Articles | Volume 14, issue 18
https://doi.org/10.5194/acp-14-9993-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-14-9993-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
19 Sep 2014
Research article |
| 19 Sep 2014
Experimental determination of the temperature dependence of water activities for a selection of aqueous organic solutions
G. Ganbavale
Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
C. Marcolli
Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
Marcolli Chemistry and Physics Consulting GmbH, Zurich, Switzerland
U. K. Krieger
Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
Department of Atmospheric and Oceanic Sciences, McGill University, Montreal, Quebec, Canada
G. Stratmann
Department of Atmospheric Physics, DLR Oberpfaffenhofen, Germany
T. Peter
Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland
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Ryan Schmedding and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-1690, https://doi.org/10.5194/egusphere-2024-1690, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger
EGUsphere, https://doi.org/10.5194/egusphere-2024-1459, https://doi.org/10.5194/egusphere-2024-1459, 2024
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The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remain below an hour for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.
Sandro Vattioni, Andrea Stenke, Beiping Luo, Gabriel Chiodo, Timofei Sukhodolov, Elia Wunderlin, and Thomas Peter
Geosci. Model Dev., 17, 4181–4197, https://doi.org/10.5194/gmd-17-4181-2024, https://doi.org/10.5194/gmd-17-4181-2024, 2024
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We investigate the sensitivity of aerosol size distributions in the presence of strong SO2 injections for climate interventions or after volcanic eruptions to the call sequence and frequency of the routines for nucleation and condensation in sectional aerosol models with operator splitting. Using the aerosol–chemistry–climate model SOCOL-AERv2, we show that the radiative and chemical outputs are sensitive to these settings at high H2SO4 supersaturations and how to obtain reliable results.
Christina V. Brodowsky, Timofei Sukhodolov, Gabriel Chiodo, Valentina Aquila, Slimane Bekki, Sandip S. Dhomse, Michael Höpfner, Anton Laakso, Graham W. Mann, Ulrike Niemeier, Giovanni Pitari, Ilaria Quaglia, Eugene Rozanov, Anja Schmidt, Takashi Sekiya, Simone Tilmes, Claudia Timmreck, Sandro Vattioni, Daniele Visioni, Pengfei Yu, Yunqian Zhu, and Thomas Peter
Atmos. Chem. Phys., 24, 5513–5548, https://doi.org/10.5194/acp-24-5513-2024, https://doi.org/10.5194/acp-24-5513-2024, 2024
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The aerosol layer is an essential part of the climate system. We characterize the sulfur budget in a volcanically quiescent (background) setting, with a special focus on the sulfate aerosol layer using, for the first time, a multi-model approach. The aim is to identify weak points in the representation of the atmospheric sulfur budget in an intercomparison of nine state-of-the-art coupled global circulation models.
Sandro Vattioni, Rahel Weber, Aryehe Feinberg, Andrea Stenke, John A. Dykema, Beiping Luo, Georgios A. Kelesidis, Christian A. Bruun, Timofei Sukhodolov, Frank N. Keutsch, Thomas Peter, and Gabriel Chiodo
EGUsphere, https://doi.org/10.5194/egusphere-2024-444, https://doi.org/10.5194/egusphere-2024-444, 2024
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We quantified impacts and efficiency of stratospheric solar climate intervention via solid particle injection. Microphysical interactions of solid particles with the sulfur cycle were interactively coupled to the heterogeneous chemistry scheme and the radiative transfer code of an aerosol-chemistry climate model. Compared to injection of SO2 we find a stronger cooling efficiency for solid particles only when normalizing to the aerosol load, but not when normalizing to the injection rate.
Jan Clemens, Bärbel Vogel, Lars Hoffmann, Sabine Griessbach, Nicole Thomas, Suvarna Fadnavis, Rolf Müller, Thomas Peter, and Felix Ploeger
Atmos. Chem. Phys., 24, 763–787, https://doi.org/10.5194/acp-24-763-2024, https://doi.org/10.5194/acp-24-763-2024, 2024
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The source regions of the Asian tropopause aerosol layer (ATAL) are debated. We use balloon-borne measurements of the layer above Nainital (India) in August 2016 and atmospheric transport models to find ATAL source regions. Most air originated from the Tibetan plateau. However, the measured ATAL was stronger when more air originated from the Indo-Gangetic Plain and weaker when more air originated from the Pacific. Hence, the results indicate important anthropogenic contributions to the ATAL.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Franziska Zilker, Timofei Sukhodolov, Gabriel Chiodo, Marina Friedel, Tatiana Egorova, Eugene Rozanov, Jan Sedlacek, Svenja Seeber, and Thomas Peter
Atmos. Chem. Phys., 23, 13387–13411, https://doi.org/10.5194/acp-23-13387-2023, https://doi.org/10.5194/acp-23-13387-2023, 2023
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The Montreal Protocol (MP) has successfully reduced the Antarctic ozone hole by banning chlorofluorocarbons (CFCs) that destroy the ozone layer. Moreover, CFCs are strong greenhouse gases (GHGs) that would have strengthened global warming. In this study, we investigate the surface weather and climate in a world without the MP at the end of the 21st century, disentangling ozone-mediated and GHG impacts of CFCs. Overall, we avoided 1.7 K global surface warming and a poleward shift in storm tracks.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 23, 7741–7765, https://doi.org/10.5194/acp-23-7741-2023, https://doi.org/10.5194/acp-23-7741-2023, 2023
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Aerosol particles below 100 nm in diameter have high surface-area-to-volume ratios. The enrichment of compounds in the surface of an aerosol particle may lead to depletion of that species in the interior bulk of the particle. We present a framework for modeling the equilibrium bulk–surface partitioning of mixed organic–inorganic particles, including cases of co-condensation of semivolatile organic compounds and species with extremely limited solubility in the bulk or surface of a particle.
Anand Kumar, Kristian Klumpp, Chen Barak, Giora Rytwo, Michael Plötze, Thomas Peter, and Claudia Marcolli
Atmos. Chem. Phys., 23, 4881–4902, https://doi.org/10.5194/acp-23-4881-2023, https://doi.org/10.5194/acp-23-4881-2023, 2023
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Smectites are a major class of clay minerals that are ice nucleation (IN) active. They form platelets that swell or even delaminate in water by intercalation of water between their layers. We hypothesize that at least three smectite layers need to be stacked together to host a critical ice embryo on clay mineral edges and that the larger the surface edge area is, the higher the freezing temperature. Edge sites on such clay particles play a crucial role in imparting IN ability to such particles.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, and Thomas Peter
Atmos. Chem. Phys., 23, 4801–4817, https://doi.org/10.5194/acp-23-4801-2023, https://doi.org/10.5194/acp-23-4801-2023, 2023
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The future ozone evolution in SOCOLv4 simulations under SSP2-4.5 and SSP5-8.5 scenarios has been assessed for the period 2015–2099 and subperiods using the DLM approach. The SOCOLv4 projects a decline in tropospheric ozone in the 2030s in SSP2-4.5 and in the 2060s in SSP5-8.5. The stratospheric ozone increase is ~3 times higher in SSP5-8.5, confirming the important role of GHGs in ozone evolution. We also showed that tropospheric ozone strongly impacts the total column in the tropics.
Thomas Berkemeier, Matteo Krüger, Aryeh Feinberg, Marcel Müller, Ulrich Pöschl, and Ulrich K. Krieger
Geosci. Model Dev., 16, 2037–2054, https://doi.org/10.5194/gmd-16-2037-2023, https://doi.org/10.5194/gmd-16-2037-2023, 2023
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Kinetic multi-layer models (KMs) successfully describe heterogeneous and multiphase atmospheric chemistry. In applications requiring repeated execution, however, these models can be too expensive. We trained machine learning surrogate models on output of the model KM-SUB and achieved high correlations. The surrogate models run orders of magnitude faster, which suggests potential applicability in global optimization tasks and as sub-modules in large-scale atmospheric models.
Kristian Klumpp, Claudia Marcolli, Ana Alonso-Hellweg, Christopher H. Dreimol, and Thomas Peter
Atmos. Chem. Phys., 23, 1579–1598, https://doi.org/10.5194/acp-23-1579-2023, https://doi.org/10.5194/acp-23-1579-2023, 2023
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The prerequisites of a particle surface for efficient ice nucleation are still poorly understood. This study compares the ice nucleation activity of two chemically identical but morphologically different minerals (kaolinite and halloysite). We observe, on average, not only higher ice nucleation activities for halloysite than kaolinite but also higher diversity between individual samples. We identify the particle edges as being the most likely site for ice nucleation.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, William Ball, and Thomas Peter
Atmos. Chem. Phys., 22, 15333–15350, https://doi.org/10.5194/acp-22-15333-2022, https://doi.org/10.5194/acp-22-15333-2022, 2022
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Applying the dynamic linear model, we confirm near-global ozone recovery (55°N–55°S) in the mesosphere, upper and middle stratosphere, and a steady increase in the troposphere. We also show that modern chemistry–climate models (CCMs) like SOCOLv4 may reproduce the observed trend distribution of lower stratospheric ozone, despite exhibiting a lower magnitude and statistical significance. The obtained ozone trend pattern in SOCOLv4 is generally consistent with observations and reanalysis datasets.
Nikou Hamzehpour, Claudia Marcolli, Sara Pashai, Kristian Klumpp, and Thomas Peter
Atmos. Chem. Phys., 22, 14905–14930, https://doi.org/10.5194/acp-22-14905-2022, https://doi.org/10.5194/acp-22-14905-2022, 2022
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Playa surfaces in Iran that emerged through Lake Urmia (LU) desiccation have become a relevant dust source of regional relevance. Here, we identify highly erodible LU playa surfaces and determine their physicochemical properties and mineralogical composition and perform emulsion-freezing experiments with them. We find high ice nucleation activities (up to 250 K) that correlate positively with organic matter and clay content and negatively with pH, salinity, K-feldspars, and quartz.
Nikou Hamzehpour, Claudia Marcolli, Kristian Klumpp, Debora Thöny, and Thomas Peter
Atmos. Chem. Phys., 22, 14931–14956, https://doi.org/10.5194/acp-22-14931-2022, https://doi.org/10.5194/acp-22-14931-2022, 2022
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Dust aerosols from dried lakebeds contain mineral particles, as well as soluble salts and (bio-)organic compounds. Here, we investigate ice nucleation (IN) activity of dust samples from Lake Urmia playa, Iran. We find high IN activity of the untreated samples that decreases after organic matter removal but increases after removing soluble salts and carbonates, evidencing inhibiting effects of soluble salts and carbonates on the IN activity of organic matter and minerals, especially microcline.
Marina Friedel, Gabriel Chiodo, Andrea Stenke, Daniela I. V. Domeisen, and Thomas Peter
Atmos. Chem. Phys., 22, 13997–14017, https://doi.org/10.5194/acp-22-13997-2022, https://doi.org/10.5194/acp-22-13997-2022, 2022
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In spring, winds the Arctic stratosphere change direction – an event called final stratospheric warming (FSW). Here, we examine whether the interannual variability in Arctic stratospheric ozone impacts the timing of the FSW. We find that Arctic ozone shifts the FSW to earlier and later dates in years with high and low ozone via the absorption of UV light. The modulation of the FSW by ozone has consequences for surface climate in ozone-rich years, which may result in better seasonal predictions.
Florin N. Isenrich, Nadia Shardt, Michael Rösch, Julia Nette, Stavros Stavrakis, Claudia Marcolli, Zamin A. Kanji, Andrew J. deMello, and Ulrike Lohmann
Atmos. Meas. Tech., 15, 5367–5381, https://doi.org/10.5194/amt-15-5367-2022, https://doi.org/10.5194/amt-15-5367-2022, 2022
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Ice nucleation in the atmosphere influences cloud properties and lifetimes. Microfluidic instruments have recently been used to investigate ice nucleation, but these instruments are typically made out of a polymer that contributes to droplet instability over extended timescales and relatively high temperature uncertainty. To address these drawbacks, we develop and validate a new microfluidic instrument that uses fluoropolymer tubing to extend droplet stability and improve temperature accuracy.
Clare E. Singer, Benjamin W. Clouser, Sergey M. Khaykin, Martina Krämer, Francesco Cairo, Thomas Peter, Alexey Lykov, Christian Rolf, Nicole Spelten, Armin Afchine, Simone Brunamonti, and Elisabeth J. Moyer
Atmos. Meas. Tech., 15, 4767–4783, https://doi.org/10.5194/amt-15-4767-2022, https://doi.org/10.5194/amt-15-4767-2022, 2022
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In situ measurements of water vapor in the upper troposphere are necessary to study cloud formation and hydration of the stratosphere but challenging due to cold–dry conditions. We compare measurements from three water vapor instruments from the StratoClim campaign in 2017. In clear sky (clouds), point-by-point differences were <1.5±8 % (<1±8 %). This excellent agreement allows detection of fine-scale structures required to understand the impact of convection on stratospheric water vapor.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817, https://doi.org/10.5194/acp-22-8805-2022, https://doi.org/10.5194/acp-22-8805-2022, 2022
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In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166, https://doi.org/10.5194/acp-22-4149-2022, https://doi.org/10.5194/acp-22-4149-2022, 2022
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Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Kristian Klumpp, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 22, 3655–3673, https://doi.org/10.5194/acp-22-3655-2022, https://doi.org/10.5194/acp-22-3655-2022, 2022
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Surface interactions with solutes can significantly alter the ice nucleation activity of mineral dust. Past studies revealed the sensitivity of microcline, one of the most ice-active types of dust in the atmosphere, to inorganic solutes. This study focuses on the interaction of microcline with bio-organic substances and the resulting effects on its ice nucleation activity. We observe strongly hampered ice nucleation activity due to the presence of carboxylic and amino acids but not for polyols.
Joseph Lilek and Andreas Zuend
Atmos. Chem. Phys., 22, 3203–3233, https://doi.org/10.5194/acp-22-3203-2022, https://doi.org/10.5194/acp-22-3203-2022, 2022
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Depending on temperature and chemical makeup, certain aerosols can be highly viscous or glassy, with atmospheric implications. We have therefore implemented two major upgrades to the predictive viscosity model AIOMFAC-VISC. First, we created a new viscosity model for aqueous electrolyte solutions containing an arbitrary number of ion species. Second, we integrated the electrolyte model within the existing AIOMFAC-VISC framework to enable viscosity predictions for organic–inorganic mixtures.
Debra K. Weisenstein, Daniele Visioni, Henning Franke, Ulrike Niemeier, Sandro Vattioni, Gabriel Chiodo, Thomas Peter, and David W. Keith
Atmos. Chem. Phys., 22, 2955–2973, https://doi.org/10.5194/acp-22-2955-2022, https://doi.org/10.5194/acp-22-2955-2022, 2022
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This paper explores a potential method of geoengineering that could be used to slow the rate of change of climate over decadal scales. We use three climate models to explore how injections of accumulation-mode sulfuric acid aerosol change the large-scale stratospheric particle size distribution and radiative forcing response for the chosen scenarios. Radiative forcing per unit sulfur injected and relative to the change in aerosol burden is larger with particulate than with SO2 injections.
Hang Yin, Jing Dou, Liviana Klein, Ulrich K. Krieger, Alison Bain, Brandon J. Wallace, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 22, 973–1013, https://doi.org/10.5194/acp-22-973-2022, https://doi.org/10.5194/acp-22-973-2022, 2022
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Iodine and carbonate species are important components in marine and dust aerosols, respectively. We introduce an extended version of the AIOMFAC thermodynamic mixing model, which includes the ions I−, IO3−, HCO3−, CO32−, OH−, and CO2(aq) as new species, and we discuss two methods for solving the carbonate dissociation equilibria numerically. We also present new experimental water activity data for aqueous iodide and iodate systems.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Bernd Kärcher and Claudia Marcolli
Atmos. Chem. Phys., 21, 15213–15220, https://doi.org/10.5194/acp-21-15213-2021, https://doi.org/10.5194/acp-21-15213-2021, 2021
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Aerosol–cloud interactions play an important role in climate change. Simulations of the competition between homogeneous solution droplet freezing and heterogeneous ice nucleation can be compromised by the misapplication of ice-active particle fractions frequently derived from laboratory measurements or parametrizations. Our study frames the problem and establishes a solution that is easy to implement in cloud models.
Timofei Sukhodolov, Tatiana Egorova, Andrea Stenke, William T. Ball, Christina Brodowsky, Gabriel Chiodo, Aryeh Feinberg, Marina Friedel, Arseniy Karagodin-Doyennel, Thomas Peter, Jan Sedlacek, Sandro Vattioni, and Eugene Rozanov
Geosci. Model Dev., 14, 5525–5560, https://doi.org/10.5194/gmd-14-5525-2021, https://doi.org/10.5194/gmd-14-5525-2021, 2021
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This paper features the new atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0 and its validation. The model performance is evaluated against reanalysis products and observations of atmospheric circulation and trace gas distribution, with a focus on stratospheric processes. Although we identified some problems to be addressed in further model upgrades, we demonstrated that SOCOLv4.0 is already well suited for studies related to chemistry–climate–aerosol interactions.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
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We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Claudia Marcolli, Fabian Mahrt, and Bernd Kärcher
Atmos. Chem. Phys., 21, 7791–7843, https://doi.org/10.5194/acp-21-7791-2021, https://doi.org/10.5194/acp-21-7791-2021, 2021
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Pores are aerosol particle features that trigger ice nucleation, as they take up water by capillary condensation below water saturation that freezes at low temperatures. The pore ice can then grow into macroscopic ice crystals making up cirrus clouds. Here, we investigate the pores in soot aggregates responsible for pore condensation and freezing (PCF). Moreover, we present a framework to parameterize soot PCF that is able to predict the ice nucleation activity based on soot properties.
Manuel Graf, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Thomas Peter, Ruud Dirksen, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 14, 1365–1378, https://doi.org/10.5194/amt-14-1365-2021, https://doi.org/10.5194/amt-14-1365-2021, 2021
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Water vapor is the most important natural greenhouse gas. The accurate and frequent measurement of its abundance, especially in the upper troposphere and lower stratosphere (UTLS), is technically challenging. We developed and characterized a mid-IR absorption spectrometer for highly accurate water vapor measurements in the UTLS. The instrument is sufficiently small and lightweight (3.9 kg) to be carried by meteorological balloons, which enables frequent and cost-effective soundings.
Weigang Wang, Ting Lei, Andreas Zuend, Hang Su, Yafang Cheng, Yajun Shi, Maofa Ge, and Mingyuan Liu
Atmos. Chem. Phys., 21, 2179–2190, https://doi.org/10.5194/acp-21-2179-2021, https://doi.org/10.5194/acp-21-2179-2021, 2021
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Aerosol mixing state regulates the interactions between water molecules and particles and thus controls aerosol activation and hygroscopic growth, which thereby influences visibility degradation, cloud formation, and its radiative forcing. However, there are few studies attempting to investigate their interactions with water molecules. Here, we investigated the effect of organic coatings on the hygroscopic behavior of the inorganic core.
Michael Steiner, Beiping Luo, Thomas Peter, Michael C. Pitts, and Andrea Stenke
Geosci. Model Dev., 14, 935–959, https://doi.org/10.5194/gmd-14-935-2021, https://doi.org/10.5194/gmd-14-935-2021, 2021
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We evaluate polar stratospheric clouds (PSCs) as simulated by the chemistry–climate model (CCM) SOCOLv3.1 in comparison with measurements by the CALIPSO satellite. A cold bias results in an overestimated PSC area and mountain-wave ice is underestimated, but we find overall good temporal and spatial agreement of PSC occurrence and composition. This work confirms previous studies indicating that simplified PSC schemes may also achieve good approximations of the fundamental properties of PSCs.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, https://doi.org/10.5194/acp-21-2053-2021, 2021
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This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
Teresa Jorge, Simone Brunamonti, Yann Poltera, Frank G. Wienhold, Bei P. Luo, Peter Oelsner, Sreeharsha Hanumanthu, Bhupendra B. Singh, Susanne Körner, Ruud Dirksen, Manish Naja, Suvarna Fadnavis, and Thomas Peter
Atmos. Meas. Tech., 14, 239–268, https://doi.org/10.5194/amt-14-239-2021, https://doi.org/10.5194/amt-14-239-2021, 2021
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Balloon-borne frost point hygrometers are crucial for the monitoring of water vapour in the upper troposphere and lower stratosphere. We found that when traversing a mixed-phase cloud with big supercooled droplets, the intake tube of the instrument collects on its inner surface a high percentage of these droplets. The newly formed ice layer will sublimate at higher levels and contaminate the measurement. The balloon is also a source of contamination, but only at higher levels during the ascent.
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
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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.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Ales Kuchar, William Ball, Pavle Arsenovic, Ellis Remsberg, Patrick Jöckel, Markus Kunze, David A. Plummer, Andrea Stenke, Daniel Marsh, Doug Kinnison, and Thomas Peter
Atmos. Chem. Phys., 21, 201–216, https://doi.org/10.5194/acp-21-201-2021, https://doi.org/10.5194/acp-21-201-2021, 2021
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The solar signal in the mesospheric H2O and CO was extracted from the CCMI-1 model simulations and satellite observations using multiple linear regression (MLR) analysis. MLR analysis shows a pronounced and statistically robust solar signal in both H2O and CO. The model results show a general agreement with observations reproducing a negative/positive solar signal in H2O/CO. The pattern of the solar signal varies among the considered models, reflecting some differences in the model setup.
Sreeharsha Hanumanthu, Bärbel Vogel, Rolf Müller, Simone Brunamonti, Suvarna Fadnavis, Dan Li, Peter Ölsner, Manish Naja, Bhupendra Bahadur Singh, Kunchala Ravi Kumar, Sunil Sonbawne, Hannu Jauhiainen, Holger Vömel, Beiping Luo, Teresa Jorge, Frank G. Wienhold, Ruud Dirkson, and Thomas Peter
Atmos. Chem. Phys., 20, 14273–14302, https://doi.org/10.5194/acp-20-14273-2020, https://doi.org/10.5194/acp-20-14273-2020, 2020
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During boreal summer, anthropogenic sources yield the Asian Tropopause Aerosol Layer (ATAL), found in Asia between about 13 and 18 km altitude. Balloon-borne measurements of the ATAL conducted in northern India in 2016 show the strong variability of the ATAL. To explain its observed variability, model simulations are performed to deduce the origin of air masses on the Earth's surface, which is important to develop recommendations for regulations of anthropogenic surface emissions of the ATAL.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Robert O. David, Jonas Fahrni, Claudia Marcolli, Fabian Mahrt, Dominik Brühwiler, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 9419–9440, https://doi.org/10.5194/acp-20-9419-2020, https://doi.org/10.5194/acp-20-9419-2020, 2020
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Ice crystal formation plays an important role in controlling the Earth's climate. However, the mechanisms responsible for ice formation in the atmosphere are still uncertain. Here we use surrogates for atmospherically relevant porous particles to determine the role of pore diameter and wettability on the ability of porous particles to nucleate ice in the atmosphere. Our results are consistent with the pore condensation and freeing mechanism.
Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314, https://doi.org/10.5194/acp-20-8293-2020, https://doi.org/10.5194/acp-20-8293-2020, 2020
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The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Nir Bluvshtein, Ulrich K. Krieger, and Thomas Peter
Atmos. Meas. Tech., 13, 3191–3203, https://doi.org/10.5194/amt-13-3191-2020, https://doi.org/10.5194/amt-13-3191-2020, 2020
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Light-absorbing organic particles undergo transformations during their exposure in the atmosphere. The role these particles play in the global radiative balance is uncertain. This study describes high-sensitivity and high-precision measurements of light absorption by a single particle levitated in an electrodynamic balance. This high level of sensitivity enables future studies to explore the major processes responsible for changes to the particle's light absorptivity.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
María Cascajo-Castresana, Robert O. David, Maiara A. Iriarte-Alonso, Alexander M. Bittner, and Claudia Marcolli
Atmos. Chem. Phys., 20, 3291–3315, https://doi.org/10.5194/acp-20-3291-2020, https://doi.org/10.5194/acp-20-3291-2020, 2020
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Atmospheric ice-nucleating particles are rare but relevant for cloud glaciation. A source of particles that nucleate ice above −15 °C is biological material including some proteins. Here we show that proteins of very diverse functions and structures can nucleate ice. Among these, the iron storage protein apoferritin stands out, with activity up to −4 °C. We show that its activity does not stem from correctly assembled proteins but from misfolded protein monomers or oligomers and aggregates.
Claudia Marcolli
Atmos. Chem. Phys., 20, 3209–3230, https://doi.org/10.5194/acp-20-3209-2020, https://doi.org/10.5194/acp-20-3209-2020, 2020
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Pore condensation and freezing (PCF) is an ice nucleation mechanism explaining ice formation at low ice supersaturation. It is assumed that liquid water condenses in pores of solid aerosol particles below water saturation followed by ice nucleation within the pores. This study discusses conditions of pore filling, homogeneous ice nucleation within the volume of porewater, and growth of ice out of the pores, taking the effect of negative pressure within pores below water saturation into account.
Natalie R. Gervasi, David O. Topping, and Andreas Zuend
Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, https://doi.org/10.5194/acp-20-2987-2020, 2020
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Organic aerosols have been shown to exist often in a semi-solid or amorphous, glassy state. Highly viscous particles behave differently than their well-mixed liquid analogues with consequences for a variety of aerosol processes. Here, we introduce a new predictive mixture viscosity model called AIOMFAC-VISC. It enables us to predict the viscosity of aqueous organic mixtures as a function of temperature and chemical composition, covering the full range of liquid, semi-solid, and glassy states.
Aryeh Feinberg, Moustapha Maliki, Andrea Stenke, Bruno Sudret, Thomas Peter, and Lenny H. E. Winkel
Atmos. Chem. Phys., 20, 1363–1390, https://doi.org/10.5194/acp-20-1363-2020, https://doi.org/10.5194/acp-20-1363-2020, 2020
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The amount of the micronutrient selenium in food largely depends on the amount and form of selenium in soil. The atmosphere acts as a source of selenium to soils through deposition, yet little information is available about atmospheric selenium cycling. Therefore, we built the first global atmospheric selenium model. Through sensitivity and uncertainty analysis we determine that selenium can be transported thousands of kilometers and that measurements of selenium emissions should be prioritized.
Robert O. David, Maria Cascajo-Castresana, Killian P. Brennan, Michael Rösch, Nora Els, Julia Werz, Vera Weichlinger, Lin S. Boynton, Sophie Bogler, Nadine Borduas-Dedekind, Claudia Marcolli, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 6865–6888, https://doi.org/10.5194/amt-12-6865-2019, https://doi.org/10.5194/amt-12-6865-2019, 2019
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Here we present the development and applicability of the DRoplet Ice Nuclei Counter Zurich (DRINCZ). DRINCZ allows for ice nuclei in the immersion mode to be quantified between 0 and -25 °C with an uncertainty of ±0.9 °C. Furthermore, we present a new method for assessing biases in drop-freezing apparatuses and cumulative ice-nucleating-particle concentrations from snow samples collected in the Austrian Alps at the Sonnblick Observatory.
Kyle Gorkowski, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 19, 13383–13407, https://doi.org/10.5194/acp-19-13383-2019, https://doi.org/10.5194/acp-19-13383-2019, 2019
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We present the new Binary Activity Thermodynamics (BAT) model, which is a water-sensitive reduced-complexity organic aerosol thermodynamics model. It can use bulk properties like O : C, molar mass, and RH to predict organic activity coefficients and water uptake behavior. We show applications in RH-dependent organic co-condensation, liquid–liquid phase separation, and Kohler curve predictions, and we validate the BAT model against laboratory measurements.
William T. Ball, Justin Alsing, Johannes Staehelin, Sean M. Davis, Lucien Froidevaux, and Thomas Peter
Atmos. Chem. Phys., 19, 12731–12748, https://doi.org/10.5194/acp-19-12731-2019, https://doi.org/10.5194/acp-19-12731-2019, 2019
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We analyse long-term stratospheric ozone (60° S–60° N) trends over the 1985–2018 period. Previous work has suggested that lower stratosphere ozone declined over 1998–2016. We demonstrate that a large ozone upsurge in 2017 is likely related to QBO variability, but that lower stratospheric ozone trends likely remain lower in 2018 than in 1998. Tropical stratospheric ozone (30° S–30° N) shows highly probable decreases in both the lower stratosphere and in the integrated stratospheric ozone layer.
Vanessa Brocchi, Gisèle Krysztofiak, Adrien Deroubaix, Greta Stratmann, Daniel Sauer, Hans Schlager, Konrad Deetz, Guillaume Dayma, Claude Robert, Stéphane Chevrier, and Valéry Catoire
Atmos. Chem. Phys., 19, 11401–11411, https://doi.org/10.5194/acp-19-11401-2019, https://doi.org/10.5194/acp-19-11401-2019, 2019
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This study reports the first flaring in situ measurements in southern West Africa. According to the measurements, oil rig flaring plumes in Ghana lead to increases in NO2 and aerosols but not always in CO and not in SO2. Flaring measurements can be reproduced using FLEXPART model, adjusting both the emission flux and the injection height. The DACCIWA satellite flaring inventory provides a reasonable estimate of flaring emission.
Aryeh Feinberg, Timofei Sukhodolov, Bei-Ping Luo, Eugene Rozanov, Lenny H. E. Winkel, Thomas Peter, and Andrea Stenke
Geosci. Model Dev., 12, 3863–3887, https://doi.org/10.5194/gmd-12-3863-2019, https://doi.org/10.5194/gmd-12-3863-2019, 2019
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We have improved several aspects of atmospheric sulfur cycling in SOCOL-AER, an aerosol–chemistry–climate model. The newly implemented features in SOCOL-AERv2 include interactive deposition schemes, improved sulfur mass conservation, and expanded tropospheric chemistry. SOCOL-AERv2 shows better agreement with stratospheric aerosol observations and sulfur deposition networks compared to SOCOL-AERv1. SOCOL-AERv2 can be used to study impacts of sulfate aerosol on climate, chemistry, and ecosystems.
Hoi Ki Lam, Sze Man Shum, James F. Davies, Mijung Song, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 19, 9581–9593, https://doi.org/10.5194/acp-19-9581-2019, https://doi.org/10.5194/acp-19-9581-2019, 2019
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We show the presence of dissolved inorganic salts could reduce the overall heterogeneous reactivity of organic compounds with gas–phase OH radicals at the surface by lowering the surface concentration of organic compounds. Until recently, the kinetic parameters reported in the literature were mostly measured based on experiments with pure organic particles. The lifetime of organic compounds or chemical tracers against heterogeneous OH reaction in the atmosphere could be longer than expected.
Pavle Arsenovic, Alessandro Damiani, Eugene Rozanov, Bernd Funke, Andrea Stenke, and Thomas Peter
Atmos. Chem. Phys., 19, 9485–9494, https://doi.org/10.5194/acp-19-9485-2019, https://doi.org/10.5194/acp-19-9485-2019, 2019
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Low-energy electrons (LEE) are the dominant source of odd nitrogen, which destroys ozone, in the mesosphere and stratosphere in polar winter in the geomagnetically active periods. However, the observed stratospheric ozone anomalies can be reproduced only when accounting for both low- and middle-range energy electrons (MEE) in the chemistry-climate model. Ozone changes may induce further dynamical and thermal changes in the atmosphere. We recommend including both LEE and MEE in climate models.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6035–6058, https://doi.org/10.5194/acp-19-6035-2019, https://doi.org/10.5194/acp-19-6035-2019, 2019
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This paper not only interests the atmospheric science community but has a potential to cater to a broader audience. We discuss both long- and
short-term effects of various
atmospherically relevantchemical species on a fairly abundant mineral surface
Quartz. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6059–6084, https://doi.org/10.5194/acp-19-6059-2019, https://doi.org/10.5194/acp-19-6059-2019, 2019
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This paper not only interests the Atmospheric Science community but has a potential to cater to a broader audience. We discuss both long- and short-term effects of various
atmospherically relevantchemical species on fairly abundant mineral surfaces like feldspars and clays. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Sandro Vattioni, Debra Weisenstein, David Keith, Aryeh Feinberg, Thomas Peter, and Andrea Stenke
Atmos. Chem. Phys., 19, 4877–4897, https://doi.org/10.5194/acp-19-4877-2019, https://doi.org/10.5194/acp-19-4877-2019, 2019
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This study is among the first modeling studies on stratospheric sulfate geoengineering that interactively couple a size-resolved sectional aerosol module to well-described stratospheric chemistry and radiation schemes in a global 3-D chemistry–climate model. We found that compared with SO2 injection, the direct emission of aerosols results in more effective radiative forcing and that sensitivities to different injection strategies vary for different forms of injected sulfur.
James F. Davies, Andreas Zuend, and Kevin R. Wilson
Atmos. Chem. Phys., 19, 2933–2946, https://doi.org/10.5194/acp-19-2933-2019, https://doi.org/10.5194/acp-19-2933-2019, 2019
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The formation of cloud droplets involves the condensation of water onto preexisting particles in the atmosphere. The efficiency of this process depends on the nature of the particles, and recent work has shown that organic-rich particles may exhibit a suppressed surface tension that promotes the formation of cloud droplets. In this technical note, we discuss the mechanism for this and highlight the evolution of surface tension as the key factor in the extent of surface effects.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
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Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Simone Brunamonti, Teresa Jorge, Peter Oelsner, Sreeharsha Hanumanthu, Bhupendra B. Singh, K. Ravi Kumar, Sunil Sonbawne, Susanne Meier, Deepak Singh, Frank G. Wienhold, Bei Ping Luo, Maxi Boettcher, Yann Poltera, Hannu Jauhiainen, Rijan Kayastha, Jagadishwor Karmacharya, Ruud Dirksen, Manish Naja, Markus Rex, Suvarna Fadnavis, and Thomas Peter
Atmos. Chem. Phys., 18, 15937–15957, https://doi.org/10.5194/acp-18-15937-2018, https://doi.org/10.5194/acp-18-15937-2018, 2018
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Based on balloon-borne measurements performed in India and Nepal in 2016–2017, we infer the vertical distributions of water vapor, ozone and aerosols in the atmosphere, from the surface to 30 km altitude. Our measurements show that the atmospheric dynamics of the Asian summer monsoon system over the polluted Indian subcontinent lead to increased concentrations of water vapor and aerosols in the high atmosphere (approximately 14–20 km altitude), which can have an important effect on climate.
Mehrnoush M. Fard, Ulrich K. Krieger, and Thomas Peter
Atmos. Chem. Phys., 18, 13511–13530, https://doi.org/10.5194/acp-18-13511-2018, https://doi.org/10.5194/acp-18-13511-2018, 2018
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Atmospheric aerosol particles may undergo liquid–liquid phase separation (LLPS) when exposed to varying relative humidity, with an aqueous organic phase enclosing an aqueous inorganic phase below a threshold of relative humidity. Brown carbon (BrC) compounds will redistribute to the organic phase upon LLPS. We use numerical modeling to study the shortwave radiative impact of LLPS containing BrC and conclude that it is not significant for atmospheric aerosol.
Fabian Mahrt, Claudia Marcolli, Robert O. David, Philippe Grönquist, Eszter J. Barthazy Meier, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 13363–13392, https://doi.org/10.5194/acp-18-13363-2018, https://doi.org/10.5194/acp-18-13363-2018, 2018
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The ice nucleation ability of different soot particles in the cirrus and mixed-phase cloud temperature regime is presented. The impact of aerosol particle size, particle morphology, organic matter and hydrophilicity on ice nucleation is examined. We propose ice nucleation proceeds via a pore condensation freezing mechanism for soot particles with the necessary physicochemical properties that nucleated ice well below water saturation.
Timofei Sukhodolov, Jian-Xiong Sheng, Aryeh Feinberg, Bei-Ping Luo, Thomas Peter, Laura Revell, Andrea Stenke, Debra K. Weisenstein, and Eugene Rozanov
Geosci. Model Dev., 11, 2633–2647, https://doi.org/10.5194/gmd-11-2633-2018, https://doi.org/10.5194/gmd-11-2633-2018, 2018
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The Pinatubo eruption in 1991 is the strongest directly observed volcanic event. In a series of experiments, we simulate its influence on the stratospheric aerosol layer using a state-of-the-art aerosol–chemistry–climate model, SOCOL-AERv1.0, and compare our results to observations. We show that SOCOL-AER reproduces the most important atmospheric effects and can therefore be used to study the climate effects of future volcanic eruptions and geoengineering by artificial sulfate aerosol.
Anand Kumar, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 18, 7057–7079, https://doi.org/10.5194/acp-18-7057-2018, https://doi.org/10.5194/acp-18-7057-2018, 2018
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We have performed immersion freezing experiments with microcline (most active ice nucleation, IN, K-feldspar polymorph) and investigated the effect of ammonium and non-ammonium solutes on its IN efficiency. We report increased IN efficiency of microcline in dilute ammonia- or ammonium-containing solutions, which opens up a pathway for condensation freezing occurring at a warmer temperature than immersion freezing.
Fabian Schoenenberger, Stephan Henne, Matthias Hill, Martin K. Vollmer, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Simon O'Doherty, Michela Maione, Lukas Emmenegger, Thomas Peter, and Stefan Reimann
Atmos. Chem. Phys., 18, 4069–4092, https://doi.org/10.5194/acp-18-4069-2018, https://doi.org/10.5194/acp-18-4069-2018, 2018
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Anthropogenic halocarbon emissions contribute to stratospheric ozone depletion and global warming. We measured atmospheric halocarbons for 6 months on Crete to extend the coverage of the existing observation network to the Eastern Mediterranean. The derived emission estimates showed a contribution of 16.8 % (13.6–23.3 %) and 53.2 % (38.1–84.2 %) of this region to the total HFC and HCFC emissions of the analyzed European domain and a reduction of the underlying uncertainties by 40–80 %.
Larry W. Thomason, Nicholas Ernest, Luis Millán, Landon Rieger, Adam Bourassa, Jean-Paul Vernier, Gloria Manney, Beiping Luo, Florian Arfeuille, and Thomas Peter
Earth Syst. Sci. Data, 10, 469–492, https://doi.org/10.5194/essd-10-469-2018, https://doi.org/10.5194/essd-10-469-2018, 2018
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We describe the construction of a continuous 38-year record of stratospheric aerosol optical properties. The Global Space-based Stratospheric Aerosol Climatology, or GloSSAC, provided the input data to the construction of the Climate Model Intercomparison Project stratospheric aerosol forcing data set (1979 to 2014) and is now extended through 2016. GloSSAC focuses on the the SAGE series of instruments through mid-2005 and on OSIRIS and CALIPSO after that time.
Pavle Arsenovic, Eugene Rozanov, Julien Anet, Andrea Stenke, Werner Schmutz, and Thomas Peter
Atmos. Chem. Phys., 18, 3469–3483, https://doi.org/10.5194/acp-18-3469-2018, https://doi.org/10.5194/acp-18-3469-2018, 2018
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Global warming will persist in the 21st century, even if the solar activity undergoes an unusually strong and long decline. Decreased ozone production caused by reduction of solar activity and change of atmospheric dynamics due to the global warming might result in further thinning of the tropical ozone layer. Globally, total ozone would not recover to the pre-ozone hole values as long as the decline of solar activity lasts. This may let more ultra-violet radiation reach the Earth's surface.
William T. Ball, Justin Alsing, Daniel J. Mortlock, Johannes Staehelin, Joanna D. Haigh, Thomas Peter, Fiona Tummon, Rene Stübi, Andrea Stenke, John Anderson, Adam Bourassa, Sean M. Davis, Doug Degenstein, Stacey Frith, Lucien Froidevaux, Chris Roth, Viktoria Sofieva, Ray Wang, Jeannette Wild, Pengfei Yu, Jerald R. Ziemke, and Eugene V. Rozanov
Atmos. Chem. Phys., 18, 1379–1394, https://doi.org/10.5194/acp-18-1379-2018, https://doi.org/10.5194/acp-18-1379-2018, 2018
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Using a robust analysis, with artefact-corrected ozone data, we confirm upper stratospheric ozone is recovering following the Montreal Protocol, but that lower stratospheric ozone (50° S–50° N) has continued to decrease since 1998, and the ozone layer as a whole (60° S–60° N) may be lower today than in 1998. No change in total column ozone may be due to increasing tropospheric ozone. State-of-the-art models do not reproduce lower stratospheric ozone decreases.
Ting Lei, Andreas Zuend, Yafang Cheng, Hang Su, Weigang Wang, and Maofa Ge
Atmos. Chem. Phys., 18, 1045–1064, https://doi.org/10.5194/acp-18-1045-2018, https://doi.org/10.5194/acp-18-1045-2018, 2018
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Measurements and thermodynamic equilibrium predictions for organic–inorganic aerosols related to components from biomass burning emissions demonstrate a diversity of hygroscopic growth and shrinking behavior, which we observed using a hygroscopicity tandem differential mobility analyzer (HTDMA). Controlled laboratory experiments with single solutes and/or with mixed organic–inorganic systems of known phase state will be useful to constrain model parameters of thermodynamic equilibrium models.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
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Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Adam W. Birdsall, Ulrich K. Krieger, and Frank N. Keutsch
Atmos. Meas. Tech., 11, 33–47, https://doi.org/10.5194/amt-11-33-2018, https://doi.org/10.5194/amt-11-33-2018, 2018
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We have developed a laboratory system that provides mass spectra of individual particles, roughly 20 microns in diameter, after they have been levitated in an electric field. Measured evaporation of polyethylene glycol particles was found to agree with a kinetic model. The system can be used to study fundamental chemical and physical processes involving particles that are difficult to isolate and study with other techniques, and hence improve our understanding of atmospheric particles.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
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In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Laura E. Revell, Andrea Stenke, Beiping Luo, Stefanie Kremser, Eugene Rozanov, Timofei Sukhodolov, and Thomas Peter
Atmos. Chem. Phys., 17, 13139–13150, https://doi.org/10.5194/acp-17-13139-2017, https://doi.org/10.5194/acp-17-13139-2017, 2017
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Compiling stratospheric aerosol data sets after a major volcanic eruption is difficult as the stratosphere becomes too optically opaque for satellite instruments to measure accurately. We performed ensemble chemistry–climate model simulations with two stratospheric aerosol data sets compiled for two international modelling activities and compared the simulated volcanic aerosol-induced effects from the 1991 Mt Pinatubo eruption on tropical stratospheric temperature and ozone with observations.
Sandra Bastelberger, Ulrich K. Krieger, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 17, 8453–8471, https://doi.org/10.5194/acp-17-8453-2017, https://doi.org/10.5194/acp-17-8453-2017, 2017
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We present quantitative condensed-phase diffusivity measurements of a volatile organic (tetraethylene glycol) in highly viscous single aerosol particles (aqueous sucrose). The condensed-phase diffusivity exhibits a strong temperature and humidity dependence. Our results suggest that diffusion limitations of volatile organics in highly viscous organic aerosol may severely impact gas–particle partitioning under cold and dry conditions.
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
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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.
Lisa Stirnweis, Claudia Marcolli, Josef Dommen, Peter Barmet, Carla Frege, Stephen M. Platt, Emily A. Bruns, Manuel Krapf, Jay G. Slowik, Robert Wolf, Andre S. H. Prévôt, Urs Baltensperger, and Imad El-Haddad
Atmos. Chem. Phys., 17, 5035–5061, https://doi.org/10.5194/acp-17-5035-2017, https://doi.org/10.5194/acp-17-5035-2017, 2017
Lukas Kaufmann, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 17, 3525–3552, https://doi.org/10.5194/acp-17-3525-2017, https://doi.org/10.5194/acp-17-3525-2017, 2017
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To improve the understanding of heterogeneous ice nucleation, we have subjected different ice nuclei to repeated freezing cycles and evaluated the freezing temperatures with different parameterizations of classical nucleation theory. It was found that two fit parameters were necessary to describe the temperature dependence of the nucleation rate.
Claudia Marcolli
Atmos. Chem. Phys., 17, 1595–1622, https://doi.org/10.5194/acp-17-1595-2017, https://doi.org/10.5194/acp-17-1595-2017, 2017
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Laboratory studies from the last century have shown that some types of particles are susceptible to pre-activation, i.e. they are able to develop macroscopic ice at warmer temperatures or lower relative humidities after they had been involved in an ice nucleation event before. This review analyses these works under the presumption that pre-activation occurs by ice preserved in pores, and it discusses atmospheric scenarios for which pre-activation might be important.
William T. Ball, Aleš Kuchař, Eugene V. Rozanov, Johannes Staehelin, Fiona Tummon, Anne K. Smith, Timofei Sukhodolov, Andrea Stenke, Laura Revell, Ancelin Coulon, Werner Schmutz, and Thomas Peter
Atmos. Chem. Phys., 16, 15485–15500, https://doi.org/10.5194/acp-16-15485-2016, https://doi.org/10.5194/acp-16-15485-2016, 2016
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We find monthly, mid-latitude temperature changes above 40 km are related to ozone and temperature variations throughout the middle atmosphere. We develop an index to represent this atmospheric variability. In statistical analysis, the index can account for up to 60 % of variability in tropical temperature and ozone above 27 km. The uncertainties can be reduced by up to 35 % and 20 % in temperature and ozone, respectively. This index is an important tool to quantify current and future ozone recovery.
Laura E. Revell, Andrea Stenke, Eugene Rozanov, William Ball, Stefan Lossow, and Thomas Peter
Atmos. Chem. Phys., 16, 13067–13080, https://doi.org/10.5194/acp-16-13067-2016, https://doi.org/10.5194/acp-16-13067-2016, 2016
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Water vapour in the stratosphere plays an important role in atmospheric chemistry and the Earth's radiative balance. We have analysed trends in stratospheric water vapour through the 21st century as simulated by a coupled chemistry–climate model following a range of greenhouse gas emission scenarios. We have also quantified the contribution that methane oxidation in the stratosphere makes to projected water vapour trends.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
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Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Lukas Kaufmann, Claudia Marcolli, Julian Hofer, Valeria Pinti, Christopher R. Hoyle, and Thomas Peter
Atmos. Chem. Phys., 16, 11177–11206, https://doi.org/10.5194/acp-16-11177-2016, https://doi.org/10.5194/acp-16-11177-2016, 2016
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We investigated dust samples from dust source regions all over the globe with respect to their ice nucleation activity and their mineralogical composition. Stones of reference minerals were milled and investigated the same way as the natural dust samples. We found that the mineralogical composition is a major determinant of ice nucleation ability. Natural samples consist of mixtures of minerals with remarkably similar ice nucleation ability.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
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The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
Claudia Marcolli, Baban Nagare, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8915–8937, https://doi.org/10.5194/acp-16-8915-2016, https://doi.org/10.5194/acp-16-8915-2016, 2016
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Silver iodide is one of the best-investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Nevertheless, many open questions remain. This paper gives an overview of silver iodide as an ice nucleus and tries to identify the factors that influence the ice nucleation ability of silver iodide.
Lindsay Renbaum-Wolff, Mijung Song, Claudia Marcolli, Yue Zhang, Pengfei F. Liu, James W. Grayson, Franz M. Geiger, Scot T. Martin, and Allan K. Bertram
Atmos. Chem. Phys., 16, 7969–7979, https://doi.org/10.5194/acp-16-7969-2016, https://doi.org/10.5194/acp-16-7969-2016, 2016
Erika Kienast-Sjögren, Christian Rolf, Patric Seifert, Ulrich K. Krieger, Bei P. Luo, Martina Krämer, and Thomas Peter
Atmos. Chem. Phys., 16, 7605–7621, https://doi.org/10.5194/acp-16-7605-2016, https://doi.org/10.5194/acp-16-7605-2016, 2016
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We present a climatology of mid-latitude cirrus cloud properties based on 13 000 hours of automatically analyzed lidar measurements at three different sites. Jungfraujoch,
situated at 3580 m a.s.l., is found to be ideal to measure high and optically thin
cirrus. We use our retrieved optical properties together with a radiation model and
estimate the radiative forcing by mid-latitude cirrus.
All cirrus clouds detected here have a positive net radiative effect.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
B. Nagare, C. Marcolli, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 15, 13759–13776, https://doi.org/10.5194/acp-15-13759-2015, https://doi.org/10.5194/acp-15-13759-2015, 2015
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We determined collision efficiencies of cloud droplets with aerosol particles experimentally and found that they were around 1 order of magnitude higher than theoretical formulations that include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This is most probably due to uncertainties and inaccuracies in the theoretical formulations of thermophoretic and diffusiophoretic processes.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
J.-X. Sheng, D. K. Weisenstein, B.-P. Luo, E. Rozanov, F. Arfeuille, and T. Peter
Atmos. Chem. Phys., 15, 11501–11512, https://doi.org/10.5194/acp-15-11501-2015, https://doi.org/10.5194/acp-15-11501-2015, 2015
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We have conducted a perturbed parameter model ensemble to investigate Mt.
Pinatubo's 1991 initial sulfur mass emission. Our results suggest that (a) the initial mass loading of the Pinatubo eruption is ~14 Mt of SO2; (b) the injection vertical distribution is strongly skewed towards the lower stratosphere, leading to a peak mass sulfur injection at 18-21 km; (c) the injection magnitude and height affect early southward transport of the volcanic cloud observed by SAGE II.
E. Hammer, N. Bukowiecki, B. P. Luo, U. Lohmann, C. Marcolli, E. Weingartner, U. Baltensperger, and C. R. Hoyle
Atmos. Chem. Phys., 15, 10309–10323, https://doi.org/10.5194/acp-15-10309-2015, https://doi.org/10.5194/acp-15-10309-2015, 2015
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An important quantity which determines aerosol activation and cloud formation is the effective peak supersaturation. The box model ZOMM was used to simulate the effective peak supersaturation experienced by an air parcel approaching a high-alpine research station in Switzerland. With the box model the sensitivity of the effective peak supersaturation to key aerosol and dynamical parameters was investigated.
E. Kienast-Sjögren, A. K. Miltenberger, B. P. Luo, and T. Peter
Atmos. Chem. Phys., 15, 7429–7447, https://doi.org/10.5194/acp-15-7429-2015, https://doi.org/10.5194/acp-15-7429-2015, 2015
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Sensitivities of Lagrangian cirrus modelling on input data uncertainties have been examined. We found a strong dependence on the temporal resolution of the trajectories and underlying numerical weather prediction (NWP) data as well as on the specific moisture content. Furthermore, we found a large day-to-day variability in the vertical wind spectrum, demonstrating the necessity to apply NWP models with high spatial and temporal resolution for Lagrangian cirrus modelling.
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
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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.
L. E. Revell, F. Tummon, A. Stenke, T. Sukhodolov, A. Coulon, E. Rozanov, H. Garny, V. Grewe, and T. Peter
Atmos. Chem. Phys., 15, 5887–5902, https://doi.org/10.5194/acp-15-5887-2015, https://doi.org/10.5194/acp-15-5887-2015, 2015
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We have examined the effects of ozone precursor emissions and climate change on the tropospheric ozone budget. Under RCP 6.0, ozone in the future is governed primarily by changes in nitrogen oxides (NOx). Methane is also important, and induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. This study highlights the critical role that emission policies globally have to play in determining tropospheric ozone evolution through the 21st century.
N. Hodas, A. Zuend, W. Mui, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 5027–5045, https://doi.org/10.5194/acp-15-5027-2015, https://doi.org/10.5194/acp-15-5027-2015, 2015
G. Ganbavale, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 15, 447–493, https://doi.org/10.5194/acp-15-447-2015, https://doi.org/10.5194/acp-15-447-2015, 2015
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This study presents a new, improved parameterisation of the temperature dependence of activity coefficients implemented in the AIOMFAC group-contribution model. The AIOMFAC model with the improved parameterisation is applicable for a large variety of aqueous organic as well as water-free organic solutions of relevance for atmospheric aerosols. The new model parameters were determined based on published and new thermodynamic equilibrium data covering a temperature range from ~190 to 440 K.
T. Sukhodolov, E. Rozanov, A. I. Shapiro, J. Anet, C. Cagnazzo, T. Peter, and W. Schmutz
Geosci. Model Dev., 7, 2859–2866, https://doi.org/10.5194/gmd-7-2859-2014, https://doi.org/10.5194/gmd-7-2859-2014, 2014
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The performance of the main generations of the ECHAM shortwave radiation schemes is analysed in terms of the representation of the solar signal in the heating rates. The way to correct missing or underrepresented spectral intervals in the solar signal in the heating rates is suggested using the example of ECHAM6 and six-band ECHAM5 schemes. The suggested method is computationally fast and suitable for any other radiation scheme.
S. Pandey Deolal, S. Henne, L. Ries, S. Gilge, U. Weers, M. Steinbacher, J. Staehelin, and T. Peter
Atmos. Chem. Phys., 14, 12553–12571, https://doi.org/10.5194/acp-14-12553-2014, https://doi.org/10.5194/acp-14-12553-2014, 2014
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Mixing ratios of Peroxyacetyl nitrate (PAN) at Jungfraujoch (Switzerland) and Zugspitze (Germany) show a seasonal variation with maxima in spring, typical for remote sites in the lower atmosphere in northern mid-latitudes. The detailed analysis of PAN measurements of May 2008 indicates that PAN at these high mountain sites is dominated by photochemical formation in the relatively cold polluted European planetary boundary layer rather than formation in the free troposphere.
T. Lei, A. Zuend, W. G. Wang, Y. H. Zhang, and M. F. Ge
Atmos. Chem. Phys., 14, 11165–11183, https://doi.org/10.5194/acp-14-11165-2014, https://doi.org/10.5194/acp-14-11165-2014, 2014
S. Molleker, S. Borrmann, H. Schlager, B. Luo, W. Frey, M. Klingebiel, R. Weigel, M. Ebert, V. Mitev, R. Matthey, W. Woiwode, H. Oelhaf, A. Dörnbrack, G. Stratmann, J.-U. Grooß, G. Günther, B. Vogel, R. Müller, M. Krämer, J. Meyer, and F. Cairo
Atmos. Chem. Phys., 14, 10785–10801, https://doi.org/10.5194/acp-14-10785-2014, https://doi.org/10.5194/acp-14-10785-2014, 2014
D. W. Fahey, R.-S. Gao, O. Möhler, H. Saathoff, C. Schiller, V. Ebert, M. Krämer, T. Peter, N. Amarouche, L. M. Avallone, R. Bauer, Z. Bozóki, L. E. Christensen, S. M. Davis, G. Durry, C. Dyroff, R. L. Herman, S. Hunsmann, S. M. Khaykin, P. Mackrodt, J. Meyer, J. B. Smith, N. Spelten, R. F. Troy, H. Vömel, S. Wagner, and F. G. Wienhold
Atmos. Meas. Tech., 7, 3177–3213, https://doi.org/10.5194/amt-7-3177-2014, https://doi.org/10.5194/amt-7-3177-2014, 2014
S. Muthers, J. G. Anet, A. Stenke, C. C. Raible, E. Rozanov, S. Brönnimann, T. Peter, F. X. Arfeuille, A. I. Shapiro, J. Beer, F. Steinhilber, Y. Brugnara, and W. Schmutz
Geosci. Model Dev., 7, 2157–2179, https://doi.org/10.5194/gmd-7-2157-2014, https://doi.org/10.5194/gmd-7-2157-2014, 2014
A. Cirisan, B. P. Luo, I. Engel, F. G. Wienhold, M. Sprenger, U. K. Krieger, U. Weers, G. Romanens, G. Levrat, P. Jeannet, D. Ruffieux, R. Philipona, B. Calpini, P. Spichtinger, and T. Peter
Atmos. Chem. Phys., 14, 7341–7365, https://doi.org/10.5194/acp-14-7341-2014, https://doi.org/10.5194/acp-14-7341-2014, 2014
I. Suter, R. Zech, J. G. Anet, and T. Peter
Clim. Past, 10, 1183–1194, https://doi.org/10.5194/cp-10-1183-2014, https://doi.org/10.5194/cp-10-1183-2014, 2014
J. G. Anet, S. Muthers, E. V. Rozanov, C. C. Raible, A. Stenke, A. I. Shapiro, S. Brönnimann, F. Arfeuille, Y. Brugnara, J. Beer, F. Steinhilber, W. Schmutz, and T. Peter
Clim. Past, 10, 921–938, https://doi.org/10.5194/cp-10-921-2014, https://doi.org/10.5194/cp-10-921-2014, 2014
I. Engel, B. P. Luo, S. M. Khaykin, F. G. Wienhold, H. Vömel, R. Kivi, C. R. Hoyle, J.-U. Grooß, M. C. Pitts, and T. Peter
Atmos. Chem. Phys., 14, 3231–3246, https://doi.org/10.5194/acp-14-3231-2014, https://doi.org/10.5194/acp-14-3231-2014, 2014
C. Marcolli
Atmos. Chem. Phys., 14, 2071–2104, https://doi.org/10.5194/acp-14-2071-2014, https://doi.org/10.5194/acp-14-2071-2014, 2014
F. Arfeuille, D. Weisenstein, H. Mack, E. Rozanov, T. Peter, and S. Brönnimann
Clim. Past, 10, 359–375, https://doi.org/10.5194/cp-10-359-2014, https://doi.org/10.5194/cp-10-359-2014, 2014
J.-U. Grooß, I. Engel, S. Borrmann, W. Frey, G. Günther, C. R. Hoyle, R. Kivi, B. P. Luo, S. Molleker, T. Peter, M. C. Pitts, H. Schlager, G. Stiller, H. Vömel, K. A. Walker, and R. Müller
Atmos. Chem. Phys., 14, 1055–1073, https://doi.org/10.5194/acp-14-1055-2014, https://doi.org/10.5194/acp-14-1055-2014, 2014
J. Staufer, J. Staehelin, R. Stübi, T. Peter, F. Tummon, and V. Thouret
Atmos. Meas. Tech., 7, 241–266, https://doi.org/10.5194/amt-7-241-2014, https://doi.org/10.5194/amt-7-241-2014, 2014
J. Staufer, J. Staehelin, R. Stübi, T. Peter, F. Tummon, and V. Thouret
Atmos. Meas. Tech., 6, 3393–3406, https://doi.org/10.5194/amt-6-3393-2013, https://doi.org/10.5194/amt-6-3393-2013, 2013
S. M. Khaykin, I. Engel, H. Vömel, I. M. Formanyuk, R. Kivi, L. I. Korshunov, M. Krämer, A. D. Lykov, S. Meier, T. Naebert, M. C. Pitts, M. L. Santee, N. Spelten, F. G. Wienhold, V. A. Yushkov, and T. Peter
Atmos. Chem. Phys., 13, 11503–11517, https://doi.org/10.5194/acp-13-11503-2013, https://doi.org/10.5194/acp-13-11503-2013, 2013
F. Arfeuille, B. P. Luo, P. Heckendorn, D. Weisenstein, J. X. Sheng, E. Rozanov, M. Schraner, S. Brönnimann, L. W. Thomason, and T. Peter
Atmos. Chem. Phys., 13, 11221–11234, https://doi.org/10.5194/acp-13-11221-2013, https://doi.org/10.5194/acp-13-11221-2013, 2013
J. G. Anet, S. Muthers, E. Rozanov, C. C. Raible, T. Peter, A. Stenke, A. I. Shapiro, J. Beer, F. Steinhilber, S. Brönnimann, F. Arfeuille, Y. Brugnara, and W. Schmutz
Atmos. Chem. Phys., 13, 10951–10967, https://doi.org/10.5194/acp-13-10951-2013, https://doi.org/10.5194/acp-13-10951-2013, 2013
I. Engel, B. P. Luo, M. C. Pitts, L. R. Poole, C. R. Hoyle, J.-U. Grooß, A. Dörnbrack, and T. Peter
Atmos. Chem. Phys., 13, 10769–10785, https://doi.org/10.5194/acp-13-10769-2013, https://doi.org/10.5194/acp-13-10769-2013, 2013
A. Stenke, C. R. Hoyle, B. Luo, E. Rozanov, J. Gröbner, L. Maag, S. Brönnimann, and T. Peter
Atmos. Chem. Phys., 13, 9713–9729, https://doi.org/10.5194/acp-13-9713-2013, https://doi.org/10.5194/acp-13-9713-2013, 2013
C. R. Hoyle, I. Engel, B. P. Luo, M. C. Pitts, L. R. Poole, J.-U. Grooß, and T. Peter
Atmos. Chem. Phys., 13, 9577–9595, https://doi.org/10.5194/acp-13-9577-2013, https://doi.org/10.5194/acp-13-9577-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
A. Stenke, M. Schraner, E. Rozanov, T. Egorova, B. Luo, and T. Peter
Geosci. Model Dev., 6, 1407–1427, https://doi.org/10.5194/gmd-6-1407-2013, https://doi.org/10.5194/gmd-6-1407-2013, 2013
A. J. Huisman, U. K. Krieger, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 13, 6647–6662, https://doi.org/10.5194/acp-13-6647-2013, https://doi.org/10.5194/acp-13-6647-2013, 2013
F. Hasebe, Y. Inai, M. Shiotani, M. Fujiwara, H. Vömel, N. Nishi, S.-Y. Ogino, T. Shibata, S. Iwasaki, N. Komala, T. Peter, and S. J. Oltmans
Atmos. Chem. Phys., 13, 4393–4411, https://doi.org/10.5194/acp-13-4393-2013, https://doi.org/10.5194/acp-13-4393-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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
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
Characterization of the particle size distribution, mineralogy and Fe mode of occurrence of dust-emitting sediments across the Mojave Desert, California, USA
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
Technical note: Improved synthetic routes to cis- and trans-(2-methyloxirane-2,3-diyl)dimethanol (cis- and trans-β-isoprene epoxydiol)
Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples
Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime
Formation of highly oxygenated organic molecules from the oxidation of limonene by OH radical: significant contribution of H-abstraction pathway
Measurement report: Atmospheric aging of combustion-derived particles – impact on stable free radical concentration and its ability to produce reactive oxygen species in aqueous media
Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants
An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles
Simultaneous formation of sulfate and nitrate via co-uptake of SO2 and NO2 by aqueous NaCl droplets: combined effect of nitrate photolysis and chlorine chemistry
Photo-induced shrinking of aqueous glycine aerosol droplets
Sulfate formation via aerosol-phase SO2 oxidation by model biomass burning photosensitizers: 3,4-dimethoxybenzaldehyde, vanillin and syringaldehyde using single-particle mixing-state analysis
Yields and molecular composition of gas-phase and secondary organic aerosol from the photooxidation of the volatile consumer product benzyl alcohol: formation of highly oxygenated and hydroxy nitro-aromatic compounds
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
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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.
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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-434, https://doi.org/10.5194/egusphere-2024-434, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understand the effect of dust upon climate. We found two different playa lakes according to the groundwater regime which implies differences on crusts cohesion state and its mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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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
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to 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
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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
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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
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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
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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.
Molly Frauenheim, Jason D. Surratt, Zhenfa Zhang, and Avram Gold
Atmos. Chem. Phys., 23, 7859–7866, https://doi.org/10.5194/acp-23-7859-2023, https://doi.org/10.5194/acp-23-7859-2023, 2023
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We report synthesis of the isoprene-derived photochemical oxidation products trans- and cis-β-epoxydiols in high overall yields from inexpensive, readily available starting compounds. Protection/deprotection steps or time-consuming purification is not required, and the reactions can be scaled up to gram quantities. The procedures provide accessibility of these important compounds to atmospheric chemistry laboratories with only basic capabilities in organic synthesis.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
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The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Hao Luo, Luc Vereecken, Hongru Shen, Sungah Kang, Iida Pullinen, Mattias Hallquist, Hendrik Fuchs, Andreas Wahner, Astrid Kiendler-Scharr, Thomas F. Mentel, and Defeng Zhao
Atmos. Chem. Phys., 23, 7297–7319, https://doi.org/10.5194/acp-23-7297-2023, https://doi.org/10.5194/acp-23-7297-2023, 2023
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Oxidation of limonene, an element emitted by trees and chemical products, by OH, a daytime oxidant, forms many highly oxygenated organic molecules (HOMs), including C10-20 compounds. HOMs play an important role in new particle formation and growth. HOM formation can be explained by the chemistry of peroxy radicals. We found that a minor branching ratio initial pathway plays an unexpected, significant role. Considering this pathway enables accurate simulations of HOMs and other concentrations.
Heather L. Runberg and Brian J. Majestic
Atmos. Chem. Phys., 23, 7213–7223, https://doi.org/10.5194/acp-23-7213-2023, https://doi.org/10.5194/acp-23-7213-2023, 2023
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Environmentally persistent free radicals (EPFRs) are an emerging pollutant found in soot particles. Understanding how these change as they move through the atmosphere is important to human health. Here, soot was generated in the laboratory and exposed to simulated sunlight. The concentrations and characteristics of EPFRs in the soot were measured and found to be unchanged. However, it was also found that the ability of soot to form hydroxyl radicals was stronger for fresh soot.
Wenqing Jiang, Christopher Niedek, Cort Anastasio, and Qi Zhang
Atmos. Chem. Phys., 23, 7103–7120, https://doi.org/10.5194/acp-23-7103-2023, https://doi.org/10.5194/acp-23-7103-2023, 2023
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We studied how aqueous-phase secondary organic aerosol (aqSOA) form and evolve from a phenolic carbonyl commonly present in biomass burning smoke. The composition and optical properties of the aqSOA are significantly affected by photochemical reactions and are dependent on the oxidants' concentration and identity in water. During photoaging, the aqSOA initially becomes darker, but prolonged aging leads to the formation of volatile products, resulting in significant mass loss and photobleaching.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Ruifeng Zhang and Chak Keung Chan
Atmos. Chem. Phys., 23, 6113–6126, https://doi.org/10.5194/acp-23-6113-2023, https://doi.org/10.5194/acp-23-6113-2023, 2023
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Research into sulfate and nitrate formation from co-uptake of NO2 and SO2, especially under irradiation, is rare. We studied the co-uptake of NO2 and SO2 by NaCl droplets under various conditions, including irradiation and dark, and RHs, using Raman spectroscopy flow cell and kinetic model simulation. Significant nitrate formation from NO2 hydrolysis can be photolyzed to generate OH radicals that can further react with chloride to produce reactive chlorine species and promote sulfate formation.
Shinnosuke Ishizuka, Oliver Reich, Grégory David, and Ruth Signorell
Atmos. Chem. Phys., 23, 5393–5402, https://doi.org/10.5194/acp-23-5393-2023, https://doi.org/10.5194/acp-23-5393-2023, 2023
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Photosensitizers play an important role in the photochemistry of atmospheric aerosols. Our study provides evidence that mesoscopic glycine clusters forming in aqueous droplets act as unconventional photosensitizers in the visible light spectrum. We observed the influence of these photoactive molecular aggregates in single optically trapped aqueous droplets. Such mesoscopic photosensitizers might be more important for aerosol photochemistry than previously anticipated.
Liyuan Zhou, Zhancong Liang, Beatrix Rosette Go Mabato, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, and Chak K. Chan
Atmos. Chem. Phys., 23, 5251–5261, https://doi.org/10.5194/acp-23-5251-2023, https://doi.org/10.5194/acp-23-5251-2023, 2023
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This study reveals the sulfate formation in photosensitized particles from biomass burning under UV and SO2, of which the relative atmospheric importance in sulfate production was qualitatively compared to nitrate photolysis. On the basis of single-particle aerosol mass spectrometry measurements, the number percentage of sulfate-containing particles and relative peak area of sulfate in single-particle spectra exhibited a descending order of 3,4-dimethoxybenzaldehyde > vanillin > syringaldehyde.
Mohammed Jaoui, Kenneth S. Docherty, Michael Lewandowski, and Tadeusz E. Kleindienst
Atmos. Chem. Phys., 23, 4637–4661, https://doi.org/10.5194/acp-23-4637-2023, https://doi.org/10.5194/acp-23-4637-2023, 2023
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VCPs are a class of chemicals widely used in industrial and consumer products (e.g., coatings, adhesives, inks, personal care products) and are an important component of total VOCs in urban atmospheres. This study provides SOA yields and detailed chemical analysis of the gas- and aerosol-phase products of the photooxidation of one of these VCPs, benzyl alcohol. These results will allow better links between characterized sources and their resulting criteria for pollutant formation.
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