Articles | Volume 21, issue 20
https://doi.org/10.5194/acp-21-15725-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-15725-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Technical note
| 
21 Oct 2021
Technical note |
| 21 Oct 2021
| 21 Oct 2021
Technical note: Adsorption and desorption equilibria from statistical thermodynamics and rates from transition state theory
Daniel A. Knopf
CORRESPONDING AUTHOR
School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, New York, USA
Laboratory of Environmental Chemistry, Paul Scherrer Institute, Villigen, Switzerland
Related authors
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, and Ulla Wandinger
EGUsphere, https://doi.org/10.5194/egusphere-2024-2008, https://doi.org/10.5194/egusphere-2024-2008, 2024
Short summary
Short summary
In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. We found a clear impact of wildfire smoke on cirrus evolution.
Albert Ansmann, Cristofer Jimenez, Daniel A. Knopf, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, and Ronny Engelmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2009, https://doi.org/10.5194/egusphere-2024-2009, 2024
Short summary
Short summary
In this study, we focus on the potential impact of wildfire smoke on cirrus formation. Aerosol and cirrus observations with lidar and radar during the MOSAiC expedition, presented in part 1 (egusphere-2024-2008) are closely linked to comprehensive modeling of ice nucleation in cirrus evolution processes, presented in this part 2 (egusphere-2024-2009). A clear impact of wildfire smoke on cirrus formation was found.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
Short summary
Short summary
The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Rodanthi-Elisavet Mamouri, Albert Ansmann, Kevin Ohneiser, Daniel A. Knopf, Argyro Nisantzi, Johannes Bühl, Ronny Engelmann, Annett Skupin, Patric Seifert, Holger Baars, Dragos Ene, Ulla Wandinger, and Diofantos Hadjimitsis
Atmos. Chem. Phys., 23, 14097–14114, https://doi.org/10.5194/acp-23-14097-2023, https://doi.org/10.5194/acp-23-14097-2023, 2023
Short summary
Short summary
For the first time, rather clear evidence is found that wildfire smoke particles can trigger strong cirrus formation. This finding is of importance because intensive and large wildfires may occur increasingly often in the future as climate change proceeds. Based on lidar observations in Cyprus in autumn 2020, we provide detailed insight into the cirrus formation at the tropopause in the presence of aged wildfire smoke (here, 8–9 day old Californian wildfire smoke).
Albert Ansmann, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Jessie M. Creamean, Matthew C. Boyer, Daniel A. Knopf, Sandro Dahlke, Marion Maturilli, Henriette Gebauer, Johannes Bühl, Cristofer Jimenez, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 23, 12821–12849, https://doi.org/10.5194/acp-23-12821-2023, https://doi.org/10.5194/acp-23-12821-2023, 2023
Short summary
Short summary
The 1-year MOSAiC (2019–2020) expedition with the German ice breaker Polarstern was the largest polar field campaign ever conducted. The Polarstern, with our lidar aboard, drifted with the pack ice north of 85° N for more than 7 months (October 2019 to mid-May 2020). We measured the full annual cycle of aerosol conditions in terms of aerosol optical and cloud-process-relevant properties. We observed a strong contrast between polluted winter and clean summer aerosol conditions.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
Short summary
Short summary
Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Albert Ansmann, Kevin Ohneiser, Alexandra Chudnovsky, Daniel A. Knopf, Edwin W. Eloranta, Diego Villanueva, Patric Seifert, Martin Radenz, Boris Barja, Félix Zamorano, Cristofer Jimenez, Ronny Engelmann, Holger Baars, Hannes Griesche, Julian Hofer, Dietrich Althausen, and Ulla Wandinger
Atmos. Chem. Phys., 22, 11701–11726, https://doi.org/10.5194/acp-22-11701-2022, https://doi.org/10.5194/acp-22-11701-2022, 2022
Short summary
Short summary
For the first time we present a systematic study on the impact of wildfire smoke on ozone depletion in the Arctic (2020) and Antarctic stratosphere (2020, 2021). Two major fire events in Siberia and Australia were responsible for the observed record-breaking stratospheric smoke pollution. Our analyses were based on lidar observations of smoke parameters (Polarstern, Punta Arenas) and NDACC Arctic and Antarctic ozone profiles as well as on Antarctic OMI satellite observations of column ozone.
Kevin Ohneiser, Albert Ansmann, Bernd Kaifler, Alexandra Chudnovsky, Boris Barja, Daniel A. Knopf, Natalie Kaifler, Holger Baars, Patric Seifert, Diego Villanueva, Cristofer Jimenez, Martin Radenz, Ronny Engelmann, Igor Veselovskii, and Félix Zamorano
Atmos. Chem. Phys., 22, 7417–7442, https://doi.org/10.5194/acp-22-7417-2022, https://doi.org/10.5194/acp-22-7417-2022, 2022
Short summary
Short summary
We present and discuss 2 years of long-term lidar observations of the largest stratospheric perturbation by wildfire smoke ever observed. The smoke originated from the record-breaking Australian fires in 2019–2020 and affects climate conditions and even the ozone layer in the Southern Hemisphere. The obvious link between dense smoke occurrence in the stratosphere and strong ozone depletion found in the Arctic and in the Antarctic in 2020 can be regarded as a new aspect of climate change.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
Short summary
Short summary
Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
Short summary
Short summary
Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
Short summary
Short summary
This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Albert Ansmann, Kevin Ohneiser, Rodanthi-Elisavet Mamouri, Daniel A. Knopf, Igor Veselovskii, Holger Baars, Ronny Engelmann, Andreas Foth, Cristofer Jimenez, Patric Seifert, and Boris Barja
Atmos. Chem. Phys., 21, 9779–9807, https://doi.org/10.5194/acp-21-9779-2021, https://doi.org/10.5194/acp-21-9779-2021, 2021
Short summary
Short summary
We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area concentration of wildfire smoke layers, and related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations. The new analysis scheme is applied to ground-based lidar observations of stratospheric Australian smoke over southern South America and to spaceborne lidar observations of tropospheric North American smoke.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
Short summary
Short summary
We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Israel Silber, Ann M. Fridlind, Johannes Verlinde, Andrew S. Ackerman, Grégory V. Cesana, and Daniel A. Knopf
Atmos. Chem. Phys., 21, 3949–3971, https://doi.org/10.5194/acp-21-3949-2021, https://doi.org/10.5194/acp-21-3949-2021, 2021
Short summary
Short summary
Long-term ground-based radar and sounding measurements over Alaska (Antarctica) indicate that more than 85 % (75 %) of supercooled clouds are precipitating at cloud base and that 75 % (50 %) are precipitating to the surface. Such high prevalence is reconciled with lesser spaceborne estimates by considering radar sensitivity. Results provide a strong observational constraint for polar cloud processes in large-scale models.
Jienan Li, Seanna M. Forrester, and Daniel A. Knopf
Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, https://doi.org/10.5194/acp-20-6055-2020, 2020
Short summary
Short summary
Organic aerosol is ubiquitous in the atmosphere and can change its phase state from liquid to solid in response to temperature. Our laboratory measurements demonstrate that the chemical reactivity of typical organic aerosol species with atmospheric oxidants is modulated by the species’ phase state. We find that under temperatures typical of the middle and upper troposphere the chemical lifetime of organic aerosol can be significantly extended due to the reduced reactive uptake of gas oxidants.
Ryan C. Moffet, Rachel E. O'Brien, Peter A. Alpert, Stephen T. Kelly, Don Q. Pham, Mary K. Gilles, Daniel A. Knopf, and Alexander Laskin
Atmos. Chem. Phys., 16, 14515–14525, https://doi.org/10.5194/acp-16-14515-2016, https://doi.org/10.5194/acp-16-14515-2016, 2016
Short summary
Short summary
Atmospheric black carbon (BC), commonly known as soot, is an important constituent of the earth that imparts a warming similar to that of carbon dioxide. However, BC is much shorter lived and has uncertain warming due to its mixture with other solid and liquid components. Here, advanced microscopic methods have provided a detailed look at thousands of BC particles sampled from central California; these measurements will lead towards a better understanding of the effects that BC has on climate.
Peter A. Alpert and Daniel A. Knopf
Atmos. Chem. Phys., 16, 2083–2107, https://doi.org/10.5194/acp-16-2083-2016, https://doi.org/10.5194/acp-16-2083-2016, 2016
Short summary
Short summary
A stochastic immersion freezing model is introduced capable of reproducing laboratory data for a variety of experimental methods using a time and surface area dependent ice nucleation process. The assumption that droplets contain identical surface area is evaluated. A quantitative uncertainty analysis of the laboratory observed freezing process is presented. Our results imply that ice nuclei surface area assumptions are crucial for interpretation of experimental immersion freezing results.
J. H. Slade, R. Thalman, J. Wang, and D. A. Knopf
Atmos. Chem. Phys., 15, 10183–10201, https://doi.org/10.5194/acp-15-10183-2015, https://doi.org/10.5194/acp-15-10183-2015, 2015
Short summary
Short summary
Aerosol particles undergo chemical modification during atmospheric transport due to reactions with trace gas species such as OH radicals affecting cloud formation and, thus, prediction of climate. Here, the cloud formation potential of surrogate biomass burning aerosol (BBA) is studied as a function of particle composition and OH exposure. We find that OH oxidation can alter the cloud formation potential of BBA, but its significance depends on the available water-soluble particulate material.
Y. J. Rigg, P. A. Alpert, and D. A. Knopf
Atmos. Chem. Phys., 13, 6603–6622, https://doi.org/10.5194/acp-13-6603-2013, https://doi.org/10.5194/acp-13-6603-2013, 2013
S. M. Forrester and D. A. Knopf
Atmos. Chem. Phys., 13, 6507–6522, https://doi.org/10.5194/acp-13-6507-2013, https://doi.org/10.5194/acp-13-6507-2013, 2013
Kevin Kilchhofer, Alexandre Barth, Battist Utinger, Markus Kalberer, and Markus Ammann
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-36, https://doi.org/10.5194/ar-2024-36, 2024
Preprint under review for AR
Short summary
Short summary
We report a substantial build-up of reactive molecules by sunlight in organic particulate matter causing adverse health effects. Metals naturally or by traffic emitted can complex with organic materials and initiate photochemical processes. At low humidity organic particles may become highly viscous, which lets the accumulate reactive species. We found that copper acts as an reducing species to remove some of the harmful species in the particles.
Kevin Kilchhofer, Markus Ammann, Laura Torrent, Ka Yuen Cheung, and Peter Aaron Alpert
EGUsphere, https://doi.org/10.5194/egusphere-2024-3226, https://doi.org/10.5194/egusphere-2024-3226, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Aerosol particles composed of metal complexes generate radicals as the result of photochemical reactions. Reactive species generated are hazardous to human health. We report microscopy data with particles composed of an organic proxy exposed to UV light. We found that copper influenced the reoxidation and initial iron reduction via photolysis of the complex. New model results suggest that we need to account a decreased photochemical activity and use a copper-induced reoxidation reaction.
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, and Ulla Wandinger
EGUsphere, https://doi.org/10.5194/egusphere-2024-2008, https://doi.org/10.5194/egusphere-2024-2008, 2024
Short summary
Short summary
In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. We found a clear impact of wildfire smoke on cirrus evolution.
Albert Ansmann, Cristofer Jimenez, Daniel A. Knopf, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, and Ronny Engelmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2009, https://doi.org/10.5194/egusphere-2024-2009, 2024
Short summary
Short summary
In this study, we focus on the potential impact of wildfire smoke on cirrus formation. Aerosol and cirrus observations with lidar and radar during the MOSAiC expedition, presented in part 1 (egusphere-2024-2008) are closely linked to comprehensive modeling of ice nucleation in cirrus evolution processes, presented in this part 2 (egusphere-2024-2009). A clear impact of wildfire smoke on cirrus formation was found.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
Short summary
Short summary
The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Rodanthi-Elisavet Mamouri, Albert Ansmann, Kevin Ohneiser, Daniel A. Knopf, Argyro Nisantzi, Johannes Bühl, Ronny Engelmann, Annett Skupin, Patric Seifert, Holger Baars, Dragos Ene, Ulla Wandinger, and Diofantos Hadjimitsis
Atmos. Chem. Phys., 23, 14097–14114, https://doi.org/10.5194/acp-23-14097-2023, https://doi.org/10.5194/acp-23-14097-2023, 2023
Short summary
Short summary
For the first time, rather clear evidence is found that wildfire smoke particles can trigger strong cirrus formation. This finding is of importance because intensive and large wildfires may occur increasingly often in the future as climate change proceeds. Based on lidar observations in Cyprus in autumn 2020, we provide detailed insight into the cirrus formation at the tropopause in the presence of aged wildfire smoke (here, 8–9 day old Californian wildfire smoke).
Albert Ansmann, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Jessie M. Creamean, Matthew C. Boyer, Daniel A. Knopf, Sandro Dahlke, Marion Maturilli, Henriette Gebauer, Johannes Bühl, Cristofer Jimenez, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 23, 12821–12849, https://doi.org/10.5194/acp-23-12821-2023, https://doi.org/10.5194/acp-23-12821-2023, 2023
Short summary
Short summary
The 1-year MOSAiC (2019–2020) expedition with the German ice breaker Polarstern was the largest polar field campaign ever conducted. The Polarstern, with our lidar aboard, drifted with the pack ice north of 85° N for more than 7 months (October 2019 to mid-May 2020). We measured the full annual cycle of aerosol conditions in terms of aerosol optical and cloud-process-relevant properties. We observed a strong contrast between polluted winter and clean summer aerosol conditions.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
Short summary
Short summary
Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
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
Short summary
Short summary
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.
Albert Ansmann, Kevin Ohneiser, Alexandra Chudnovsky, Daniel A. Knopf, Edwin W. Eloranta, Diego Villanueva, Patric Seifert, Martin Radenz, Boris Barja, Félix Zamorano, Cristofer Jimenez, Ronny Engelmann, Holger Baars, Hannes Griesche, Julian Hofer, Dietrich Althausen, and Ulla Wandinger
Atmos. Chem. Phys., 22, 11701–11726, https://doi.org/10.5194/acp-22-11701-2022, https://doi.org/10.5194/acp-22-11701-2022, 2022
Short summary
Short summary
For the first time we present a systematic study on the impact of wildfire smoke on ozone depletion in the Arctic (2020) and Antarctic stratosphere (2020, 2021). Two major fire events in Siberia and Australia were responsible for the observed record-breaking stratospheric smoke pollution. Our analyses were based on lidar observations of smoke parameters (Polarstern, Punta Arenas) and NDACC Arctic and Antarctic ozone profiles as well as on Antarctic OMI satellite observations of column ozone.
Kevin Ohneiser, Albert Ansmann, Bernd Kaifler, Alexandra Chudnovsky, Boris Barja, Daniel A. Knopf, Natalie Kaifler, Holger Baars, Patric Seifert, Diego Villanueva, Cristofer Jimenez, Martin Radenz, Ronny Engelmann, Igor Veselovskii, and Félix Zamorano
Atmos. Chem. Phys., 22, 7417–7442, https://doi.org/10.5194/acp-22-7417-2022, https://doi.org/10.5194/acp-22-7417-2022, 2022
Short summary
Short summary
We present and discuss 2 years of long-term lidar observations of the largest stratospheric perturbation by wildfire smoke ever observed. The smoke originated from the record-breaking Australian fires in 2019–2020 and affects climate conditions and even the ozone layer in the Southern Hemisphere. The obvious link between dense smoke occurrence in the stratosphere and strong ozone depletion found in the Arctic and in the Antarctic in 2020 can be regarded as a new aspect of climate change.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
Short summary
Short summary
Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
Short summary
Short summary
Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
Short summary
Short summary
The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
Short summary
Short summary
This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Albert Ansmann, Kevin Ohneiser, Rodanthi-Elisavet Mamouri, Daniel A. Knopf, Igor Veselovskii, Holger Baars, Ronny Engelmann, Andreas Foth, Cristofer Jimenez, Patric Seifert, and Boris Barja
Atmos. Chem. Phys., 21, 9779–9807, https://doi.org/10.5194/acp-21-9779-2021, https://doi.org/10.5194/acp-21-9779-2021, 2021
Short summary
Short summary
We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area concentration of wildfire smoke layers, and related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations. The new analysis scheme is applied to ground-based lidar observations of stratospheric Australian smoke over southern South America and to spaceborne lidar observations of tropospheric North American smoke.
Thorsten Bartels-Rausch, Xiangrui Kong, Fabrizio Orlando, Luca Artiglia, Astrid Waldner, Thomas Huthwelker, and Markus Ammann
The Cryosphere, 15, 2001–2020, https://doi.org/10.5194/tc-15-2001-2021, https://doi.org/10.5194/tc-15-2001-2021, 2021
Short summary
Short summary
Chemical reactions in sea salt embedded in coastal polar snow impact the composition and air quality of the atmosphere. Here, we investigate the phase changes of sodium chloride. This is of importance as chemical reactions proceed faster in liquid solutions compared to in solid salt and the precise precipitation temperature of sodium chloride is still under debate. We focus on the upper nanometres of sodium chloride–ice samples because of their role as a reactive interface in the environment.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
Short summary
Short summary
We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
Short summary
Short summary
Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
Israel Silber, Ann M. Fridlind, Johannes Verlinde, Andrew S. Ackerman, Grégory V. Cesana, and Daniel A. Knopf
Atmos. Chem. Phys., 21, 3949–3971, https://doi.org/10.5194/acp-21-3949-2021, https://doi.org/10.5194/acp-21-3949-2021, 2021
Short summary
Short summary
Long-term ground-based radar and sounding measurements over Alaska (Antarctica) indicate that more than 85 % (75 %) of supercooled clouds are precipitating at cloud base and that 75 % (50 %) are precipitating to the surface. Such high prevalence is reconciled with lesser spaceborne estimates by considering radar sensitivity. Results provide a strong observational constraint for polar cloud processes in large-scale models.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
Short summary
Short summary
Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Jacinta Edebeli, Jürg C. Trachsel, Sven E. Avak, Markus Ammann, Martin Schneebeli, Anja Eichler, and Thorsten Bartels-Rausch
Atmos. Chem. Phys., 20, 13443–13454, https://doi.org/10.5194/acp-20-13443-2020, https://doi.org/10.5194/acp-20-13443-2020, 2020
Short summary
Short summary
Earth’s snow cover is very dynamic and can change its physical properties within hours, as is well known by skiers. Snow is also a well-known host of chemical reactions – the products of which impact air composition and quality. Here, we present laboratory experiments that show how the dynamics of snow make snow essentially inert with respect to gas-phase ozone with time despite its content of reactive chemicals. Impacts on polar atmospheric chemistry are discussed.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, https://doi.org/10.5194/acp-20-13497-2020, 2020
Short summary
Short summary
Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Jan-David Förster, Christian Gurk, Mark Lamneck, Haijie Tong, Florian Ditas, Sarah S. Steimer, Peter A. Alpert, Markus Ammann, Jörg Raabe, Markus Weigand, Benjamin Watts, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Meas. Tech., 13, 3717–3729, https://doi.org/10.5194/amt-13-3717-2020, https://doi.org/10.5194/amt-13-3717-2020, 2020
Short summary
Short summary
A gas flow system coupled with a microreactor for X-ray microspectroscopy is presented. Its core objective is to mimic the atmospheric processing of aerosol particles under laboratory conditions in a controlled gas-phase environment and allow in situ observations with high spatial and chemical resolution. We here emphasize its analytical capabilities and show initial results from hydration–dehydration experiments and the observation of water ice at low temperature and high relative humidity.
Jienan Li, Seanna M. Forrester, and Daniel A. Knopf
Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, https://doi.org/10.5194/acp-20-6055-2020, 2020
Short summary
Short summary
Organic aerosol is ubiquitous in the atmosphere and can change its phase state from liquid to solid in response to temperature. Our laboratory measurements demonstrate that the chemical reactivity of typical organic aerosol species with atmospheric oxidants is modulated by the species’ phase state. We find that under temperatures typical of the middle and upper troposphere the chemical lifetime of organic aerosol can be significantly extended due to the reduced reactive uptake of gas oxidants.
Pablo Corral Arroyo, Raffael Aellig, Peter A. Alpert, Rainer Volkamer, and Markus Ammann
Atmos. Chem. Phys., 19, 10817–10828, https://doi.org/10.5194/acp-19-10817-2019, https://doi.org/10.5194/acp-19-10817-2019, 2019
Short summary
Short summary
Oxidation of bromide and iodide is an important process in the troposphere that leads to gas-phase halogen compounds which impact the oxidation capacity of the atmosphere. Imidazole-2-carboxaldehyde (IC), an aromatic carbonyl, is a product of the multiphase chemistry of glyoxal (an oxidation product of isoprene), a major biogenic volatile organic compound. In this study we demonstrate that IC photochemistry leads to efficient oxidation of bromide and iodide and liberation of halogen compounds.
Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232, https://doi.org/10.5194/acp-19-2209-2019, https://doi.org/10.5194/acp-19-2209-2019, 2019
Short summary
Short summary
VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Guo Li, Hang Su, Uwe Kuhn, Hannah Meusel, Markus Ammann, Min Shao, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 18, 2669–2686, https://doi.org/10.5194/acp-18-2669-2018, https://doi.org/10.5194/acp-18-2669-2018, 2018
Short summary
Short summary
Coated-wall flow tube reactors are frequently used to investigate gas uptake and heterogeneous or multiphase reaction kinetics under laminar flow conditions. In previous applications, the effects of coating surface roughness on flow conditions were not well quantified. In this study, a criterion is proposed to eliminate/minimize the potential effects of coating surface roughness on laminar flow in coated-wall flow tube experiments and validate the applications of diffusion correction methods.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
Short summary
Short summary
In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
Short summary
Short summary
Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Goran Gržinić, Thorsten Bartels-Rausch, Andreas Türler, and Markus Ammann
Atmos. Chem. Phys., 17, 6493–6502, https://doi.org/10.5194/acp-17-6493-2017, https://doi.org/10.5194/acp-17-6493-2017, 2017
Short summary
Short summary
Nitrogen oxides (NOx) largely control the ozone budget in the troposphere globally. Dinitrogen pentoxide (N2O5) is an important species as a nighttime reservoir for nitrogen oxides. Loss of N2O5 to aerosol particles is therefore important for the budget of NOx and the oxidation capacity. Here we provide direct evidence for its efficient accommodation into aqueous aerosol particles and its fast dissociation, which has not been elucidated as directly in previous studies.
Ryan C. Moffet, Rachel E. O'Brien, Peter A. Alpert, Stephen T. Kelly, Don Q. Pham, Mary K. Gilles, Daniel A. Knopf, and Alexander Laskin
Atmos. Chem. Phys., 16, 14515–14525, https://doi.org/10.5194/acp-16-14515-2016, https://doi.org/10.5194/acp-16-14515-2016, 2016
Short summary
Short summary
Atmospheric black carbon (BC), commonly known as soot, is an important constituent of the earth that imparts a warming similar to that of carbon dioxide. However, BC is much shorter lived and has uncertain warming due to its mixture with other solid and liquid components. Here, advanced microscopic methods have provided a detailed look at thousands of BC particles sampled from central California; these measurements will lead towards a better understanding of the effects that BC has on climate.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
Short summary
Short summary
Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Laura González Palacios, Pablo Corral Arroyo, Kifle Z. Aregahegn, Sarah S. Steimer, Thorsten Bartels-Rausch, Barbara Nozière, Christian George, Markus Ammann, and Rainer Volkamer
Atmos. Chem. Phys., 16, 11823–11836, https://doi.org/10.5194/acp-16-11823-2016, https://doi.org/10.5194/acp-16-11823-2016, 2016
Short summary
Short summary
The sources of radicals at aerosol surfaces are highly uncertain. Here we investigate the HO2 radical production from the UV irradiation of imidazole-2-carboxaldehyde (IC) in bulk aqueous films containing IC and citric acid, as well as IC in ammonium sulfate aerosols. We find that IC is an efficient photosensitizer that forms HO2 radicals from H-donor chemistry. IC is a proxy species for brown carbon in atmospheric aerosols.
Guo Li, Hang Su, Xin Li, Uwe Kuhn, Hannah Meusel, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Yafang Cheng
Atmos. Chem. Phys., 16, 10299–10311, https://doi.org/10.5194/acp-16-10299-2016, https://doi.org/10.5194/acp-16-10299-2016, 2016
Short summary
Short summary
Indoor and outdoor formaldehyde (HCHO) are both of considerable concern because of its health effects and its role in atmospheric chemistry. The heterogeneous reactions between gaseous HCHO with soils can pose important impact on both HCHO budget and soil ecosystem. Our results confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions. Soil and soil-derived airborne particles can either act as a source or a sink for HCHO.
Peter A. Alpert and Daniel A. Knopf
Atmos. Chem. Phys., 16, 2083–2107, https://doi.org/10.5194/acp-16-2083-2016, https://doi.org/10.5194/acp-16-2083-2016, 2016
Short summary
Short summary
A stochastic immersion freezing model is introduced capable of reproducing laboratory data for a variety of experimental methods using a time and surface area dependent ice nucleation process. The assumption that droplets contain identical surface area is evaluated. A quantitative uncertainty analysis of the laboratory observed freezing process is presented. Our results imply that ice nuclei surface area assumptions are crucial for interpretation of experimental immersion freezing results.
G. Gržinić, T. Bartels-Rausch, T. Berkemeier, A. Türler, and M. Ammann
Atmos. Chem. Phys., 15, 13615–13625, https://doi.org/10.5194/acp-15-13615-2015, https://doi.org/10.5194/acp-15-13615-2015, 2015
Short summary
Short summary
The heterogeneous loss of dinitrogen pentoxide (N2O5) to citric acid aerosol, a proxy for highly oxygenated secondary organic aerosol, is shown to be substantially lower than to other aqueous organic aerosol proxies investigated previously. This is attributed to the widely changing viscosity within the atmospherically relevant humidity range. It may explain some of the unexpectedly low loss rates of N2O5 to aerosol particles derived from field studies.
J. H. Slade, R. Thalman, J. Wang, and D. A. Knopf
Atmos. Chem. Phys., 15, 10183–10201, https://doi.org/10.5194/acp-15-10183-2015, https://doi.org/10.5194/acp-15-10183-2015, 2015
Short summary
Short summary
Aerosol particles undergo chemical modification during atmospheric transport due to reactions with trace gas species such as OH radicals affecting cloud formation and, thus, prediction of climate. Here, the cloud formation potential of surrogate biomass burning aerosol (BBA) is studied as a function of particle composition and OH exposure. We find that OH oxidation can alter the cloud formation potential of BBA, but its significance depends on the available water-soluble particulate material.
S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, https://doi.org/10.5194/amt-8-2397-2015, 2015
Short summary
Short summary
Atmospheric aerosol is often subject to supersaturated or supercooled conditions where bulk measurements are not possible. Here we demonstrate how measurements using single particle electrodynamic levitation combined with light scattering spectroscopy allow the retrieval of thermodynamic data, optical properties and water diffusivity of such metastable particles even when auxiliary bulk data are not available due to lack of sufficient amounts of sample.
S. S. Steimer, M. Lampimäki, E. Coz, G. Grzinic, and M. Ammann
Atmos. Chem. Phys., 14, 10761–10772, https://doi.org/10.5194/acp-14-10761-2014, https://doi.org/10.5194/acp-14-10761-2014, 2014
M. Ammann, R. A. Cox, J. N. Crowley, M. E. Jenkin, A. Mellouki, M. J. Rossi, J. Troe, and T. J. Wallington
Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, https://doi.org/10.5194/acp-13-8045-2013, 2013
T. Bartels-Rausch, S. N. Wren, S. Schreiber, F. Riche, M. Schneebeli, and M. Ammann
Atmos. Chem. Phys., 13, 6727–6739, https://doi.org/10.5194/acp-13-6727-2013, https://doi.org/10.5194/acp-13-6727-2013, 2013
T. Berkemeier, A. J. Huisman, M. Ammann, M. Shiraiwa, T. Koop, and U. Pöschl
Atmos. Chem. Phys., 13, 6663–6686, https://doi.org/10.5194/acp-13-6663-2013, https://doi.org/10.5194/acp-13-6663-2013, 2013
Y. J. Rigg, P. A. Alpert, and D. A. Knopf
Atmos. Chem. Phys., 13, 6603–6622, https://doi.org/10.5194/acp-13-6603-2013, https://doi.org/10.5194/acp-13-6603-2013, 2013
S. M. Forrester and D. A. Knopf
Atmos. Chem. Phys., 13, 6507–6522, https://doi.org/10.5194/acp-13-6507-2013, https://doi.org/10.5194/acp-13-6507-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photooxidation: Remarkably enhancing effects of seeds and ammonia
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement Report: Changes of ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice core record
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
Short summary
Short summary
We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
Short summary
Short summary
We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
Short summary
Short summary
Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
Short summary
Short summary
Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
Short summary
Short summary
Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
Short summary
Short summary
Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
Short summary
Short summary
This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
Short summary
Short summary
In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Si Zhang, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2119, https://doi.org/10.5194/egusphere-2024-2119, 2024
Short summary
Short summary
SOA from acetone photooxidation can be formed more readily on neutral aerosols than on acidic aerosols, while heterogeneous reaction of carbonyl with ammonium is only active on acidic aerosols in the presence of NH3, which produces light-absorbing N-containing compounds. Our work suggested that the heterogeneous oxidation of highly volatile VOC, for example acetone, is an importance source of SOA in the atmosphere, which should be accounted for in the future model studies.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
Short summary
Short summary
Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
EGUsphere, https://doi.org/10.5194/egusphere-2024-1381, https://doi.org/10.5194/egusphere-2024-1381, 2024
Short summary
Short summary
A record of ammonium covering the years 1750 to 2008 was extracted from a 182-meter-long ice core drilled in 2009 at Mt. Elbrus in the Caucasus, Russia. Changes in ammonia emissions in southeastern Europe during the pre-industrial and industrial periods were investigated. The level of ammonium in 1750 indicates a significant contribution of natural sources to the ammonia budget, contrasting with present-day conditions, where agricultural emissions outweigh those from biogenic sources in Europe.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
Short summary
Short summary
The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
EGUsphere, https://doi.org/10.5194/egusphere-2024-1880, https://doi.org/10.5194/egusphere-2024-1880, 2024
Short summary
Short summary
The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolite and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
Short summary
Short summary
The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
Short summary
Short summary
We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
Short summary
Short summary
Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
Short summary
Short summary
Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
Short summary
Short summary
We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
Short summary
Short summary
We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
Short summary
Short summary
Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
Short summary
Short summary
The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
Short summary
Short summary
We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
Short summary
Short summary
Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
Short summary
Short summary
Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
Short summary
Short summary
PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
Short summary
Short summary
The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
Short summary
Short summary
In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
Short summary
Short summary
This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
Short summary
Short summary
We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
Short summary
Short summary
We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
Short summary
Short summary
The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
Short summary
Short summary
Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
Short summary
Short summary
Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
Short summary
Short summary
We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
Short summary
Short summary
D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
Short summary
Short summary
Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
Short summary
Short summary
Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
Short summary
Short summary
A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
Short summary
Short summary
Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
Short summary
Short summary
In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
Short summary
Short summary
Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
Short summary
Short summary
With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
Short summary
Short summary
In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
Short summary
Short summary
Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
Short summary
Short summary
Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
Short summary
Short summary
Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
Short summary
Short summary
Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
Short summary
Short summary
Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
Short summary
Short summary
Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
Short summary
Short summary
The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
Cited articles
Ammann, M. and Pöschl, U.: Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 2: Exemplary practical applications and numerical simulations, Atmos. Chem. Phys., 7, 6025–6045, https://doi.org/10.5194/acp-7-6025-2007, 2007.
Ammann, M., Cox, R. A., Crowley, J. N., Jenkin, M. E., Mellouki, A., Rossi, M. J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VI – heterogeneous reactions with liquid substrates, Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, 2013.
Arangio, A. M., Slade, J. H., Berkemeier, T., Pöschl, U., Knopf, D. A., and Shiraiwa, M.: Multiphase Chemical Kinetics of OH Radical Uptake by Molecular Organic Markers of Biomass Burning Aerosols: Humidity and Temperature Dependence, Surface Reaction, and Bulk Diffusion, J. Phys. Chem. A, 119, 4533–4544, https://doi.org/10.1021/jp510489z, 2015.
Arrhenius, S. A.: Über die Dissociationswärme und den Einfluss der Temperatur auf den Dissociationsgrad der Elektrolyte, Z. Phys. Chem., 4, 96–116, 1889a.
Arrhenius, S. A.: Über die Reaktionsgeschwindigkeit bei der Inversion von Rohrzucker durch Säuren, Z. Phys. Chem., 4, 226–248, 1889b.
Atkins, P. and de Paula, J.: Physical Chemistry, 8th edn., W. H. Freeman and Company, New York, 1040 pp., 2006.
Bartels-Rausch, T., Huthwelker, T., Gäggeler, H. W., and Ammann, M.: Atmospheric pressure coated-wall flow-tube study of acetone adsorption on ice, J. Phys. Chem. A, 109, 4531–4539, https://doi.org/10.1021/jp045187l, 2005.
Bolis, V.: Fundamentals in Adsorption at the Solid-Gas
Interface. Concepts and Thermodynamics, in: Calorimetry and Thermal
Methods in Catalysis, vol. 154, edited by: Auroux, A., Springer-Verlag, Berlin, Heidelberg, 3–50, 2013.
Campbell, C. T., Arnadottir, L., and Sellers, J. R. V.: Kinetic Prefactors of Reactions on Solid Surfaces, Z. Phys. Chem., 227, 1435–1454, https://doi.org/10.1524/zpch.2013.0395, 2013.
Campbell, C. T., Sprowl, L. H., and Arnadottir, L.: Equilibrium Constants and Rate Constants for Adsorbates: Two-Dimensional (2D) Ideal Gas, 2D Ideal Lattice Gas, and Ideal Hindered Translator Models, J. Phys. Chem. C, 120, 10283–10297, https://doi.org/10.1021/acs.jpcc.6b00975, 2016.
Chorkendorff, I. and Niemantsverdriet, J. W.: Concepts of Modern Catalysis and Kinetics, 2nd edn., Wiley-VCH, Weinheim, 477 pp., 2007.
Crowley, J. N., Ammann, M., Cox, R. A., Hynes, R. G., Jenkin, M. E., Mellouki, A., Rossi, M. J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume V – heterogeneous reactions on solid substrates, Atmos. Chem. Phys., 10, 9059–9223, https://doi.org/10.5194/acp-10-9059-2010, 2010.
Crowley, J. N., Ammann, M., Cox, R. A., Hynes, R. G., Jenkin, M. E., Mellouki, A., Rossi, M. J., Troe, J., and Wallington, T. J.: Corrigendum to “Evaluated kinetic and photochemical data for atmospheric chemistry: Volume V – heterogeneous reactions on solid substrates” published in Atmos. Chem. Phys. 10, 9059–9223, 2010, Atmos. Chem. Phys., 13, 7359–7359, https://doi.org/10.5194/acp-13-7359-2013, 2013.
Cussler, E. L.: Diffusion – Mass Transfer in Fluid Systems, Cambridge University Press, New York,
631 pp., 2009.
de Boer, J. H.: The Dynamical Character of Adsorption, Clarendon Press, Oxford, 240 pp., 1968.
Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, https://doi.org/10.5194/acp-11-3303-2011, 2011.
Donaldson, D. J., Ammann, M., Bartels-Rausch, T., and Pöschl, U.: Standard States and Thermochemical Kinetics in Heterogeneous Atmospheric Chemistry, J. Phys. Chem. A, 116, 6312–6316, https://doi.org/10.1021/jp212015g, 2012.
Eyring, H.: The activated complex in chemical reactions, J. Chem. Phys., 3, 107–115, https://doi.org/10.1063/1.1749604, 1935.
Finlayson-Pitts, B. J. and Pitts, J. N.: Chemistry of the Upper and Lower Atmosphere: Theory, Experiments and Applications, Academic Press, San Diego, CA, London, xxii, 969 pp., 2000.
Frenkel, J.: Theory of the adsorption and related occurrences, Z. Phys., 26, 117–138, https://doi.org/10.1007/bf01327320, 1924.
George, I. J. and Abbatt, J. P. D.: Heterogeneous oxidation of atmospheric aerosol particles by gas-phase radicals, Nat. Chem., 2, 713–722, https://doi.org/10.1038/Nchem.806, 2010.
Hanson, D. R. and Ravishankara, A. R.: The Loss of CF2O On Ice, NAT, and Sulfuric-Acid-Solutions, Geophys. Res. Lett., 18, 1699–1701, 1991.
Hill, T. L.: An Introduction to Statistical Thermodynamics, Dover Publications, New York, 501 pp., 1986.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Kemball, C. and Rideal, E. K.: The adsorption of vapours
on mercury. 1. Non-polar substances, P. Roy. Soc. Lond. A Mat., 187, 53–73, https://doi.org/10.1098/rspa.1946.0065, 1946.
Kisliuk, P.: The sticking probabilities of gases chemisorbed on the surfaces of solids, J. Phys. Chem. Solids, 3, 95–101, https://doi.org/10.1016/0022-3697(57)90054-9, 1957.
Kolasinski, K. W.: Surface Science: Foundations of Catalysis and Nanoscience, 3rd edn., John Wiley & Sons, Ltd., West Sussex, United Kingdom, 556 pp., 2012.
Kolb, C. E., Worsnop, D. R., Zahniser, M. S., Davidovits, P., Keyser, L. F., Leu, M.-T., Molina, M. J., Hanson, D. R., Ravishankara, A. R., Williams, L. R., and Tolbert, M. A.: Laboratory Studies of Atmospheric Heterogeneous Chemistry, in: Progress and Problems in Atmospheric Chemistry, edited by: Barker, J. R., World Scientific, Singapore, 771–875, 1995.
Kolb, C. E., Cox, R. A., Abbatt, J. P. D., Ammann, M., Davis, E. J., Donaldson, D. J., Garrett, B. C., George, C., Griffiths, P. T., Hanson, D. R., Kulmala, M., McFiggans, G., Pöschl, U., Riipinen, I., Rossi, M. J., Rudich, Y., Wagner, P. E., Winkler, P. M., Worsnop, D. R., and O'Dowd, C. D.: An overview of current issues in the uptake of atmospheric trace gases by aerosols and clouds, Atmos. Chem. Phys., 10, 10561–10605, 2010.
Kroll, J. H., Donahue, N. M., Jimenez, J. L., Kessler,
S. H., Canagaratna, M. R., Wilson, K. R., Altieri, K. E., Mazzoleni,
L. R., Wozniak, A. S., Bluhm, H., Mysak, E. R., Smith, J. D., Kolb,
C. E., and Worsnop, D. R.: Carbon oxidation state as a metric for
describing the chemistry of atmospheric organic aerosol, Nat. Chem.,
3, 133–139, https://doi.org/10.1038/NCHEM.948, 2011.
Laidler, K. J.: The mechanisms of some elementary surface reactions, J. Phys. Colloid Chem., 53, 712–732, https://doi.org/10.1021/j150470a010, 1949.
Laidler, K. J., Glasstone, S., and Eyring, H.: Application of the Theory of Absolute Reaction Rates to Heterogeneous Processes II. Chemical Reactions on Surfaces, J. Chem. Phys., 8, 667–676, https://doi.org/10.1063/1.1750737, 1940.
Langmuir, I.: A theory of adsorption, Phys. Rev., 6, 79–80, 1915.
Langmuir, I.: The evaporation, condensation and reflection of molecules and the mechanism of adsorption, Phys. Rev., 8, 149–176, https://doi.org/10.1103/PhysRev.8.149, 1916.
Langmuir, I.: The adsorption of gases on plane surfaces of glass, mica and platinum, J. Am. Chem. Soc., 40, 1361–1403, https://doi.org/10.1021/ja02242a004, 1918.
Langmuir, I.: Vapor pressures, evaporation, condensation and adsorption, J. Am. Chem. Soc., 54, 2798–2832, https://doi.org/10.1021/ja01346a022, 1932.
Li, J. and Knopf, D. A.: Representation of Multiphase OH
Oxidation of Amorphous Organic Aerosol for Tropospheric Conditions,
Environ. Sci. Technol., 55, 7266–7275, https://doi.org/10.1021/acs.est.0c07668, 2021.
Li, J., Forrester, S. M., and Knopf, D. A.: Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures, Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, 2020.
McNaught, A. D. and Wilkinson, A.: IUPAC. Compendium of Chemical Terminology (the “Gold Book”), 2nd edn., Blackwell Scientific Publications, Oxford, 2014.
McQuarrie, D. A.: Statistical mechanics, University Science Books, Sausalito, CA, 631 pp., 2000.
Moise, T., Flores, J. M., and Rudich, Y.: Optical properties of secondary organic aerosols and their changes by chemical processes, Chem. Rev., 115, 4400–4439, https://doi.org/10.1021/cr5005259, 2015.
Pilling, M. J. and Seakins, P. W.: Reaction Kinetics, 2nd edn., Oxford Science Publications, Oxford University Press, New York, USA, 320 pp., 1996.
Pöschl, U. and Shiraiwa, M.: Multiphase Chemistry at the Atmosphere-Biosphere Interface Influencing Climate and Public Health in the Anthropocene, Chem. Rev., 115, 4440–4475, https://doi.org/10.1021/cr500487s, 2015.
Pöschl, U., Rudich, Y., and Ammann, M.: Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology, Atmos. Chem. Phys., 7, 5989–6023, 2007.
Ravishankara, A. R.: Heterogeneous and multiphase chemistry in the troposphere, Science, 276, 1058–1065, 1997.
Rowland, F. S.: Stratospheric ozone depletion, Annu. Rev. Phys. Chem., 42, 731–768, https://doi.org/10.1146/annurev.physchem.42.1.731, 1991.
Rudich, Y., Donahue, N. M., and Mentel, T. F.: Aging of organic aerosol: Bridging the gap between laboratory and field studies, Annu. Rev. Phys. Chem., 58, 321–352, https://doi.org/10.1146/annurev.physchem.58.032806.104432, 2007.
Savara, A.: Standard States for Adsorption on Solid Surfaces: 2D Gases, Surface Liquids, and Langmuir Adsorbates, J. Phys. Chem. C, 117, 15710–15715, https://doi.org/10.1021/jp404398z, 2013.
Shiraiwa, M. and Pöschl, U.: Mass accommodation and gas–particle partitioning in secondary organic aerosols: dependence on diffusivity, volatility, particle-phase reactions, and penetration depth, Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, 2021.
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801, https://doi.org/10.1029/2012gl054008, 2012.
Shiraiwa, M., Pfrang, C., Koop, T., and Pöschl, U.: Kinetic multi-layer model of gas-particle interactions in aerosols and clouds (KM-GAP): linking condensation, evaporation and chemical reactions of organics, oxidants and water, Atmos. Chem. Phys., 12, 2777–2794, 2012.
Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453, https://doi.org/10.1039/c3cp51595h, 2013.
Solomon, S.: Stratospheric ozone depletion: A review of concepts and history, Rev. Geophys., 37, 275–316, 1999.
Sprowl, L. H., Campbell, C. T., and Arnadottir, L.: Hindered Translator and Hindered Rotor Models for Adsorbates: Partition Functions and Entropies, J. Phys. Chem. C, 120, 9719–9731, https://doi.org/10.1021/acs.jpcc.5b11616, 2016.
Tabazadeh, A. and Turco, R. P.: A Model for Heterogeneous Chemical Processes on the Surfaces of Ice and Nitric-Acid Trihydrate Particles, J. Geophys. Res., 98, 12727–12740, 1993.
Tully, J. C.: The dynamics of adsorption and desorption, Surf. Sci., 299, 667–677, https://doi.org/10.1016/0039-6028(94)90688-2, 1994.
Short summary
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.
Adsorption on and desorption of gas molecules from solid or liquid surfaces or interfaces...
Altmetrics
Final-revised paper
Preprint