Articles | Volume 15, issue 15
https://doi.org/10.5194/acp-15-8975-2015
© Author(s) 2015. 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-15-8975-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
13 Aug 2015
Research article |
| 13 Aug 2015
Hygroscopic and phase separation properties of ammonium sulfate/organics/water ternary solutions
M. A. Zawadowicz
Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
S. R. Proud
Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
University of Copenhagen, Copenhagen, Denmark
S. S. Seppalainen
Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
D. J. Cziczo
CORRESPONDING AUTHOR
Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
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Paul A. Barrett, Steven J. Abel, Hugh Coe, Ian Crawford, Amie Dobracki, James Haywood, Steve Howell, Anthony Jones, Justin Langridge, Greg M. McFarquhar, Graeme J. Nott, Hannah Price, Jens Redemann, Yohei Shinozuka, Kate Szpek, Jonathan W. Taylor, Robert Wood, Huihui Wu, Paquita Zuidema, Stéphane Bauguitte, Ryan Bennett, Keith Bower, Hong Chen, Sabrina Cochrane, Michael Cotterell, Nicholas Davies, David Delene, Connor Flynn, Andrew Freedman, Steffen Freitag, Siddhant Gupta, David Noone, Timothy B. Onasch, James Podolske, Michael R. Poellot, Sebastian Schmidt, Stephen Springston, Arthur J. Sedlacek III, Jamie Trembath, Alan Vance, Maria A. Zawadowicz, and Jianhao Zhang
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Fabian Mahrt, Carolin Rösch, Kunfeng Gao, Christopher H. Dreimol, Maria A. Zawadowicz, and Zamin A. Kanji
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Paul A. Barrett, Steven J. Abel, Hugh Coe, Ian Crawford, Amie Dobracki, James Haywood, Steve Howell, Anthony Jones, Justin Langridge, Greg M. McFarquhar, Graeme J. Nott, Hannah Price, Jens Redemann, Yohei Shinozuka, Kate Szpek, Jonathan W. Taylor, Robert Wood, Huihui Wu, Paquita Zuidema, Stéphane Bauguitte, Ryan Bennett, Keith Bower, Hong Chen, Sabrina Cochrane, Michael Cotterell, Nicholas Davies, David Delene, Connor Flynn, Andrew Freedman, Steffen Freitag, Siddhant Gupta, David Noone, Timothy B. Onasch, James Podolske, Michael R. Poellot, Sebastian Schmidt, Stephen Springston, Arthur J. Sedlacek III, Jamie Trembath, Alan Vance, Maria A. Zawadowicz, and Jianhao Zhang
Atmos. Meas. Tech., 15, 6329–6371, https://doi.org/10.5194/amt-15-6329-2022, https://doi.org/10.5194/amt-15-6329-2022, 2022
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To better understand weather and climate, it is vital to go into the field and collect observations. Often measurements take place in isolation, but here we compared data from two aircraft and one ground-based site. This was done in order to understand how well measurements made on one platform compared to those made on another. Whilst this is easy to do in a controlled laboratory setting, it is more challenging in the real world, and so these comparisons are as valuable as they are rare.
Libby Koolik, Michael Roesch, Carmen Dameto de Espana, Christopher Nathan Rapp, Lesly J. Franco Deloya, Chuanyang Shen, A. Gannet Hallar, Ian B. McCubbin, and Daniel J. Cziczo
Atmos. Meas. Tech., 15, 3213–3222, https://doi.org/10.5194/amt-15-3213-2022, https://doi.org/10.5194/amt-15-3213-2022, 2022
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A new inlet for studying the small particles, droplets, and ice crystals that constitute mixed-phase clouds has been constructed and is described here. This new inlet was tested in the laboratory. We present the performance of the new inlet to demonstrate its capability of separating ice, droplets, and small particles.
Shuaiqi Tang, Jerome D. Fast, Kai Zhang, Joseph C. Hardin, Adam C. Varble, John E. Shilling, Fan Mei, Maria A. Zawadowicz, and Po-Lun Ma
Geosci. Model Dev., 15, 4055–4076, https://doi.org/10.5194/gmd-15-4055-2022, https://doi.org/10.5194/gmd-15-4055-2022, 2022
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We developed an Earth system model (ESM) diagnostics package to compare various types of aerosol properties simulated in ESMs with aircraft, ship, and surface measurements from six field campaigns across spatial scales. The diagnostics package is coded and organized to be flexible and modular for future extension to other field campaign datasets and adapted to higher-resolution model simulations. Future releases will include comprehensive cloud and aerosol–cloud interaction diagnostics.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
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Maria A. Zawadowicz, Kaitlyn Suski, Jiumeng Liu, Mikhail Pekour, Jerome Fast, Fan Mei, Arthur J. Sedlacek, Stephen Springston, Yang Wang, Rahul A. Zaveri, Robert Wood, Jian Wang, and John E. Shilling
Atmos. Chem. Phys., 21, 7983–8002, https://doi.org/10.5194/acp-21-7983-2021, https://doi.org/10.5194/acp-21-7983-2021, 2021
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This paper describes the results of a recent field campaign in the eastern North Atlantic, where two mass spectrometers were deployed aboard a research aircraft to measure the chemistry of aerosols and trace gases. Very clean conditions were found, dominated by local sulfate-rich acidic aerosol and very aged organics. Evidence of
long-range transport of aerosols from the continents was also identified.
Michael Rösch and Daniel J. Cziczo
Atmos. Meas. Tech., 13, 6807–6812, https://doi.org/10.5194/amt-13-6807-2020, https://doi.org/10.5194/amt-13-6807-2020, 2020
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The need for a simple atomizer with a high-output stability combined with the capabilities of CAD software and high-resolution 3D printing has allowed for the design, production and testing of the PRinted drOpleT Generator (PROTeGE) to generate liquid particles from solutions. The size and number concentrations of the generated particles have been characterized with different ammonium sulfate and PSL solutions. PROTeGE is easy to operate, requires minimal maintenance and is cost-effective.
Martin J. Wolf, Megan Goodell, Eric Dong, Lilian A. Dove, Cuiqi Zhang, Lesly J. Franco, Chuanyang Shen, Emma G. Rutkowski, Domenic N. Narducci, Susan Mullen, Andrew R. Babbin, and Daniel J. Cziczo
Atmos. Chem. Phys., 20, 15341–15356, https://doi.org/10.5194/acp-20-15341-2020, https://doi.org/10.5194/acp-20-15341-2020, 2020
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Sea spray is the largest aerosol source on Earth. These aerosol particles can impact climate by inducing ice formation in clouds. The role that ocean biology plays in determining the composition and ice nucleation abilities of sea spray aerosol is unclarified. In this study, we demonstrate that atomized seawater from highly productive ocean regions is more effective at nucleating ice than seawater from lower-productivity regions.
Gourihar Kulkarni, Naruki Hiranuma, Ottmar Möhler, Kristina Höhler, Swarup China, Daniel J. Cziczo, and Paul J. DeMott
Atmos. Meas. Tech., 13, 6631–6643, https://doi.org/10.5194/amt-13-6631-2020, https://doi.org/10.5194/amt-13-6631-2020, 2020
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This study presents a new continuous-flow-diffusion-chamber-style operated ice chamber (Modified Compact Ice Chamber, MCIC) to measure the immersion-freezing efficiency of atmospheric particles. MCIC allowed us to obtain maximum droplet-freezing efficiency at higher time resolution without droplet breakthrough ambiguity. Its evaluation was performed by reproducing published data from the recent ice nucleation workshop and past laboratory data for standard and airborne ice-nucleating particles.
Cuiqi Zhang, Yue Zhang, Martin J. Wolf, Leonid Nichman, Chuanyang Shen, Timothy B. Onasch, Longfei Chen, and Daniel J. Cziczo
Atmos. Chem. Phys., 20, 13957–13984, https://doi.org/10.5194/acp-20-13957-2020, https://doi.org/10.5194/acp-20-13957-2020, 2020
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Black carbon (BC) is considered the second most important global warming agent. However, the role of BC aerosol–cloud–climate interactions in the cirrus formation remains uncertain. Our study of selected BC types and sizes suggests that increases in diameter, compactness, and/or surface oxidation of BC particles lead to more efficient ice nucleation (IN) via pore condensation freezing (PCF) pathways，and that coatings of common secondary organic aerosol (SOA) materials can inhibit ice formation.
Libby Koolik, Michael Roesch, Lesly J. Franco Deloya, Chuanyang Shen, A. Gannet Hallar, Ian B. McCubbin, and Daniel J. Cziczo
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-42, https://doi.org/10.5194/amt-2020-42, 2020
Revised manuscript not accepted
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The phaSe seParation Inlet for Droplets icE residuals and inteRstitial aerosols (SPIDER) combines an omni-directional inlet, a Large-Pumped Counterflow Virtual Impactor, a flow tube evaporation chamber, and a Pumped Counterflow Virtual Impactor to separate droplets, ice crystals, and interstitial aerosols for simultaneous sampling. This new inlet for studying mixed-phase clouds is described here, with laboratory verification tests and a deployment at a mountain-top research facility.
Maria A. Zawadowicz, Karl D. Froyd, Anne E. Perring, Daniel M. Murphy, Dominick V. Spracklen, Colette L. Heald, Peter R. Buseck, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 13859–13870, https://doi.org/10.5194/acp-19-13859-2019, https://doi.org/10.5194/acp-19-13859-2019, 2019
Short summary
Short summary
We report measurements of small particles of biological origin (for example, fragments of bacteria, pollen, or fungal spores) in the atmosphere over the continental United States. We use a recently developed identification technique based on airborne mass spectrometry in conjunction with an extensive aircraft dataset. We show that biological particles are present at altitudes up to 10 km and we quantify typical concentrations.
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Nsikanabasi Silas Umo, Robert Wagner, Romy Ullrich, Alexei Kiselev, Harald Saathoff, Peter G. Weidler, Daniel J. Cziczo, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 19, 8783–8800, https://doi.org/10.5194/acp-19-8783-2019, https://doi.org/10.5194/acp-19-8783-2019, 2019
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Annually, over 600 Tg of coal fly ash (CFA) is produced; a significant proportion of this amount is injected into the atmosphere, which could significantly contribute to heterogeneous ice formation in clouds. This study presents an improved understanding of CFA particles' behaviour in forming ice in clouds, especially when exposed to lower temperatures before being re-circulated in the upper troposphere or entrained into the lower troposphere.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Costa D. Christopoulos, Sarvesh Garimella, Maria A. Zawadowicz, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Meas. Tech., 11, 5687–5699, https://doi.org/10.5194/amt-11-5687-2018, https://doi.org/10.5194/amt-11-5687-2018, 2018
Short summary
Short summary
Compositional analysis of atmospheric and laboratory aerosols is often conducted with mass spectrometry. In this study, machine learning is used to automatically differentiate particles on the basis of chemistry and size. The ability of the machine learning algorithm was then tested on a data set for which the particles were not initially known to judge its ability.
Matthew Osman, Maria A. Zawadowicz, Sarah B. Das, and Daniel J. Cziczo
Atmos. Meas. Tech., 10, 4459–4477, https://doi.org/10.5194/amt-10-4459-2017, https://doi.org/10.5194/amt-10-4459-2017, 2017
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This study presents the first-time attempt at using time-of-flight single particle mass spectrometry (SPMS) as an emerging online technique for measuring insoluble particles in glacial snow and ice. Using samples from two Greenlandic ice cores, we show that SPMS can constrain the aerodynamic size, composition, and relative abundance of most particulate types on a per-particle basis, reducing the preparation time and resources required of conventional, filter-based particle retrieval methods.
Sarvesh Garimella, Daniel A. Rothenberg, Martin J. Wolf, Robert O. David, Zamin A. Kanji, Chien Wang, Michael Rösch, and Daniel J. Cziczo
Atmos. Chem. Phys., 17, 10855–10864, https://doi.org/10.5194/acp-17-10855-2017, https://doi.org/10.5194/acp-17-10855-2017, 2017
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This study investigates systematic and variable low bias in the measurement of ice nucleating particle concentration using continuous flow diffusion chambers. We find that non-ideal instrument behavior exposes particles to different humidities and/or temperatures than predicted from theory. We use a machine learning approach to quantify and minimize the uncertainty associated with this measurement bias.
Maria A. Zawadowicz, Karl D. Froyd, Daniel M. Murphy, and Daniel J. Cziczo
Atmos. Chem. Phys., 17, 7193–7212, https://doi.org/10.5194/acp-17-7193-2017, https://doi.org/10.5194/acp-17-7193-2017, 2017
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This paper reports the results of laboratory and field measurements of primary biological aerosol particles using single-particle mass spectrometry (SPMS). Identification of biological particles using SPMS can be challenging, as their mass spectra can present features similar to phosphorus-containing minerals and combustion by-products. Using a large database of laboratory measurements, a criterion for the identification of biological particles has been developed.
Michael Roesch, Carolin Roesch, and Daniel J. Cziczo
Atmos. Meas. Tech., 10, 1999–2007, https://doi.org/10.5194/amt-10-1999-2017, https://doi.org/10.5194/amt-10-1999-2017, 2017
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This study describes the design, manufacture and proof-of-concept of the 3-D printed fluidized bed generator PRIZE, which is a compact, simple and low-cost addition to existing dry particle generation instruments. The generator is capable of dispersing aerosol particles from dry material without itself generating significant particles (< 5 % by number at 0.2 g of ATD without a stainless steel insert, negligible with). It is therefore ideal for use in minimally appointed lab and field conditions.
Naruki Hiranuma, Ottmar Möhler, Gourihar Kulkarni, Martin Schnaiter, Steffen Vogt, Paul Vochezer, Emma Järvinen, Robert Wagner, David M. Bell, Jacqueline Wilson, Alla Zelenyuk, and Daniel J. Cziczo
Atmos. Meas. Tech., 9, 3817–3836, https://doi.org/10.5194/amt-9-3817-2016, https://doi.org/10.5194/amt-9-3817-2016, 2016
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A new pumped counterflow virtual impactor (PCVI) called the ice-selecting PCVI (IS-PCVI) has been developed to collect ice crystal residuals for investigating physico-chemical properties of ice-nucleating particles. The results show that the ice crystals of volume-equivalent diameter ~ 10 to 30 µm can be efficiently separated from the supercooled droplets and interstitial particles. The IS-PCVI is efficient when the counterflow-to-input flow ratio is within 0.09 to 0.18.
Sarvesh Garimella, Thomas Bjerring Kristensen, Karolina Ignatius, Andre Welti, Jens Voigtländer, Gourihar R. Kulkarni, Frank Sagan, Gregory Lee Kok, James Dorsey, Leonid Nichman, Daniel Alexander Rothenberg, Michael Rösch, Amélie Catharina Ruth Kirchgäßner, Russell Ladkin, Heike Wex, Theodore W. Wilson, Luis Antonio Ladino, Jon P. D. Abbatt, Olaf Stetzer, Ulrike Lohmann, Frank Stratmann, and Daniel James Cziczo
Atmos. Meas. Tech., 9, 2781–2795, https://doi.org/10.5194/amt-9-2781-2016, https://doi.org/10.5194/amt-9-2781-2016, 2016
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The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nuclei counter manufactured by Droplet Measurement Technologies in Boulder, CO. This study characterizes the SPIN chamber, reporting data from laboratory measurements and quantifying uncertainties. Overall, we report that the SPIN is able to reproduce previous CFDC ice nucleation measurements.
K. Ardon-Dryer, Y.-W. Huang, and D. J. Cziczo
Atmos. Chem. Phys., 15, 9159–9171, https://doi.org/10.5194/acp-15-9159-2015, https://doi.org/10.5194/acp-15-9159-2015, 2015
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The collection between aerosol and a water droplet is an important mechanism for removing particles from the atmosphere, and has an influence on cloud dynamics, precipitation processes and cloud lifetime. In this experiment, the collection process was studied on a single-droplet basis, with atmospherically relevant conditions (droplet sizes, charges and flow). Collection efficiency values were found to be in agreement with previous experimental and theoretical studies.
D. B. Atkinson, J. G. Radney, J. Lum, K. R. Kolesar, D. J. Cziczo, M. S. Pekour, Q. Zhang, A. Setyan, A. Zelenyuk, and C. D. Cappa
Atmos. Chem. Phys., 15, 4045–4061, https://doi.org/10.5194/acp-15-4045-2015, https://doi.org/10.5194/acp-15-4045-2015, 2015
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This work describes an analysis of measurements of the influence of water uptake on the light-scattering properties of sub- and supermicron-sized particles as observed in the Sacramento, CA, USA region during the 2010 CARES field campaign. The observations are used to derive campaign-average effective hygroscopicity parameters for submicron oxygenated organic aerosol and for supermicron particles, and the influence of chloride displacement reactions on particle hygroscopicity is examined.
S. Garimella, Y.-W. Huang, J. S. Seewald, and D. J. Cziczo
Atmos. Chem. Phys., 14, 6003–6019, https://doi.org/10.5194/acp-14-6003-2014, https://doi.org/10.5194/acp-14-6003-2014, 2014
B. Friedman, A. Zelenyuk, J. Beranek, G. Kulkarni, M. Pekour, A. Gannet Hallar, I. B. McCubbin, J. A. Thornton, and D. J Cziczo
Atmos. Chem. Phys., 13, 11839–11851, https://doi.org/10.5194/acp-13-11839-2013, https://doi.org/10.5194/acp-13-11839-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Probing Iceland's Dust-Emitting Sediments: Particle Size Distribution, Mineralogy, Cohesion, Fe Mode of Occurrence, and Reflectance Spectra Signatures
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
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
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
Comparison of water-soluble and insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Molecular fingerprints and health risks of smoke from home-use incense burning
Photoenhanced sulfates formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
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
A combined gas- and particle-phase analysis of highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis
Comparison of aqueous secondary organic aerosol (aqSOA) product distributions from guaiacol oxidation by non-phenolic and phenolic methoxybenzaldehydes as photosensitizers in the absence and presence of ammonium nitrate
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.
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.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-157, https://doi.org/10.5194/egusphere-2024-157, 2024
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The knowledge of properties from dust emitted in high latitudes as Iceland (HLD) 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 threefold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
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.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
EGUsphere, https://doi.org/10.5194/egusphere-2023-2657, https://doi.org/10.5194/egusphere-2023-2657, 2023
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Cooking is one of the major particle sources in urban areas. Previous laboratory studies demonstrated the chemical lifetimes of cooking organic aerosols 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.
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.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
EGUsphere, https://doi.org/10.5194/egusphere-2023-2417, https://doi.org/10.5194/egusphere-2023-2417, 2023
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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 was the major source of BrC were characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coals. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, such information could be used for source appointment.
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.
Chong Han, Jiawei Ma, Wangjin Yang, and Hongxing Yang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1273, https://doi.org/10.5194/egusphere-2023-1273, 2023
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We provide direct evidences that light prominently enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where 3SO2 can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. It is suggested that the SO2 photochemistry on non-photoactive mineral dust significantly contributes to sulfates, highlighting previously unknown pathway to better explain the missing sources of atmospheric sulfates.
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.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Beatrix Rosette Go Mabato, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak K. Chan
Atmos. Chem. Phys., 23, 2859–2875, https://doi.org/10.5194/acp-23-2859-2023, https://doi.org/10.5194/acp-23-2859-2023, 2023
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We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud and fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings are useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA predictive models.
Cited articles
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Braban, C. F. and Abbatt, J. P. D.: A study of the phase transition behavior of internally mixed ammonium sulfate – malonic acid aerosols, Atmos. Chem. Phys., 4, 1451–1459, https://doi.org/10.5194/acp-4-1451-2004, 2004.
Braban, C. F., Abbatt, J. P. D., and Cziczo, D. J.: Deliquescence of Ammonium Sulfate Particles at Sub-Eutectic Temperatures, Geophys. Res. Lett., 28, 3879–3882, 2001.
Braban, C. F., Carroll, M. F., Styler, S. A., and Abbatt, J. P. D.: Phase transitions of malonic and oxalic acid aerosols, J. Phys. Chem. A, 107, 6594–6602, 2003.
Buajarern, J., Mitchem, L., and Reid, J. P.: Characterizing multiphase organic/inorganic/aqueous aerosol droplets, J. Phys. Chem. A, 111, 9054–9061, 2007.
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Weers, U., and Peter, T.: Liquid-liquid phase separation in mixed organic/inorganic aerosol particles, J. Phys. Chem. A, 113, 10966–10978, 2009.
Clegg, S. L., Seinfeld, J. H., and Brimblecombe, P.: Thermodynamic modeling of aqueous aerosols containing electrolytes and dissolved organic compounds, J. Aerosol Sci., 32, 713–738, 2001.
Cruz, C. N. and Pandis, S. N.: The effect of organic coatings on the cloud condensation nuclei activation of inorganic atmospheric aerosol, J. Geophys. Res., 103, 13111–13123, 1998.
Cruz, C. N. and Pandis, S. N.: Deliquescence and hygroscopic growth of mixed inorganic-organic atmospheric aerosol, Environ. Sci. Technol., 34, 4313–4319, 2000.
Cziczo, D. J. and Abbatt, J. P. D.: Deliquescence, efflorescence, and supercooling of ammonium sulfate aerosols at low temperature: Implications for cirrus cloud formation and aerosol phase in the atmosphere, J. Geophys. Res., 104, 13781–13790, 1999.
Cziczo, D. J. and Abbatt, J. P. D.: Infrared observations of the response of NaCl, MgCl2, NH4HSO4 and NH4NO3 aerosols to changes in relative humidity from 298 to 238 K, J. Phys. Chem. A, 104, 2038–2047, 2000.
Cziczo, D. J., Nowak, J. B., Hu, J. H., and Abbatt, J. P. D.: Infrared spectroscopy of model tropospheric aerosols as a function of relative humidity: Observation of deliquescence and crystallization, J. Geophys. Res., 102, 18843–18850, 1997.
Earle, M. E., Kuhn, T., Khalizov, A. F., and Sloan, J. J.: Volume nucleation rates for homogeneous freezing in supercooled water microdroplets: results from a combined experimental and modelling approach, Atmos. Chem. Phys., 10, 7945–7961, https://doi.org/10.5194/acp-10-7945-2010, 2010.
Fried, A., Henry, B. E., and Calvert, J. G.: The reaction probability of N2O5 with sulfuric acid aerosols at stratospheric temperatures and compositions, J. Geophys. Res., 99, 3517–3532, 1994.
Grassian, V. H.: Heterogeneous uptake and reaction of nitrogen oxides and volatile organic compounds on the surface of atmospheric particles including oxides, carbonates, soot and mineral dust: Implications for the chemical balance of the troposphere, Int. Rev. Phys. Chem., 20, 467–548, 2001.
Hallquist, M., Stewart, D. J., Stephenson, S. K., and Cox, R. A.: Hydrolysis of N2O5 on sub-micron sulfate aerosols, Phys. Chem. Chem. Phys., 5, 3453–3463, 2003.
Hu, J. H. and Abbatt, J. P. D.: Reaction probabilities for N2O5 hydrolysis on sulfuric acid and ammonium sulfate aerosols at room temperature, J. Phys. Chem. A, 101, 871–878, 1997.
Lambe, A. T., Onasch, T. B., Massoli, P., Croasdale, D. R., Wright, J. P., Ahern, A. T., Williams, L. R., Worsnop, D. R., Brune, W. H., and Davidovits, P.: Laboratory studies of the chemical composition and cloud condensation nuclei (CCN) activity of secondary organic aerosol (SOA) and oxidized primary organic aerosol (OPOA), Atmos. Chem. Phys., 11, 8913–8928, https://doi.org/10.5194/acp-11-8913-2011, 2011.
King, S. M., Butcher, A. C., Rosenoern, T., Coz, E., Lieke, K. I., de Leeuw, G., Nilsson, E. D., and Bilde, M.: Investigating Primary Marine Aerosol Properties: CCN Activity of Sea Salt and Mixed Inorganic–Organic Particles, Environ. Sci. Technol., 46, 10405–10412, 2012.
Koop, T., Kapilashrami, A., Molina, L. T., and Molina, M. J.: Phase transitions of sea- salt/water mixtures at low temperatures: Implications for ozone chemistry in the polar marine boundary layer, J. Geophys. Res., 105, 26393–26402, 2000.
Liu, Y., Yang, Z., Desyaterik, Y., Gassman, P. L., Wang, H., and Laskin, A.: Hygroscopic behavior of substrate-deposited particles studied by micro-FT-IR spectroscopy and complementary methods of particle analysis, Anal. Chem., 80, 633–642, 2008.
Marcolli, C. and Krieger, U. K.: Phase changes during hygroscopic cycles of mixed organic/inorganic model systems of tropospheric aerosols, J. Phys. Chem. A, 110, 1881–1893, 2006.
Martin, S. T.: Phase transitions of aqueous atmospheric particles, Chem. Rev., 100, 3403–3453, 2000.
Murphy, D. M., Thomson, D. S., Middlebrook, A. M., and Schein, M. E.: In situ single-particle characterization at Cape Grim, J. Geophys. Res., 103, 16485–16491, 1998.
Parsons, M. T., Knopf, D. A., and Bertram, A. K.: Deliquescence and crystallization of ammonium sulfate particles internally mixed with water-soluble organic compounds, J. Phys. Chem. A, 108, 11600–11608, 2004.
Parsons, M. T., Riffell, J. L., and Bertram, A. K.: Crystallization of aqueous inorganic-malonic acid particles: Nucleation rates, dependence on size and dependence on the ammonium-to-sulfate ratio, J. Phys. Chem. A, 110, 8101–8115, 2006.
Robinson, C. B., Schill, G. P., and Tolbert, M. A.: Optical growth of highly viscous organic/sulfate particles, J. Atmos. Chem., 71, 145–156, 2014.
Saxena, P., Hildemann, L. M., McMurry, P. H., and Seinfeld, J. H.: Organics alter hygroscopic behavior of atmospheric particles, J. Geophys. Res., 100, 18755–18770, 1995.
Schill, G. P., De Haan, D. O., and Tolbert, M. A.: Heterogeneous ice nucleation on simulated secondary organic aerosol, Environ. Sci. Technol., 48, 1675–1682, 2014.
Smith, M. L., Kuwata, M., and Martin, S. T.: Secondary organic material produced by the dark ozonolysis of α-pinene minimally affects the deliquescence and efflorescence of ammonium sulfate, Aerosol Sci. Technol., 45, 244–261, 2011.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation in aerosol particles: Dependence on O:C, organic functionalities, and compositional complexity, Geophys. Res. Lett., 39, L19801, https://doi.org/10.1029/2012GL052807, 2012.
Tolocka, M. P., Saul, T. D., and Johnston, M. V.: Reactive uptake of nitric acid into aqueous sodium chloride droplets using real-time single-particle mass spectrometry, J. Phys. Chem. A, 108, 2659–2665, 2004.
Veghte, D. P., Altaf, M. B., and Freedman, M. A.: Size dependence of the structure of organic aerosol, J. Amer. Chem. Soc., 135, 16 046–16 049, 2013.
You, Y., Renbaum-Wolff, L., and Bertram, A. K.: Liquid–liquid phase separation in particles containing organics mixed with ammonium sulfate, ammonium bisulfate, ammonium nitrate or sodium chloride, Atmos. Chem. Phys., 13, 11723–11734, https://doi.org/10.5194/acp-13-11723-2013, 2013.
Zappoli, S., Andracchio, A., Fuzzi, S., Facchini, M. C., Gelencsér, A., Kiss, G., Krivácsy, Z., Molnár, Á., Mészáros, E., Hansson, H.-C., Rosman, K., and Zebühr, Y.: Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility, Atmos. Environ., 33, 2733–2743, 1999.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res. Lett., 34, L13801, https://doi.org/10.1029/2007GL029979, 2007.
Zhao, L., Wang, F., Zhang, K., Zeng, Q., and Zhang Y.: Deliquescence and efflorescence processes of aerosol particles studied by in situ FTIR and Raman spectroscopy, Chin. J. Chem. Phys., 21, 1–11, 2008.
Zuend, A., Marcolli, C., Peter, T., and Seinfeld, J. H.: Computation of liquid-liquid equilibria and phase stabilities: implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols, Atmos. Chem. Phys., 10, 7795–7820, https://doi.org/10.5194/acp-10-7795-2010, 2010.
Short summary
This work investigates hygroscopic properties of internally mixed organic/inorganic aerosol particles. Aerosol particles containing organic and inorganic components can phase separate under certain relative humidity conditions, creating particles with an inorganic core and an organic shell. This paper explores whether water uptake from gaseous phase still occurs in such phase-separated systems. It finds that phase separation does not inhibit water uptake for the five systems that were studied.
This work investigates hygroscopic properties of internally mixed organic/inorganic aerosol...
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