Hahn, Bernd Heinold, Romy Heller, Martina Krämer, Michael Ponater, Christian Rolf, Ina Tegen, and Christiane Voigt
Geosci. Model Dev., 13, 1635–1661, https://doi.org/10.5194/gmd-13-1635-2020, https://doi.org/10.5194/gmd-13-1635-2020, 2020
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A new cloud microphysical scheme is implemented in the global EMAC-MADE3 aerosol model and evaluated. The new scheme features a detailed parameterization for aerosol-driven ice formation in cirrus clouds, accounting for the competition between homogeneous and heterogeneous ice formation processes. The comparison against satellite data and in situ measurements shows that the model performance is in line with similar global coupled models featuring ice cloud parameterizations.
Fabiola Ramelli, Alexander Beck, Jan Henneberger, and Ulrike Lohmann
Atmos. Meas. Tech., 13, 925–939, https://doi.org/10.5194/amt-13-925-2020, https://doi.org/10.5194/amt-13-925-2020, 2020
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Boundary layer clouds are influenced by many physical and dynamical processes, making accurate forecasting difficult. Here we present a new measurement platform on a tethered balloon to measure cloud microphysical and meteorological profiles. The unique combination of holography and balloon-borne observations allows high-resolution measurements in a well-defined volume. Field measurements in stratus clouds over the Swiss Plateau revealed unique microphysical signatures in the cloud structure.
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.
Edward Gryspeerdt, Johannes Mülmenstädt, Andrew Gettelman, Florent F. Malavelle, Hugh Morrison, David Neubauer, Daniel G. Partridge, Philip Stier, Toshihiko Takemura, Hailong Wang, Minghuai Wang, and Kai Zhang
Atmos. Chem. Phys., 20, 613–623, https://doi.org/10.5194/acp-20-613-2020, https://doi.org/10.5194/acp-20-613-2020, 2020
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Aerosol radiative forcing is a key uncertainty in our understanding of the human forcing of the climate, with much of this uncertainty coming from aerosol impacts on clouds. Observation-based estimates of the radiative forcing are typically smaller than those from global models, but it is not clear if they are more reliable. This work shows how the forcing components in global climate models can be identified, highlighting similarities between the two methods and areas for future investigation.
Anina Gilgen, Stiig Wilkenskjeld, Jed O. Kaplan, Thomas Kühn, and Ulrike Lohmann
Clim. Past, 15, 1885–1911, https://doi.org/10.5194/cp-15-1885-2019, https://doi.org/10.5194/cp-15-1885-2019, 2019
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Using the global aerosol–climate model ECHAM-HAM-SALSA, the effect of humans on European climate in the Roman Empire was quantified. Both land use and novel estimates of anthropogenic aerosol emissions were considered. We conducted simulations with fixed sea-surface temperatures to gain a first impression about the anthropogenic impact. While land use effects induced a regional warming for one of the reconstructions, aerosol emissions led to a cooling associated with aerosol–cloud interactions.
André Welti, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 10901–10918, https://doi.org/10.5194/acp-19-10901-2019, https://doi.org/10.5194/acp-19-10901-2019, 2019
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The ice nucleation ability of singly immersed feldspar particles in suspended water droplets relevant for ice crystal formation under mixed-phase cloud conditions is presented. The effects of particle size, crystal structure, trace metal and mineralogical composition are discussed by testing up to five different diameters in the submicron range and nine different feldspar samples at conditions relevant for ice nucleation in mixed-phase clouds.
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.
Gesa K. Eirund, Anna Possner, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 9847–9864, https://doi.org/10.5194/acp-19-9847-2019, https://doi.org/10.5194/acp-19-9847-2019, 2019
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Low-level mixed-phase cloud (MPC) properties can be highly affected by the ambient aerosol concentration, especially in pristine environments like the Arctic. By employing high-resolution model simulations we investigate the response of a MPC over an open ocean and a sea ice surface to aerosol perturbations. While we find a strong initial sensitivity to changes in aerosol concentration in both cloud regimes, the magnitude as well as the long-term cloud response depends on the surface condition.
Remo Dietlicher, David Neubauer, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 9061–9080, https://doi.org/10.5194/acp-19-9061-2019, https://doi.org/10.5194/acp-19-9061-2019, 2019
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Ice crystals in clouds cover a spectrum of shapes and sizes. We show the first results of a consistent representation of the cloud ice spectrum in the climate model ECHAM6-HAM2. The simulated cloud fields are linked to their sources by new diagnostics. We find that only a small fraction of ice clouds is initiated by freezing of cloud droplets in the mixed-phase temperature regime while most ice forms at temperatures colder than −35 °C.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Stephanie Fiedler, Stefan Kinne, Wan Ting Katty Huang, Petri Räisänen, Declan O'Donnell, Nicolas Bellouin, Philip Stier, Joonas Merikanto, Twan van Noije, Risto Makkonen, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 6821–6841, https://doi.org/10.5194/acp-19-6821-2019, https://doi.org/10.5194/acp-19-6821-2019, 2019
Franz Friebel and Amewu A. Mensah
Atmos. Meas. Tech., 12, 2647–2663, https://doi.org/10.5194/amt-12-2647-2019, https://doi.org/10.5194/amt-12-2647-2019, 2019
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Simulating atmospheric aging processes in the laboratory under atmospheric conditions is a challenging task. The main obstacle is achieving long observation times with a reasonable amount of technical and financial input. We adapted the concept of the continuous-flow stirred tank reactor in order to achieve long observation times (up to 16 h) in small chamber volumes (3m3). We successfully tested this concept by oxidation of soot particles with ozone.
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.
Yvonne Boose, Philipp Baloh, Michael Plötze, Johannes Ofner, Hinrich Grothe, Berko Sierau, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 1059–1076, https://doi.org/10.5194/acp-19-1059-2019, https://doi.org/10.5194/acp-19-1059-2019, 2019
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The role non-mineral components play in the freezing behavior of atmospheric desert dust is not well known. In this study, we use chemical imaging methods to investigate this for airborne and surface-collected desert dust samples. We find that in most cases the ice nucleation behavior is determined by the dust mineralogical composition. However, volatile organic material can coat active sites and decrease the dust ice nucleation ability, while biological particles can significantly increase it.
Max B. Trueblood, Prem Lobo, Donald E. Hagen, Steven C. Achterberg, Wenyan Liu, and Philip D. Whitefield
Atmos. Chem. Phys., 18, 17029–17045, https://doi.org/10.5194/acp-18-17029-2018, https://doi.org/10.5194/acp-18-17029-2018, 2018
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We report detailed lab-based performance evaluation of a robust hygroscopic tandem differential mobility analyzer (HTDMA), in terms of hygroscopic properties such as growth factor (GF) and the hygroscopicity parameter (κ). The HTDMA was deployed during a field campaign to measure the hygroscopic properties of aircraft engine PM emissions in the exhaust plumes from a CFM56-2C1 engine burning regular jet fuel, alternative fuels, and blends.
Emma Järvinen, Olivier Jourdan, David Neubauer, Bin Yao, Chao Liu, Meinrat O. Andreae, Ulrike Lohmann, Manfred Wendisch, Greg M. McFarquhar, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 18, 15767–15781, https://doi.org/10.5194/acp-18-15767-2018, https://doi.org/10.5194/acp-18-15767-2018, 2018
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Using light diffraction it is possible to detect microscopic features within ice particles that have not yet been fully characterized. Here, this technique was applied in airborne measurements, where it was found that majority of atmospheric ice particles have features that significantly change the way ice particles interact with solar light. The microscopic features make ice-containing clouds more reflective than previously thought, which could have consequences for predicting our climate.
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.
Fabian Mahrt, Claudia Marcolli, Robert O. David, Philippe Grönquist, Eszter J. Barthazy Meier, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 13363–13392, https://doi.org/10.5194/acp-18-13363-2018, https://doi.org/10.5194/acp-18-13363-2018, 2018
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The ice nucleation ability of different soot particles in the cirrus and mixed-phase cloud temperature regime is presented. The impact of aerosol particle size, particle morphology, organic matter and hydrophilicity on ice nucleation is examined. We propose ice nucleation proceeds via a pore condensation freezing mechanism for soot particles with the necessary physicochemical properties that nucleated ice well below water saturation.
Anina Gilgen, Carole Adolf, Sandra O. Brugger, Luisa Ickes, Margit Schwikowski, Jacqueline F. N. van Leeuwen, Willy Tinner, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 11813–11829, https://doi.org/10.5194/acp-18-11813-2018, https://doi.org/10.5194/acp-18-11813-2018, 2018
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Microscopic charcoal particles are fire-specific tracers, which are presently the primary source for reconstructing past fire activity. In this study, we implement microscopic charcoal particles into a global aerosol–climate model to better understand the transport of charcoal on a large scale. We find that the model captures a significant portion of the spatial variability but fails to reproduce the extreme variability observed in the charcoal data.
Wan Ting Katty Huang, Luisa Ickes, Ina Tegen, Matteo Rinaldi, Darius Ceburnis, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 11423–11445, https://doi.org/10.5194/acp-18-11423-2018, https://doi.org/10.5194/acp-18-11423-2018, 2018
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In this study, we investigated the potential impact on clouds and climate by organic particles emitted from the ocean surface, using a global climate model. These particles have previously been found to promote ice crystal formation, which may alter the properties of clouds. Our study, however, found a weak global impact by these particles, which brings into question their relative importance and points to the need for further verification with other models and at more regional scales.
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.
Anina Gilgen, Wan Ting Katty Huang, Luisa Ickes, David Neubauer, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 10521–10555, https://doi.org/10.5194/acp-18-10521-2018, https://doi.org/10.5194/acp-18-10521-2018, 2018
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Aerosol emissions in Arctic summer and autumn are expected to increase in the future because of sea ice retreat. Using a global aerosol–climate model, we quantify the impact of increased aerosol emissions from the ocean and from Arctic shipping in the year 2050. The influence on radiation of both aerosols and clouds is analysed. Mainly driven by changes in surface albedo, the cooling effect of marine aerosols and clouds will increase. Future ship emissions might have a small net cooling effect.
Alexander Beck, Jan Henneberger, Jacob P. Fugal, Robert O. David, Larissa Lacher, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 8909–8927, https://doi.org/10.5194/acp-18-8909-2018, https://doi.org/10.5194/acp-18-8909-2018, 2018
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This study assesses the impact of surface processes (e.g. blowing snow) on in situ cloud observations at Sonnblick Observatory. Vertical profiles of ice crystal number concentrations (ICNCs) above a snow-covered surface were observed up to a height of 10 m. The ICNC near the ground is at least a factor of 2 larger than at 10 m. Therefore, in situ measurements of ICNCs at mountain-top research stations close to the surface are strongly influenced by surface processes and overestimate the ICNC.
Ulrike Lohmann and David Neubauer
Atmos. Chem. Phys., 18, 8807–8828, https://doi.org/10.5194/acp-18-8807-2018, https://doi.org/10.5194/acp-18-8807-2018, 2018
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The climate is warming, at the current rate so much so that the 2 ºC target is likely to be exceeded. Uncertainty remains as to when the 2 ºC of warming will be reached. One factor contributing to this uncertainty is how clouds change in the warmer climate. While previously most emphasis was placed on how low clouds change in the warmer climate, here we investigate the importance of mixed-phase and ice clouds.
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.
Remo Dietlicher, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 11, 1557–1576, https://doi.org/10.5194/gmd-11-1557-2018, https://doi.org/10.5194/gmd-11-1557-2018, 2018
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A new cloud scheme was implemented in the aerosol–climate model ECHAM6-HAM2. Unlike traditional schemes, it does not categorize ice particles by in-cloud and precipitation types but uses a single category with prognostic bulk particle properties. The new scheme is not only conceptually simpler but also closer to first principles as it does not rely on weakly constrained conversion rates between predefined categories and resolves falling ice by local sub-time-stepping.
Larissa Lacher, Ulrike Lohmann, Yvonne Boose, Assaf Zipori, Erik Herrmann, Nicolas Bukowiecki, Martin Steinbacher, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 15199–15224, https://doi.org/10.5194/acp-17-15199-2017, https://doi.org/10.5194/acp-17-15199-2017, 2017
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We characterize the new Horizontal Ice Nucleation Chamber HINC to measure ambient ice nucleating particle concentrations at mixed‐phase cloud conditions. Results from winter measurements at the High Altitude Research Station Jungfraujoch compare well to previous measurements. We find increased ice nucleating particle concentrations during the influence of Saharan dust events and marine events, which highlights the importance of these species on ice nucleation in the free troposphere.
David Neubauer, Matthew W. Christensen, Caroline A. Poulsen, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 13165–13185, https://doi.org/10.5194/acp-17-13165-2017, https://doi.org/10.5194/acp-17-13165-2017, 2017
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When aerosol particles take up water their number may seem to be increased optically. However if aerosol particles are removed by precipitation (formation) their numbers will decrease. We applied methods to account for such effects in model and satellite data to analyse the change in cloud properties by changes in aerosol particle number. The agreement of model and satellite data improves when these effects are accounted for.
Matthew W. Christensen, David Neubauer, Caroline A. Poulsen, Gareth E. Thomas, Gregory R. McGarragh, Adam C. Povey, Simon R. Proud, and Roy G. Grainger
Atmos. Chem. Phys., 17, 13151–13164, https://doi.org/10.5194/acp-17-13151-2017, https://doi.org/10.5194/acp-17-13151-2017, 2017
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The cloud-aerosol pairing algorithm (CAPA) is developed to quantify the impact of near-cloud aerosol retrievals on satellite-based aerosol–cloud statistical relationships. We find that previous satellite-based radiative forcing estimates of aerosol–cloud interactions represented in key climate reports are likely exaggerated by up to 50 % due to including retrieval artefacts in the aerosols located near clouds. It is demonstrated that this retrieval artefact can be corrected in current products.
Hendrik Andersen, Jan Cermak, Julia Fuchs, Reto Knutti, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 9535–9546, https://doi.org/10.5194/acp-17-9535-2017, https://doi.org/10.5194/acp-17-9535-2017, 2017
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Aerosol-cloud interactions continue to contribute large uncertainties to our climate system understanding. In this study, we use near-global satellite and reanalysis data sets to predict marine liquid-water clouds by means of artificial neural networks. We show that on the system scale, lower-tropospheric stability and boundary layer height are the main determinants of liquid-water clouds. Aerosols show the expected impact on clouds but are less relevant than some meteorological factors.
Franziska Glassmeier, Anna Possner, Bernhard Vogel, Heike Vogel, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 8651–8680, https://doi.org/10.5194/acp-17-8651-2017, https://doi.org/10.5194/acp-17-8651-2017, 2017
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We compare two chemistry and aerosol schemes – one designed for air-quality, the other for climate applications. For distribution, composition and radiative properties, the choice of aerosol types and processes turns out to be more important than their implementation. For aerosol–cloud interactions, we find cloud processes, in particular ice formation, to be the main obstacle to our understanding.
Anahita Amiri-Farahani, Robert J. Allen, David Neubauer, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 6305–6322, https://doi.org/10.5194/acp-17-6305-2017, https://doi.org/10.5194/acp-17-6305-2017, 2017
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We use observations from 2004 to 2012 to obtain estimates of the aerosol–cloud radiative effect, including its uncertainty, for dust aerosol influencing Atlantic marine stratocumulus clouds (MSc) off the coast of north Africa. Saharan dust modifies MSc in a way that acts to cool the planet. There is a strong seasonal variation, with the aerosol–cloud radiative effect switching from significantly negative during the boreal summer to weakly positive during boreal winter.
Hanna Joos, Erica Madonna, Kasja Witlox, Sylvaine Ferrachat, Heini Wernli, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 6243–6255, https://doi.org/10.5194/acp-17-6243-2017, https://doi.org/10.5194/acp-17-6243-2017, 2017
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The influence of pollution on the precipitation formation in warm conveyor belts (WCBs), the most rising air streams in low-pressure systems is investigated. We investigate in detail the cloud properties and resulting precipitation along these rising airstreams which are simulated with a global climate model. Overall, no big impact of aerosols on precipitation can be seen, however, when comparing the most polluted/cleanest WCBs, a suppression of precipitation by aerosols is observed.
Blaž Gasparini, Steffen Münch, Laure Poncet, Monika Feldmann, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 4871–4885, https://doi.org/10.5194/acp-17-4871-2017, https://doi.org/10.5194/acp-17-4871-2017, 2017
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Cirrus clouds have, unlike other cloud types, a warming impact on climate. Decreasing their frequency therefore leads to a cooling effect. Cirrus ice crystals grow larger when formed on solid aerosols, inducing a shorter cloud lifetime.
We compare simplified simulations of stripping cirrus out of the sky with simulations of seeding by aerosol injections. While we find the surface climate responses to be similar, the changes in clouds and cloud properties differ significantly.
Alexander Beck, Jan Henneberger, Sarah Schöpfer, Jacob Fugal, and Ulrike Lohmann
Atmos. Meas. Tech., 10, 459–476, https://doi.org/10.5194/amt-10-459-2017, https://doi.org/10.5194/amt-10-459-2017, 2017
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In situ observations of cloud properties in complex alpine terrain are commonly conducted at mountain-top research stations and limited to single-point measurements. The HoloGondel platform overcomes this limitation by using a cable car to obtain vertical profiles of the microphysical and meteorological cloud parameters. In this work example measurements of the vertical profiles observed in a liquid cloud and a mixed-phase cloud at the Eggishorn in the Swiss Alps are presented.
Luisa Ickes, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 1713–1739, https://doi.org/10.5194/acp-17-1713-2017, https://doi.org/10.5194/acp-17-1713-2017, 2017
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The goal of this study is to find a parameterization scheme for general circulation models to describe immersion freezing with the ability to shift and adjust the slope of the freezing curve compared to homogeneous freezing to match experimental data. We investigated how accurate different formulations of classical nucleation theory reproduce measured immersion freezing curves for different mineral dust types.
Yvonne Boose, André Welti, James Atkinson, Fabiola Ramelli, Anja Danielczok, Heinz G. Bingemer, Michael Plötze, Berko Sierau, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 15075–15095, https://doi.org/10.5194/acp-16-15075-2016, https://doi.org/10.5194/acp-16-15075-2016, 2016
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We compare the immersion freezing behavior of four airborne to 11 surface-collected dust samples to investigate the role of different minerals for atmospheric ice nucleation on desert dust. We find that present K-feldspars dominate at T > 253 K, while quartz does at colder temperatures, and surface-collected dust samples are not necessarily representative for airborne dust. For improved ice cloud prediction, modeling of quartz and feldspar emission and transport are key.
Yvonne Boose, Berko Sierau, M. Isabel García, Sergio Rodríguez, Andrés Alastuey, Claudia Linke, Martin Schnaiter, Piotr Kupiszewski, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 9067–9087, https://doi.org/10.5194/acp-16-9067-2016, https://doi.org/10.5194/acp-16-9067-2016, 2016
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Mineral dust is known to be among the most prevalent ice-nucleating particles (INPs) in the atmosphere, playing a crucial role for ice cloud formation. We present 2 months of ground-based in situ measurements of INP concentrations in the free troposphere close to the largest global dust source, the Sahara. We find that some atmospheric processes such as mixing with biological particles and ammonium increase the dust INP ability. This is important when predicting INPs based on emissions.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
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The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
Claudia Marcolli, Baban Nagare, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8915–8937, https://doi.org/10.5194/acp-16-8915-2016, https://doi.org/10.5194/acp-16-8915-2016, 2016
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Silver iodide is one of the best-investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Nevertheless, many open questions remain. This paper gives an overview of silver iodide as an ice nucleus and tries to identify the factors that influence the ice nucleation ability of silver iodide.
Sarvesh Garimella, Thomas Bjerring Kristensen, Karolina Ignatius, Andre Welti, Jens Voigtländer, Gourihar R. Kulkarni, Frank Sagan, Gregory Lee Kok, James Dorsey, Leonid Nichman, Daniel Alexander Rothenberg, Michael Rösch, Amélie Catharina Ruth Kirchgäßner, Russell Ladkin, Heike Wex, Theodore W. Wilson, Luis Antonio Ladino, Jon P. D. Abbatt, Olaf Stetzer, Ulrike Lohmann, Frank Stratmann, and Daniel James Cziczo
Atmos. Meas. Tech., 9, 2781–2795, https://doi.org/10.5194/amt-9-2781-2016, https://doi.org/10.5194/amt-9-2781-2016, 2016
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The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nuclei counter manufactured by Droplet Measurement Technologies in Boulder, CO. This study characterizes the SPIN chamber, reporting data from laboratory measurements and quantifying uncertainties. Overall, we report that the SPIN is able to reproduce previous CFDC ice nucleation measurements.
Shipeng Zhang, Minghuai Wang, Steven J. Ghan, Aijun Ding, Hailong Wang, Kai Zhang, David Neubauer, Ulrike Lohmann, Sylvaine Ferrachat, Toshihiko Takeamura, Andrew Gettelman, Hugh Morrison, Yunha Lee, Drew T. Shindell, Daniel G. Partridge, Philip Stier, Zak Kipling, and Congbin Fu
Atmos. Chem. Phys., 16, 2765–2783, https://doi.org/10.5194/acp-16-2765-2016, https://doi.org/10.5194/acp-16-2765-2016, 2016
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The variation of aerosol indirect effects (AIE) in several climate models is investigated across different dynamical regimes. Regimes with strong large-scale ascent are shown to be as important as stratocumulus regimes in studying AIE. AIE over regions with high monthly large-scale surface precipitation rate contributes the most to the total aerosol indirect forcing. These results point to the need to reduce the uncertainty in AIE in different dynamical regimes.
B. Nagare, C. Marcolli, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 15, 13759–13776, https://doi.org/10.5194/acp-15-13759-2015, https://doi.org/10.5194/acp-15-13759-2015, 2015
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We determined collision efficiencies of cloud droplets with aerosol particles experimentally and found that they were around 1 order of magnitude higher than theoretical formulations that include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This is most probably due to uncertainties and inaccuracies in the theoretical formulations of thermophoretic and diffusiophoretic processes.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
J. C. Corbin, A. Othman, J. D. Allan, D. R. Worsnop, J. D. Haskins, B. Sierau, U. Lohmann, and A. A. Mensah
Atmos. Meas. Tech., 8, 4615–4636, https://doi.org/10.5194/amt-8-4615-2015, https://doi.org/10.5194/amt-8-4615-2015, 2015
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Peak-integration uncertainties in the Aerodyne high-resolution aerosol mass spectrometer (AMS) are analyzed in detail using a combination of empirical data analysis and Monte Carlo approaches. The most general conclusion, applicable to any mass spectrometer, is that non-zero mass accuracy leads to a percentage error in constrained peak fits, even for well-resolved peaks. For overlapping peaks, this mass-accuracy effect may be viewed as a reduction in the effective m/z-calibration precision.
J. C. Corbin, U. Lohmann, B. Sierau, A. Keller, H. Burtscher, and A. A. Mensah
Atmos. Chem. Phys., 15, 11885–11907, https://doi.org/10.5194/acp-15-11885-2015, https://doi.org/10.5194/acp-15-11885-2015, 2015
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The chemical composition of wood-combustion soot is investigated using a soot-particle aerosol mass spectrometer. The analysis elucidates real-time information on BC oxygenated surface functional groups for a real-world source for the first time. Additional insights into the source of organic material in this soot are provided by positive matrix factorization of the data using a new AMS error model.
E. Hammer, N. Bukowiecki, B. P. Luo, U. Lohmann, C. Marcolli, E. Weingartner, U. Baltensperger, and C. R. Hoyle
Atmos. Chem. Phys., 15, 10309–10323, https://doi.org/10.5194/acp-15-10309-2015, https://doi.org/10.5194/acp-15-10309-2015, 2015
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An important quantity which determines aerosol activation and cloud formation is the effective peak supersaturation. The box model ZOMM was used to simulate the effective peak supersaturation experienced by an air parcel approaching a high-alpine research station in Switzerland. With the box model the sensitivity of the effective peak supersaturation to key aerosol and dynamical parameters was investigated.
P. Tuccella, G. Curci, G. A. Grell, G. Visconti, S. Crumeyrolle, A. Schwarzenboeck, and A. A. Mensah
Geosci. Model Dev., 8, 2749–2776, https://doi.org/10.5194/gmd-8-2749-2015, https://doi.org/10.5194/gmd-8-2749-2015, 2015
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A parameterization for secondary organic aerosol (SOA) production based on the volatility basis set (VBS) approach has been coupled with microphysics and radiative schemes in the WRF-Chem model. The new chemistry was evaluated on a cloud-resolving scale against ground-based and aircraft measurements collected during the IMPACT-EUCAARI campaign, and complemented with satellite data from MODIS. Sensitivity tests have been performed to study the impact of SOA on cloud prediction and development.
S. Pousse-Nottelmann, E. M. Zubler, and U. Lohmann
Atmos. Chem. Phys., 15, 9217–9236, https://doi.org/10.5194/acp-15-9217-2015, https://doi.org/10.5194/acp-15-9217-2015, 2015
V. Sant, R. Posselt, and U. Lohmann
Atmos. Chem. Phys., 15, 8717–8738, https://doi.org/10.5194/acp-15-8717-2015, https://doi.org/10.5194/acp-15-8717-2015, 2015
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We have introduced prognostic precipitation for both liquid (drizzle and rain) and solid (snow) phase precipitation into the global circulation model ECHAM5-HAM. This has a significant effect on the clouds and the parameterized collection rates, also reducing the sensitivity of the liquid water path to the anthropogenic aerosol forcing. Altogether the results suggest that the treatment of precipitation in global circulation models has a significant influence on the phase and lifetime of clouds.
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
A. Possner, E. Zubler, U. Lohmann, and C. Schär
Atmos. Chem. Phys., 15, 2185–2201, https://doi.org/10.5194/acp-15-2185-2015, https://doi.org/10.5194/acp-15-2185-2015, 2015
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For the first time, real-case simulations of ship tracks are performed at the 2km scale and evaluated against observations. Simulations show that ship tracks are quantitatively and qualitatively captured by the model. Therefore, this approach could be used to evaluate the interplay between parameterisations for aerosol–cloud interactions which occur, in the case of ship tracks, in spatially defined regions and under constrained environmental conditions.
D. Neubauer, U. Lohmann, C. Hoose, and M. G. Frontoso
Atmos. Chem. Phys., 14, 11997–12022, https://doi.org/10.5194/acp-14-11997-2014, https://doi.org/10.5194/acp-14-11997-2014, 2014
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Several biases in the representation of clouds in the stratocumulus regime in the ECHAM6-HAM2 global climate model were found by evaluating the model in the stratocumulus cloud regime. Simulations with changes in model resolution and physics to better represent clouds and aerosol in the stratocumulus regime show that the human influence on clouds and thus climate by emission of aerosol particles is sensitive to the representation of (stratocumulus) clouds.
B. Sierau, R. Y.-W. Chang, C. Leck, J. Paatero, and U. Lohmann
Atmos. Chem. Phys., 14, 7409–7430, https://doi.org/10.5194/acp-14-7409-2014, https://doi.org/10.5194/acp-14-7409-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
M. Kuebbeler, U. Lohmann, J. Hendricks, and B. Kärcher
Atmos. Chem. Phys., 14, 3027–3046, https://doi.org/10.5194/acp-14-3027-2014, https://doi.org/10.5194/acp-14-3027-2014, 2014
J. C. Corbin, B. Sierau, M. Gysel, M. Laborde, A. Keller, J. Kim, A. Petzold, T. B. Onasch, U. Lohmann, and A. A. Mensah
Atmos. Chem. Phys., 14, 2591–2603, https://doi.org/10.5194/acp-14-2591-2014, https://doi.org/10.5194/acp-14-2591-2014, 2014
A. Baklanov, K. Schlünzen, P. Suppan, J. Baldasano, D. Brunner, S. Aksoyoglu, G. Carmichael, J. Douros, J. Flemming, R. Forkel, S. Galmarini, M. Gauss, G. Grell, M. Hirtl, S. Joffre, O. Jorba, E. Kaas, M. Kaasik, G. Kallos, X. Kong, U. Korsholm, A. Kurganskiy, J. Kushta, U. Lohmann, A. Mahura, A. Manders-Groot, A. Maurizi, N. Moussiopoulos, S. T. Rao, N. Savage, C. Seigneur, R. S. Sokhi, E. Solazzo, S. Solomos, B. Sørensen, G. Tsegas, E. Vignati, B. Vogel, and Y. Zhang
Atmos. Chem. Phys., 14, 317–398, https://doi.org/10.5194/acp-14-317-2014, https://doi.org/10.5194/acp-14-317-2014, 2014
M. Paglione, A. Kiendler-Scharr, A. A. Mensah, E. Finessi, L. Giulianelli, S. Sandrini, M. C. Facchini, S. Fuzzi, P. Schlag, A. Piazzalunga, E. Tagliavini, J. S. Henzing, and S. Decesari
Atmos. Chem. Phys., 14, 25–45, https://doi.org/10.5194/acp-14-25-2014, https://doi.org/10.5194/acp-14-25-2014, 2014
J. Henneberger, J. P. Fugal, O. Stetzer, and U. Lohmann
Atmos. Meas. Tech., 6, 2975–2987, https://doi.org/10.5194/amt-6-2975-2013, https://doi.org/10.5194/amt-6-2975-2013, 2013
L. A. Ladino Moreno, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 13, 9745–9769, https://doi.org/10.5194/acp-13-9745-2013, https://doi.org/10.5194/acp-13-9745-2013, 2013
Z. A. Kanji, A. Welti, C. Chou, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 13, 9097–9118, https://doi.org/10.5194/acp-13-9097-2013, https://doi.org/10.5194/acp-13-9097-2013, 2013
C. A. Randles, S. Kinne, G. Myhre, M. Schulz, P. Stier, J. Fischer, L. Doppler, E. Highwood, C. Ryder, B. Harris, J. Huttunen, Y. Ma, R. T. Pinker, B. Mayer, D. Neubauer, R. Hitzenberger, L. Oreopoulos, D. Lee, G. Pitari, G. Di Genova, J. Quaas, F. G. Rose, S. Kato, S. T. Rumbold, I. Vardavas, N. Hatzianastassiou, C. Matsoukas, H. Yu, F. Zhang, H. Zhang, and P. Lu
Atmos. Chem. Phys., 13, 2347–2379, https://doi.org/10.5194/acp-13-2347-2013, https://doi.org/10.5194/acp-13-2347-2013, 2013
C. Chou, Z. A. Kanji, O. Stetzer, T. Tritscher, R. Chirico, M. F. Heringa, E. Weingartner, A. S. H. Prévôt, U. Baltensperger, and U. Lohmann
Atmos. Chem. Phys., 13, 761–772, https://doi.org/10.5194/acp-13-761-2013, https://doi.org/10.5194/acp-13-761-2013, 2013
M. Gysel, M. Laborde, A. A. Mensah, J. C. Corbin, A. Keller, J. Kim, A. Petzold, and B. Sierau
Atmos. Meas. Tech., 5, 3099–3107, https://doi.org/10.5194/amt-5-3099-2012, https://doi.org/10.5194/amt-5-3099-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Magnetic fraction of the atmospheric dust in Kraków – physicochemical characteristics and possible environmental impact
Modeling daytime and nighttime secondary organic aerosol formation via multiphase reactions of biogenic hydrocarbons
SO2 enhances aerosol formation from anthropogenic volatile organic compound ozonolysis by producing sulfur-containing compounds
Isothermal evaporation of α-pinene secondary organic aerosol particles formed under low NOx and high NOx conditions
Chemical characterization of organic compounds involved in iodine-initiated new particle formation from coastal macroalgal emission
The Urmia playa as a source of airborne dust and ice-nucleating particles – Part 2: Unraveling the relationship between soil dust composition and ice nucleation activity
Winter brown carbon over six of China's megacities: light absorption, molecular characterization, and improved source apportionment revealed by multilayer perceptron neural network
Chamber investigation of the formation and transformation of secondary organic aerosol in mixtures of biogenic and anthropogenic volatile organic compounds
Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types
Comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) from heavy-duty diesel vehicles using two-dimensional gas chromatography time-of-flight mass spectrometry
Measurement report: Investigation of pH- and particle-size-dependent chemical and optical properties of water-soluble organic carbon: implications for its sources and aging processes
The influence of the addition of isoprene on the volatility of particles formed from the photo-oxidation of anthropogenic–biogenic mixtures
Significant formation of sulfate aerosols contributed by the heterogeneous drivers of dust surface
Particle-phase processing of α-pinene NO3 secondary organic aerosol in the dark
Technical note: Identification of chemical composition and source of fluorescent components in atmospheric water-soluble brown carbon by excitation-emission matrix with parallel factor analysis: Potential limitation and application
Chemical characteristics and sources of PM2.5 in Hohhot, a semi-arid city in northern China: insight from the COVID-19 lockdown
The positive effect of formaldehyde on the photocatalytic renoxification of nitrate on TiO2 particles
Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical
A comprehensive study on hygroscopic behaviour and nitrate depletion of NaNO3 and dicarboxylic acid mixtures: implications for nitrate depletion in tropospheric aerosols
Secondary organic aerosols from OH oxidation of cyclic volatile methyl siloxanes as an important Si source in the atmosphere
Aqueous SOA formation from photosensitized guaiacol oxidation: Comparison between non-phenolic and phenolic methoxybenzaldehydes as photosensitizers in the absence and presence of ammonium nitrate
Effects of OH radical and SO2 concentrations on photochemical reactions of mixed anthropogenic organic gases
Effects of the sample matrix on the photobleaching and photodegradation of toluene-derived secondary organic aerosol compounds
Functionality-based formation of secondary organic aerosol from m-xylene photooxidation
Chemical composition of secondary organic aerosol particles formed from mixtures of anthropogenic and biogenic precursors
A novel pathway of atmospheric sulfate formation through carbonate radicals
A sulfuric acid nucleation potential model for the atmosphere
Optical and chemical properties and oxidative potential of aqueous-phase products from OH and 3C∗-initiated photooxidation of eugenol
The relationship between PM2.5 and anticyclonic wave activity during summer over the United States
Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions
Cellulose in atmospheric particulate matter at rural and urban sites across France and Switzerland
Kinetics, SOA yields, and chemical composition of secondary organic aerosol from β-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K
Chemical transformation of α-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates
Aqueous chemical bleaching of 4-nitrophenol brown carbon by hydroxyl radicals; products, mechanism, and light absorption
Secondary organic aerosol formation from camphene oxidation: measurements and modeling
Technical note: Real-time diagnosis of the hygroscopic growth micro-dynamics of nanoparticles with Fourier transform infrared spectroscopy
Single-particle Raman spectroscopy for studying physical and chemical processes of atmospheric particles
Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?
Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates
Secondary organic aerosol formation from the oxidation of decamethylcyclopentasiloxane at atmospherically relevant OH concentrations
Aqueous secondary organic aerosol formation from the direct photosensitized oxidation of vanillin in the absence and presence of ammonium nitrate
Evolution of volatility and composition in sesquiterpene-mixed and α-pinene secondary organic aerosol particles during isothermal evaporation
Potential new tracers and their mass fraction in the emitted PM10 from the burning of household waste in stoves
Synergetic effects of NH3 and NOx on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation
Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature
Technical note: Adsorption and desorption equilibria from statistical thermodynamics and rates from transition state theory
Nighttime chemistry of biomass burning emissions in urban areas: A dual mobile chamber study
Formation and evolution of secondary organic aerosols derived from urban-lifestyle sources: vehicle exhaust and cooking emissions
Mass spectral characterization of secondary organic aerosol from urban cooking and vehicular sources
An organic crystalline state in ageing atmospheric aerosol proxies: spatially resolved structural changes in levitated fatty acid particles
Jan M. Michalik, Wanda Wilczyńska-Michalik, Łukasz Gondek, Waldemar Tokarz, Jan Żukrowski, Marta Gajewska, and Marek Michalik
Atmos. Chem. Phys., 23, 1449–1464, https://doi.org/10.5194/acp-23-1449-2023, https://doi.org/10.5194/acp-23-1449-2023, 2023
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The magnetic fraction of the aerosols in Kraków was collected and analysed using scanning and transmission electron microscopy with energy-dispersive spectrometry, X-ray diffraction, Mössbauer spectrometry, and magnetometry. It contains metallic Fe or Fe-rich alloy and Fe oxides. The occurrence of nanometre-scale Fe3O4 particles (predominantly of anthropogenic origin) is shown. Our results can help to determine the sources and transport of pollutants, potential harmful effects, etc.
Sanghee Han and Myoseon Jang
Atmos. Chem. Phys., 23, 1209–1226, https://doi.org/10.5194/acp-23-1209-2023, https://doi.org/10.5194/acp-23-1209-2023, 2023
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The diurnal pattern in biogenic secondary organic aerosol (SOA) formation is simulated by using the UNIPAR model, which predicts SOA growth via multiphase reactions of hydrocarbons under varying NOx levels, aerosol acidity, humidity, and temperature. The simulation suggests that nighttime SOA formation, even in urban environments, where anthropogenic emission is high, is dominated by products from ozonolysis and NO3-initiated oxidation of biogenic hydrocarbons.
Zhaomin Yang, Kun Li, Narcisse T. Tsona, Xin Luo, and Lin Du
Atmos. Chem. Phys., 23, 417–430, https://doi.org/10.5194/acp-23-417-2023, https://doi.org/10.5194/acp-23-417-2023, 2023
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SO2 significantly promotes particle formation during cyclooctene ozonolysis. Carboxylic acids and their dimers were major products in particles formed in the absence of SO2. SO2 can induce production of organosulfates with stronger particle formation ability than their precursors, leading to the enhancement in particle formation. Formation mechanisms and structures of organosulfates were proposed, which is helpful for better understanding how SO2 perturbs the formation and fate of particles.
Zijun Li, Angela Buchholz, Luis M. F. Barreira, Arttu Ylisirniö, Liqing Hao, Iida Pullinen, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 23, 203–220, https://doi.org/10.5194/acp-23-203-2023, https://doi.org/10.5194/acp-23-203-2023, 2023
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Interaction between NOx and biogenic emissions can be important in suburban areas. Our study showed that the addition of NOx during α-pinene SOA formation produced considerable amounts of organic nitrates and affected the composition of non-nitrated organic compounds. The compositional difference consequently altered the primary type of aqueous-phase processes during the isothermal particle evaporation.
Yibei Wan, Xiangpeng Huang, Chong Xing, Qiongqiong Wang, Xinlei Ge, and Huan Yu
Atmos. Chem. Phys., 22, 15413–15423, https://doi.org/10.5194/acp-22-15413-2022, https://doi.org/10.5194/acp-22-15413-2022, 2022
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The organic compounds involved in continental new particle formation have been investigated in depth in the last 2 decades. In contrast, no prior work has studied the exact chemical composition of organic compounds and their role in coastal new particle formation. We present a complementary study to the ongoing laboratory and field research on iodine nucleation in the coastal atmosphere. This study provided a more complete story of coastal I-NPF from low-tide macroalgal emission.
Nikou Hamzehpour, Claudia Marcolli, Kristian Klumpp, Debora Thöny, and Thomas Peter
Atmos. Chem. Phys., 22, 14931–14956, https://doi.org/10.5194/acp-22-14931-2022, https://doi.org/10.5194/acp-22-14931-2022, 2022
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Dust aerosols from dried lakebeds contain mineral particles, as well as soluble salts and (bio-)organic compounds. Here, we investigate ice nucleation (IN) activity of dust samples from Lake Urmia playa, Iran. We find high IN activity of the untreated samples that decreases after organic matter removal but increases after removing soluble salts and carbonates, evidencing inhibiting effects of soluble salts and carbonates on the IN activity of organic matter and minerals, especially microcline.
Diwei Wang, Zhenxing Shen, Qian Zhang, Yali Lei, Tian Zhang, Shasha Huang, Jian Sun, Hongmei Xu, and Junji Cao
Atmos. Chem. Phys., 22, 14893–14904, https://doi.org/10.5194/acp-22-14893-2022, https://doi.org/10.5194/acp-22-14893-2022, 2022
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The optical properties and molecular structure of atmospheric brown carbon (BrC) in winter of several megacities in China were analyzed, and the source contribution of brown carbon was improved by using positive matrix factorization coupled with a multilayer perceptron neural network. These results can provide a basis for the more effective control of BrC to reduce its impacts on regional climates and human health.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 22, 14147–14175, https://doi.org/10.5194/acp-22-14147-2022, https://doi.org/10.5194/acp-22-14147-2022, 2022
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Mixing experiments are crucial and highly beneficial for our understanding of atmospheric chemical interactions. However, interpretation quickly becomes complex, and both the experimental design and evaluation need to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in SOA formed from mixtures of VOCs.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys., 22, 13783–13796, https://doi.org/10.5194/acp-22-13783-2022, https://doi.org/10.5194/acp-22-13783-2022, 2022
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The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types that are internally mixed within individual particles.
Xiao He, Xuan Zheng, Shaojun Zhang, Xuan Wang, Ting Chen, Xiao Zhang, Guanghan Huang, Yihuan Cao, Liqiang He, Xubing Cao, Yuan Cheng, Shuxiao Wang, and Ye Wu
Atmos. Chem. Phys., 22, 13935–13947, https://doi.org/10.5194/acp-22-13935-2022, https://doi.org/10.5194/acp-22-13935-2022, 2022
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With the use of two-dimensional gas chromatography time-of-flight mass spectrometry (GC × GC ToF-MS), we successfully give a comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emitted from heavy-duty diesel vehicles. I/SVOCs are speciated, identified, and quantified based on the patterns of the mass spectrum, and the gas–particle partitioning is fully addressed.
Yuanyuan Qin, Juanjuan Qin, Xiaobo Wang, Kang Xiao, Ting Qi, Yuwei Gao, Xueming Zhou, Shaoxuan Shi, Jingnan Li, Jingsi Gao, Ziyin Zhang, Jihua Tan, Yang Zhang, and Rongzhi Chen
Atmos. Chem. Phys., 22, 13845–13859, https://doi.org/10.5194/acp-22-13845-2022, https://doi.org/10.5194/acp-22-13845-2022, 2022
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Deep interrogation of water-soluble organic carbon (WSOC) in aerosols is critical and challenging considering its involvement in many key aerosol-associated chemical reactions. This work examined how the chemical structures (functional groups) and optical properties (UV/fluorescence properties) of WSOC were affected by pH and particle size. We found that the pH- and particle-size-dependent behaviors could be used to reveal the structures, sources, and aging of aerosol WSOC.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Tao Wang, Yangyang Liu, Hanyun Cheng, Zhenzhen Wang, Hongbo Fu, Jianmin Chen, and Liwu Zhang
Atmos. Chem. Phys., 22, 13467–13493, https://doi.org/10.5194/acp-22-13467-2022, https://doi.org/10.5194/acp-22-13467-2022, 2022
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This study compared the gas-phase, aqueous-phase, and heterogeneous SO2 oxidation pathways by combining laboratory work with a modelling study. The heterogeneous oxidation, particularly that induced by the dust surface drivers, presents positive implications for the removal of airborne SO2 and formation of sulfate aerosols. This work highlighted the atmospheric significance of heterogeneous oxidation and suggested a comparison model to evaluate the following heterogeneous laboratory research.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Tao Cao, Meiju Li, Cuncun Xu, Jianzhong Song, Xingjun Fan, Jun Li, Wanglu Jia, and Ping’an Peng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-676, https://doi.org/10.5194/acp-2022-676, 2022
Revised manuscript accepted for ACP
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This study comprehensively investigated the fluorescence data of strong light-absorbing organic compounds, water-soluble organic matter in different types of aerosol samples, soil dust, and fulvic/humic acids by an EEM-parallel factor method. The results revealed which light-absorbing species can be detected by EEM and also provided important information for identifying the chemical compositions and possible sources of these species in atmospheric BrC.
Haijun Zhou, Tao Liu, Bing Sun, Yongli Tian, Xingjun Zhou, Feng Hao, Xi Chun, Zhiqiang Wan, Peng Liu, Jingwen Wang, and Dagula Du
Atmos. Chem. Phys., 22, 12153–12166, https://doi.org/10.5194/acp-22-12153-2022, https://doi.org/10.5194/acp-22-12153-2022, 2022
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A single year’s offline measurement was conducted in Hohhot to reveal the chemical characteristics and sources of PM2.5 in a semi-arid region. We believe that our study makes a significant contribution to the literature because relatively few studies have focused on the chemical composition and sources of PM2.5 with offline measurements. A knowledge gap exists concerning how chemical composition and sources respond to implemented control measures for aerosols, particularly in a semi-arid region.
Yuhan Liu, Xuejiao Wang, Jing Shang, Weiwei Xu, Mengshuang Sheng, and Chunxiang Ye
Atmos. Chem. Phys., 22, 11347–11358, https://doi.org/10.5194/acp-22-11347-2022, https://doi.org/10.5194/acp-22-11347-2022, 2022
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In this study, the influence of HCHO on renoxification on nitrate-doped TiO2 particles is investigated by using an experimental chamber. Mass NOx release is suggested to follow the NO−3-NO3·-HNO3-NOx pathway, with HCHO involved in the transformation of NO3· to HNO3 through hydrogen abstraction. Our proposed reaction mechanism by which HCHO promotes photocatalytic renoxification is helpful for deeply understanding the atmospheric photochemical processes and nitrogen cycling.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, https://doi.org/10.5194/acp-22-11323-2022, 2022
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The oxidation of limonene, a common volatile emitted by trees and chemical products, by NO3, a nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10-30 compounds. Most of the HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted for a major fraction. Their formation can be explained by chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
Shuaishuai Ma, Qiong Li, and Yunhong Zhang
Atmos. Chem. Phys., 22, 10955–10970, https://doi.org/10.5194/acp-22-10955-2022, https://doi.org/10.5194/acp-22-10955-2022, 2022
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The nitrate phase state can play a critical role in determining the occurrence and extent of nitrate depletion in internally mixed NaNO3–DCA particles, which may be instructive for relevant aerosol reaction systems. Besides, organic acids have a potential to deplete nitrate based on the comprehensive consideration of acidity, particle-phase state, droplet water activity, and HNO3 gas-phase diffusion.
Chong Han, Hongxing Yang, Kun Li, Patrick Lee, John Liggio, Amy Leithead, and Shao-Meng Li
Atmos. Chem. Phys., 22, 10827–10839, https://doi.org/10.5194/acp-22-10827-2022, https://doi.org/10.5194/acp-22-10827-2022, 2022
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We presented yields and compositions of Si-containing SOAs generated from the reaction of cVMSs (D3–D6) with OH radicals. NOx played a negative role in cVMS SOA formation, while ammonium sulfate seeds enhanced D3–D5 SOA yields at short photochemical ages under high-NOx conditions. The aerosol mass spectra confirmed that the components of cVMS SOAs significantly relied on OH exposure. A global cVMS-derived SOA source strength was estimated in order to understand SOA formation potentials of cVMSs.
Beatrix Rosette Go Mabato, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak Keung Chan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-595, https://doi.org/10.5194/acp-2022-595, 2022
Revised manuscript accepted for ACP
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We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud/fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings would be useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA-predictive models.
Junling Li, Kun Li, Hao Zhang, Xin Zhang, Yuanyuan Ji, Wanghui Chu, Yuxue Kong, Yangxi Chu, Yanqin Ren, Yujie Zhang, Haijie Zhang, Rui Gao, Zhenhai Wu, Fang Bi, Xuan Chen, Xuezhong Wang, Weigang Wang, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 22, 10489–10504, https://doi.org/10.5194/acp-22-10489-2022, https://doi.org/10.5194/acp-22-10489-2022, 2022
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Ozone formation is enhanced by higher OH concentration and higher temperature but is influenced little by SO2. SO2 can largely enhance the particle formation. Organo-sulfates and organo-nitrates are detected in the formed particles, and the presence of SO2 can promote the formation of organo-sulfates. The results provide a scientific basis for systematically evaluating the effects of SO2, OH concentration, and temperature on the oxidation of mixed organic gases in the atmosphere.
Alexandra L. Klodt, Marley Adamek, Monica Dibley, Sergey A. Nizkorodov, and Rachel E. O'Brien
Atmos. Chem. Phys., 22, 10155–10171, https://doi.org/10.5194/acp-22-10155-2022, https://doi.org/10.5194/acp-22-10155-2022, 2022
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We investigated photochemistry of a secondary organic aerosol under three different conditions: in a dilute aqueous solution mimicking cloud droplets, in a solution of concentrated ammonium sulfate mimicking deliquesced aerosol, and in an organic matrix mimicking dry organic aerosol. We find that rate and mechanisms of photochemistry depend sensitively on these conditions, suggesting that the same organic aerosol compounds will degrade at different rates depending on their local environment.
Yixin Li, Jiayun Zhao, Mario Gomez-Hernandez, Michael Lavallee, Natalie M. Johnson, and Renyi Zhang
Atmos. Chem. Phys., 22, 9843–9857, https://doi.org/10.5194/acp-22-9843-2022, https://doi.org/10.5194/acp-22-9843-2022, 2022
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Here we elucidate the production of COOs and their roles in SOA and brown carbon formation from m-xylene oxidation by simultaneously monitoring the evolution of gas-phase products and aerosol properties in an environmental chamber. A kinetic framework is developed to predict SOA production from the concentrations and uptake coefficients for COOs. This functionality-based approach reproduces SOA formation from m-xylene oxidation well and is applicable to VOC oxidation for other species.
Yunqi Shao, Aristeidis Voliotis, Mao Du, Yu Wang, Kelly Pereira, Jacqueline Hamilton, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 9799–9826, https://doi.org/10.5194/acp-22-9799-2022, https://doi.org/10.5194/acp-22-9799-2022, 2022
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This study explored the chemical properties of secondary organic aerosol (SOA) that formed from photo-oxidation of single and mixed biogenic and anthropogenic precursors. We showed that SOA chemical properties in a mixed vapour system are mainly affected by the
higher-yield precursor's oxidation products and products from
cross-product formation. This study also identifies potential tracer compounds in a mixed vapour system that might be used in SOA source attribution in future ambient studies.
Yangyang Liu, Yue Deng, Jiarong Liu, Xiaozhong Fang, Tao Wang, Kejian Li, Kedong Gong, Aziz U. Bacha, Iqra Nabi, Qiuyue Ge, Xiuhui Zhang, Christian George, and Liwu Zhang
Atmos. Chem. Phys., 22, 9175–9197, https://doi.org/10.5194/acp-22-9175-2022, https://doi.org/10.5194/acp-22-9175-2022, 2022
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Both CO2 and carbonate salt work as the precursor of carbonate radicals, which largely promotes sulfate formation during the daytime. This study provides the first indication that the carbonate radical not only plays a role as an intermediate in tropospheric anion chemistry but also as a strong oxidant for the surface processing of trace gas in the atmosphere. CO2, carbponate radicals, and sulfate receive attention from those looking at the environment, atmosphere, aerosol, and photochemistry.
Jack S. Johnson and Coty N. Jen
Atmos. Chem. Phys., 22, 8287–8297, https://doi.org/10.5194/acp-22-8287-2022, https://doi.org/10.5194/acp-22-8287-2022, 2022
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Sulfuric acid nucleation forms particles in Earth's atmosphere that influence cloud formation and climate. This study introduces the Nucleation Potential Model, which simplifies the diverse reactions between sulfuric acid and numerous precursor gases to predict nucleation rates. Results show that the model is capable of estimating the potency and concentration of mixtures of precursor gases from laboratory and field observations and can be used to model nucleation across diverse environments.
Xudong Li, Ye Tao, Longwei Zhu, Shuaishuai Ma, Shipeng Luo, Zhuzi Zhao, Ning Sun, Xinlei Ge, and Zhaolian Ye
Atmos. Chem. Phys., 22, 7793–7814, https://doi.org/10.5194/acp-22-7793-2022, https://doi.org/10.5194/acp-22-7793-2022, 2022
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This work has, for the first time, investigated the optical and chemical properties and oxidative potential of aqueous-phase photooxidation products of eugenol (a biomass-burning-emitted compound) and elucidated the interplay among these properties. Large mass yields exceeding 100 % were found, and the aqueous processing is a source of BrC (likely relevant with humic-like substances). We also show that aqueous processing can produce species that are more toxic than that of its precursor.
Ye Wang, Natalie Mahowald, Peter Hess, Wenxiu Sun, and Gang Chen
Atmos. Chem. Phys., 22, 7575–7592, https://doi.org/10.5194/acp-22-7575-2022, https://doi.org/10.5194/acp-22-7575-2022, 2022
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PM2.5 is positively related to anticyclonic wave activity (AWA) changes close to the observing sites. Changes between current and future climates in AWA can explain up to 75 % of PM2.5 variability at some stations using a linear regression model. Our analysis indicates that higher PM2.5 concentrations occur when a positive AWA anomaly is prominent, which could be critical for understanding how pollutants respond to changing atmospheric circulation and for developing robust pollution projections.
Clarissa Baldo, Akinori Ito, Michael D. Krom, Weijun Li, Tim Jones, Nick Drake, Konstantin Ignatyev, Nicholas Davidson, and Zongbo Shi
Atmos. Chem. Phys., 22, 6045–6066, https://doi.org/10.5194/acp-22-6045-2022, https://doi.org/10.5194/acp-22-6045-2022, 2022
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High ionic strength relevant to the aerosol-water enhanced proton-promoted dissolution of iron in coal fly ash (up to 7 times) but suppressed oxalate-promoted dissolution at low pH (< 3). Fe in coal fly ash dissolved up to 7 times faster than in Saharan dust at low pH. A global model with the updated dissolution rates of iron in coal fly ash suggested a larger contribution of pyrogenic dissolved Fe over regions with a strong impact from fossil fuel combustions.
Adam Brighty, Véronique Jacob, Gaëlle Uzu, Lucille Borlaza, Sébastien Conil, Christoph Hueglin, Stuart K. Grange, Olivier Favez, Cécile Trébuchon, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 6021–6043, https://doi.org/10.5194/acp-22-6021-2022, https://doi.org/10.5194/acp-22-6021-2022, 2022
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With an revised analytical method and long-term sampling strategy, we have been able to elucidate much more information about atmospheric plant debris, a poorly understood class of particulate matter. We found weaker seasonal patterns at urban locations compared to rural locations and significant interannual variability in concentrations between previous years and 2020, during the COVID-19 pandemic. This suggests a possible man-made influence on plant debris concentration and source strength.
Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
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We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
Rongshuang Xu, Sze In Madeleine Ng, Wing Sze Chow, Yee Ka Wong, Yuchen Wang, Donger Lai, Zhongping Yao, Pui-Kin So, Jian Zhen Yu, and Man Nin Chan
Atmos. Chem. Phys., 22, 5685–5700, https://doi.org/10.5194/acp-22-5685-2022, https://doi.org/10.5194/acp-22-5685-2022, 2022
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To date, while over a hundred organosulfates (OSs) have been detected in atmospheric aerosols, many of them are still unidentified, with unknown precursors and formation processes. We found the heterogeneous OH oxidation of an α-pinene-derived organosulfate (C10H17O5SNa, αpOS-249, αpOS-249) can proceed at an efficient rate and transform into more oxygenated OSs, which have been commonly detected in atmospheric aerosols and α-pinene-derived SOA in chamber studies.
Bartłomiej Witkowski, Priyanka Jain, and Tomasz Gierczak
Atmos. Chem. Phys., 22, 5651–5663, https://doi.org/10.5194/acp-22-5651-2022, https://doi.org/10.5194/acp-22-5651-2022, 2022
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This article describes a comprehensive investigation of the aqueous oxidation of 4-nitrophenol (4NP) by hydroxyl radicals (OH). The reaction was carried out in a laboratory photoreactor. We report the formation of key intermediates under different pH conditions and the evolution of the light absorption of the reaction solution. The results provide new insights into the formation and removal (chemical bleaching) of light-absorbing organic aerosols (atmospheric brown carbon).
Qi Li, Jia Jiang, Isaac K. Afreh, Kelley C. Barsanti, and David R. Cocker III
Atmos. Chem. Phys., 22, 3131–3147, https://doi.org/10.5194/acp-22-3131-2022, https://doi.org/10.5194/acp-22-3131-2022, 2022
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Chamber-derived secondary organic aerosol (SOA) yields from camphene are reported for the first time. The role of peroxy radicals (RO2) was investigated using chemically detailed box models. We observed higher SOA yields (up to 64 %) in the experiments with added NOx than without due to the formation of highly oxygenated organic molecules (HOMs) when
NOx is present. This work can improve the representation of camphene in air quality models and provide insights into other monoterpene studies.
Xiuli Wei, Haosheng Dai, Huaqiao Gui, Jiaoshi Zhang, Yin Cheng, Jie Wang, Yixin Yang, Youwen Sun, and Jianguo Liu
Atmos. Chem. Phys., 22, 3097–3109, https://doi.org/10.5194/acp-22-3097-2022, https://doi.org/10.5194/acp-22-3097-2022, 2022
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We demonstrated the usage of the Fourier transform infrared (FTIR) spectroscopic technique to characterize in real time the hygroscopic growth properties of nanoparticles and their phase transition micro-dynamics at the molecular level. We first realize real-time measurements of water content and dry nanoparticle mass to characterize hygroscopic growth factors. We then identify in real time the hydration interactions and the dynamic hygroscopic growth process of the functional groups.
Zhancong Liang, Yangxi Chu, Masao Gen, and Chak K. Chan
Atmos. Chem. Phys., 22, 3017–3044, https://doi.org/10.5194/acp-22-3017-2022, https://doi.org/10.5194/acp-22-3017-2022, 2022
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The properties and fate of individual airborne particles can be significantly different, leading to distinct environmental impacts (e.g., climate and human health). While many instruments only analyze an ensemble of these particles, single-particle Raman spectroscopy enables unambiguous characterization of individual particles. This paper comprehensively reviews the applications of such a technique in studying atmospheric particles, especially for their physicochemical processing.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
Sophia M. Charan, Yuanlong Huang, Reina S. Buenconsejo, Qi Li, David R. Cocker III, and John H. Seinfeld
Atmos. Chem. Phys., 22, 917–928, https://doi.org/10.5194/acp-22-917-2022, https://doi.org/10.5194/acp-22-917-2022, 2022
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In this study, we investigate the secondary organic aerosol formation potential of decamethylcyclopentasiloxane (D5), which is used as a tracer for volatile chemical products and measured in high concentrations both outdoors and indoors. By performing experiments in different types of reactors, we find that D5’s aerosol formation is highly dependent on OH, and, at low OH concentrations or exposures, D5 forms little aerosol. We also reconcile results from other studies.
Beatrix Rosette Go Mabato, Yan Lyu, Yan Ji, Yong Jie Li, Dan Dan Huang, Xue Li, Theodora Nah, Chun Ho Lam, and Chak K. Chan
Atmos. Chem. Phys., 22, 273–293, https://doi.org/10.5194/acp-22-273-2022, https://doi.org/10.5194/acp-22-273-2022, 2022
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Biomass burning (BB) is a global phenomenon that releases large quantities of pollutants such as phenols and aromatic carbonyls into the atmosphere. These compounds can form secondary organic aerosols (SOAs) which play an important role in the Earth’s energy budget. In this work, we demonstrated that the direct irradiation of vanillin (VL) could generate aqueous SOA (aqSOA) such as oligomers. In the presence of nitrate, VL photo-oxidation can also form nitrated compounds.
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.
András Hoffer, Ádám Tóth, Beatrix Jancsek-Turóczi, Attila Machon, Aida Meiramova, Attila Nagy, Luminita Marmureanu, and András Gelencsér
Atmos. Chem. Phys., 21, 17855–17864, https://doi.org/10.5194/acp-21-17855-2021, https://doi.org/10.5194/acp-21-17855-2021, 2021
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Due to the widespread use of plastics high amounts of waste are burned in households worldwide, emitting vast amounts of PM10 and PAHs into the atmosphere. In this work different types of common plastics were burned in the laboratory with a view to identifying potentially specific tracer compounds and determining their emission factors. The compounds found were also successfully identified in atmospheric PM10 samples, indicating their potential use as ambient tracers for illegal waste burning.
Shijie Liu, Dandan Huang, Yiqian Wang, Si Zhang, Xiaodi Liu, Can Wu, Wei Du, and Gehui Wang
Atmos. Chem. Phys., 21, 17759–17773, https://doi.org/10.5194/acp-21-17759-2021, https://doi.org/10.5194/acp-21-17759-2021, 2021
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A series of chamber experiments was performed to probe the individual and common effects of NH3 and NOx on toluene secondary organic aerosol (SOA) formation through OH photooxidation. The synergetic effects of NH3 and NOx on the toluene SOA concentration and optical absorption were observed. The higher-volatility products formed in the presence of NOx could precipitate into the particle phase when NH3 was added. The formation pathways of N-containing OAs through NOx or NH3 are also discussed.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Daniel A. Knopf and Markus Ammann
Atmos. Chem. Phys., 21, 15725–15753, https://doi.org/10.5194/acp-21-15725-2021, https://doi.org/10.5194/acp-21-15725-2021, 2021
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Adsorption on and desorption of gas molecules from solid or liquid surfaces or interfaces represent the initial interaction of gas-to-condensed-phase processes that can define the physicochemical evolution of the condensed phase. We apply a thermodynamic and microscopic treatment of these multiphase processes to evaluate how adsorption and desorption rates and surface accommodation depend on the choice of adsorption model and standard states with implications for desorption energy and lifetimes.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Zirui Zhang, Wenfei Zhu, Min Hu, Kefan Liu, Hui Wang, Rongzhi Tang, Ruizhe Shen, Ying Yu, Rui Tan, Kai Song, Yuanju Li, Wenbin Zhang, Zhou Zhang, Hongming Xu, Shijin Shuai, Shuangde Li, Yunfa Chen, Jiayun Li, Yuesi Wang, and Song Guo
Atmos. Chem. Phys., 21, 15221–15237, https://doi.org/10.5194/acp-21-15221-2021, https://doi.org/10.5194/acp-21-15221-2021, 2021
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We comprehensively investigated the mass growth potential, oxidation degree, formation pathway, and mass spectra features of typical urban-lifestyle secondary organic aerosols (SOAs) including vehicle SOAs and cooking SOAs. The mass spectra we acquired could provide necessary references to estimate the mass fractions of vehicle and cooking SOAs in the atmosphere, which would greatly decrease the uncertainty in air quality evaluation and health risk assessment in urban areas.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
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The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Adam Milsom, Adam M. Squires, Jacob A. Boswell, Nicholas J. Terrill, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 21, 15003–15021, https://doi.org/10.5194/acp-21-15003-2021, https://doi.org/10.5194/acp-21-15003-2021, 2021
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Atmospheric aerosols can be solid, semi-solid or liquid. This phase state may impact key aerosol processes such as oxidation and water uptake, affecting cloud droplet formation and urban air pollution. We have observed a solid crystalline organic phase in a levitated proxy for cooking emissions, oleic acid. Spatially resolved structural changes were followed during ageing by X-ray scattering, revealing phase gradients, aggregate products and a markedly reduced ozonolysis reaction rate.
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Short summary
We investigated the change in cloud droplet activity of size-selected soot particles after being exposed to atmospheric levels of ozone over the course of 12 h. For this, we operated a 3 m3 aerosol chamber in continuous-flow mode. The results were fed into a climate model (ECHAM-HAM). We found that the oxidation of soot particles with ozone is a significant source of cloud condensation nuclei in the atmosphere.
We investigated the change in cloud droplet activity of size-selected soot particles after being...
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