Articles | Volume 16, issue 5
Atmos. Chem. Phys., 16, 3245–3264, 2016
https://doi.org/10.5194/acp-16-3245-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 16, 3245–3264, 2016
https://doi.org/10.5194/acp-16-3245-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 11 Mar 2016
Research article | 11 Mar 2016
Phase, composition, and growth mechanism for secondary organic aerosol from the ozonolysis of α-cedrene
Yue Zhao et al.
Related authors
Yao Wang, Yue Zhao, Yuchen Wang, Jian-Zhen Yu, Jingyuan Shao, Ping Liu, Wenfei Zhu, Zhen Cheng, Ziyue Li, Naiqiang Yan, and Huayun Xiao
Atmos. Chem. Phys., 21, 2959–2980, https://doi.org/10.5194/acp-21-2959-2021, https://doi.org/10.5194/acp-21-2959-2021, 2021
Short summary
Short summary
Organosulfates (OSs) are important constituents and tracers of secondary organic aerosols (SOAs) in the atmosphere. Here we characterized the OS species in ambient aerosols in Shanghai, China. We find that the contributions of OSs and SOAs to organic aerosols have increased in recent years and that OS production was largely controlled by the oxidant level (Ox), particularly in summer. We infer that mitigation of Ox pollution can effectively reduce the production of OSs and SOAs in eastern China.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
Short summary
Short summary
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Yue Zhao, Jeremy K. Chan, Felipe D. Lopez-Hilfiker, Megan A. McKeown, Emma L. D'Ambro, Jay G. Slowik, Jeffrey A. Riffell, and Joel A. Thornton
Atmos. Meas. Tech., 10, 3609–3625, https://doi.org/10.5194/amt-10-3609-2017, https://doi.org/10.5194/amt-10-3609-2017, 2017
Short summary
Short summary
We present a novel atmospheric pressure electrospray chemical ionization (ESCI) source that can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol. We couple the ESCI source to a high-resolution time-of-flight mass spectrometer (HRToF-MS) and assess instrument performance through calibrations using different gas standards and measurements of organic mixtures formed by ozonolysis of α-pinene.
Yue Zhao, Michelle C. Fairhurst, Lisa M. Wingen, Véronique Perraud, Michael J. Ezell, and Barbara J. Finlayson-Pitts
Atmos. Meas. Tech., 10, 1373–1386, https://doi.org/10.5194/amt-10-1373-2017, https://doi.org/10.5194/amt-10-1373-2017, 2017
Short summary
Short summary
Two model systems are studied: dicarboxylic acid particles with gaseous amines and α-cedrene ozonolysis particles. Measurements by direct analysis in real-time mass spectrometry and high-resolution time-of-flight aerosol mass spectrometry
show that the reaction of the amines with the acid particles is restricted to the surface layer, with an odd–even alternating pattern. Furthermore, in the α-cedrene study, DART-MS is able to differentiate isomers based on their volatility.
Yao Wang, Yue Zhao, Yuchen Wang, Jian-Zhen Yu, Jingyuan Shao, Ping Liu, Wenfei Zhu, Zhen Cheng, Ziyue Li, Naiqiang Yan, and Huayun Xiao
Atmos. Chem. Phys., 21, 2959–2980, https://doi.org/10.5194/acp-21-2959-2021, https://doi.org/10.5194/acp-21-2959-2021, 2021
Short summary
Short summary
Organosulfates (OSs) are important constituents and tracers of secondary organic aerosols (SOAs) in the atmosphere. Here we characterized the OS species in ambient aerosols in Shanghai, China. We find that the contributions of OSs and SOAs to organic aerosols have increased in recent years and that OS production was largely controlled by the oxidant level (Ox), particularly in summer. We infer that mitigation of Ox pollution can effectively reduce the production of OSs and SOAs in eastern China.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
Short summary
Short summary
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Yue Zhao, Jeremy K. Chan, Felipe D. Lopez-Hilfiker, Megan A. McKeown, Emma L. D'Ambro, Jay G. Slowik, Jeffrey A. Riffell, and Joel A. Thornton
Atmos. Meas. Tech., 10, 3609–3625, https://doi.org/10.5194/amt-10-3609-2017, https://doi.org/10.5194/amt-10-3609-2017, 2017
Short summary
Short summary
We present a novel atmospheric pressure electrospray chemical ionization (ESCI) source that can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol. We couple the ESCI source to a high-resolution time-of-flight mass spectrometer (HRToF-MS) and assess instrument performance through calibrations using different gas standards and measurements of organic mixtures formed by ozonolysis of α-pinene.
Julia Montoya-Aguilera, Jeremy R. Horne, Mallory L. Hinks, Lauren T. Fleming, Véronique Perraud, Peng Lin, Alexander Laskin, Julia Laskin, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, https://doi.org/10.5194/acp-17-11605-2017, 2017
Short summary
Short summary
Various plant species emit a chemical compound called indole under stressed conditions or during flowering events. Our experiments show that indole can be oxidized in the atmosphere to produce a brownish haze containing well-known indole-derived dyes, such as indigo dye. An airshed model that includes indole chemistry shows that indole aerosol makes a significant contribution to the total aerosol burden and to visibility.
Yue Zhao, Michelle C. Fairhurst, Lisa M. Wingen, Véronique Perraud, Michael J. Ezell, and Barbara J. Finlayson-Pitts
Atmos. Meas. Tech., 10, 1373–1386, https://doi.org/10.5194/amt-10-1373-2017, https://doi.org/10.5194/amt-10-1373-2017, 2017
Short summary
Short summary
Two model systems are studied: dicarboxylic acid particles with gaseous amines and α-cedrene ozonolysis particles. Measurements by direct analysis in real-time mass spectrometry and high-resolution time-of-flight aerosol mass spectrometry
show that the reaction of the amines with the acid particles is restricted to the surface layer, with an odd–even alternating pattern. Furthermore, in the α-cedrene study, DART-MS is able to differentiate isomers based on their volatility.
Véronique Perraud, Simone Meinardi, Donald R. Blake, and Barbara J. Finlayson-Pitts
Atmos. Meas. Tech., 9, 1325–1340, https://doi.org/10.5194/amt-9-1325-2016, https://doi.org/10.5194/amt-9-1325-2016, 2016
Short summary
Short summary
Gas phase organosulfur compounds in air serve as precursors of particles which impact human health, visibility, and climate. We compare here two different approaches to measuring these compounds, one an online mass spectrometry technique and the other canister sampling followed by offline analysis by gas chromatography. We show that each approach has its own advantages and limitations in measuring these compounds in complex mixtures, including some artifacts due to reactions on surfaces.
M. L. Dawson, V. Perraud, A. Gomez, K. D. Arquero, M. J. Ezell, and B. J. Finlayson-Pitts
Atmos. Meas. Tech., 7, 2733–2744, https://doi.org/10.5194/amt-7-2733-2014, https://doi.org/10.5194/amt-7-2733-2014, 2014
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Measurement report: Distinct emissions and volatility distribution of intermediate-volatility organic compounds from on-road Chinese gasoline vehicles: implication of high secondary organic aerosol formation potential
Emissions of intermediate-volatility and semi-volatile organic compounds from domestic fuels used in Delhi, India
Effects of liquid–liquid phase separation and relative humidity on the heterogeneous OH oxidation of inorganic–organic aerosols: insights from methylglutaric acid and ammonium sulfate particles
Measurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactor
Ozonolysis of fatty acid monolayers at the air–water interface: organic films may persist at the surface of atmospheric aerosols
Quantification of the role of stabilized Criegee intermediates in the formation of aerosols in limonene ozonolysis
Photochemical degradation of iron(III) citrate/citric acid aerosol quantified with the combination of three complementary experimental techniques and a kinetic process model
The production and hydrolysis of organic nitrates from OH radical oxidation of β-ocimene
Emission factors for PM10 and polycyclic aromatic hydrocarbons (PAHs) from illegal burning of different types of municipal waste in households
Kinetic modeling of formation and evaporation of secondary organic aerosol from NO3 oxidation of pure and mixed monoterpenes
Production of HONO from heterogeneous uptake of NO2 on illuminated TiO2 aerosols measured by Photo-Fragmentation Laser Induced Fluorescence
Direct contribution of ammonia to α-pinene secondary organic aerosol formation
Hygroscopic behavior of aerosols generated from solutions of 3-methyl-1,2,3-butanetricarboxylic acid, its sodium salts, and its mixtures with NaCl
Chemical composition, structures, and light absorption of N-containing aromatic compounds emitted from burning wood and charcoal in household cookstoves
Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiency
On mineral dust aerosol hygroscopicity
Distinct chemical and mineralogical composition of Icelandic dust compared to northern African and Asian dust
Secondary organic aerosol yields from the oxidation of benzyl alcohol
The Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperatures
Molecular understanding of the suppression of new-particle formation by isoprene
Characterization of secondary organic aerosol from heated cooking oil emissions: evolution in composition and volatility
Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?
Liquid–liquid phase separation and morphologies in organic particles consisting of α-pinene and β-caryophyllene ozonolysis products and mixtures with commercially available organic compounds
Characterization of primary and aged wood burning and coal combustion organic aerosols in environmental chamber and its implications for atmospheric aerosols
Oligomer and highly oxygenated organic molecule formation from oxidation of oxygenated monoterpenes emitted by California sage plants
Technical note: Emission factors, chemical composition and morphology of particles emitted from Euro 5 diesel and gasoline light duty vehicles during transient cycles
Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 2: Chemical properties and characterization
Impact of NOx on secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: the role of highly oxygenated organic nitrates
Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation
Measurement report: Diurnal and temporal variations of sugar compounds in suburban aerosols from the northern vicinity of Beijing, China: An influence of biogenic and anthropogenic sources
Glyoxal's impact on dry ammonium salts: fast and reversible surface aerosol browning
Oxygenated products formed from OH-initiated reactions of trimethylbenzene: autoxidation and accretion
Biomass-burning-derived particles from a wide variety of fuels – Part 2: Effects of photochemical aging on particle optical and chemical properties
Measured solid state and subcooled liquid vapour pressures of nitroaromatics using Knudsen effusion mass spectrometry
Polar semivolatile organic compounds in biomass-burning emissions and their chemical transformations during aging in an oxidation flow reactor
Temperature effects on optical properties and chemical composition of secondary organic aerosol derived from n-dodecane
An investigation on hygroscopic properties of 15 black carbon (BC)-containing particles from different carbon sources: roles of organic and inorganic components
Deconvolution of FIGAERO–CIMS thermal desorption profiles using positive matrix factorisation to identify chemical and physical processes during particle evaporation
Mineralogy and geochemistry of Asian dust: dependence on migration path, fractionation, and reactions with polluted air
Photochemical transformation of residential wood combustion emissions: dependence of organic aerosol composition on OH exposure
Seawater analysis by ambient mass-spectrometry-based seaomics
Molecular composition and photochemical evolution of water-soluble organic carbon (WSOC) extracted from field biomass burning aerosols using high-resolution mass spectrometry
Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures
High levels of primary biogenic organic aerosols are driven by only a few plant-associated microbial taxa
Formation of highly oxygenated organic molecules from chlorine-atom-initiated oxidation of alpha-pinene
Pre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopy
The evolutionary behavior of chromophoric brown carbon during ozone aging of fine particles from biomass burning
Technical note: Preparation and purification of atmospherically relevant α-hydroxynitrate esters of monoterpenes
Effect of inorganic-to-organic mass ratio on the heterogeneous OH reaction rates of erythritol: implications for atmospheric chemical stability of 2-methyltetrols
Ambient air quality in the Kathmandu Valley, Nepal, during the pre-monsoon: concentrations and sources of particulate matter and trace gases
Rongzhi Tang, Quanyang Lu, Song Guo, Hui Wang, Kai Song, Ying Yu, Rui Tan, Kefan Liu, Ruizhe Shen, Shiyi Chen, Limin Zeng, Spiro D. Jorga, Zhou Zhang, Wenbin Zhang, Shijin Shuai, and Allen L. Robinson
Atmos. Chem. Phys., 21, 2569–2583, https://doi.org/10.5194/acp-21-2569-2021, https://doi.org/10.5194/acp-21-2569-2021, 2021
Short summary
Short summary
We performed chassis dynamometer experiments to investigate the emissions and secondary organic aerosol (SOA) formation potential of intermediate volatility organic compounds (IVOCs) from an on-road Chinese gasoline vehicle. High IVOC emission factors (EFs) and distinct volatility distribution were recognized. Our results indicate that vehicular IVOCs contribute significantly to SOA, implying the importance of reducing IVOCs when making air pollution control policies in urban areas of China.
Gareth J. Stewart, Beth S. Nelson, W. Joe F. Acton, Adam R. Vaughan, Naomi J. Farren, James R. Hopkins, Martyn W. Ward, Stefan J. Swift, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2407–2426, https://doi.org/10.5194/acp-21-2407-2021, https://doi.org/10.5194/acp-21-2407-2021, 2021
Short summary
Short summary
Biomass burning releases many lower-molecular-weight organic species which are difficult to analyse but important for the formation of organic aerosol. This study examined a new high-resolution technique to better characterise these difficult-to-analyse organic components. Some burning sources analysed in this study, such as cow dung cake and municipal solid waste, released extremely complex mixtures containing many thousands of different lower-volatility organic compounds.
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
Short summary
Short summary
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.
David R. Hanson, Seakh Menheer, Michael Wentzel, and Joan Kunz
Atmos. Chem. Phys., 21, 1987–2001, https://doi.org/10.5194/acp-21-1987-2021, https://doi.org/10.5194/acp-21-1987-2021, 2021
Short summary
Short summary
We report experimental measurements of particle formation in a flow reactor that extend the results from this experiment to a total of more than 270 runs over a time period of ~3 years. This has allowed us to detect a general increase in the cleanliness of the system and improve our knowledge of its chemistry. In-house simulations allowed us to construct phenomenological free energies of molecular clusters of sulfuric acid and ammonia that are appropriate for application to the atmosphere.
Benjamin Woden, Maximilian W. A. Skoda, Adam Milsom, Curtis Gubb, Armando Maestro, James Tellam, and Christian Pfrang
Atmos. Chem. Phys., 21, 1325–1340, https://doi.org/10.5194/acp-21-1325-2021, https://doi.org/10.5194/acp-21-1325-2021, 2021
Short summary
Short summary
Atmospheric aerosols contain a large amount of organic compounds, whose oxidation affects their physical properties through a process known as ageing. We have simulated atmospheric ageing experimentally to elucidate the nature and behaviour of residual surface films. Our results show an increasing amount of residue at near-zero temperatures, demonstrating that an inert product film may build up during droplet ageing, even if only ordinarily short-lived reactive species are initially emitted.
Yiwei Gong and Zhongming Chen
Atmos. Chem. Phys., 21, 813–829, https://doi.org/10.5194/acp-21-813-2021, https://doi.org/10.5194/acp-21-813-2021, 2021
Short summary
Short summary
Stabilized Criegee intermediates (SCIs) are important factors in estimating aerosol formation in the atmosphere. Here the results show that SCIs account for more than 60 % of aerosol formation in limonene ozonolysis and water is an uncertainty in SCI performances. The aerosol formation potential of SCIs under high-humidity conditions is double that under dry and low-humidity conditions, suggesting SCI reactions are still important in contributing to aerosols at high relative humidity.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
Short summary
Short summary
Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Ana C. Morales, Thilina Jayarathne, Jonathan H. Slade, Alexander Laskin, and Paul B. Shepson
Atmos. Chem. Phys., 21, 129–145, https://doi.org/10.5194/acp-21-129-2021, https://doi.org/10.5194/acp-21-129-2021, 2021
Short summary
Short summary
Organic nitrates formed from the oxidation of biogenic volatile organic compounds impact both ozone and particulate matter as they remove nitrogen oxides, but they represent important aerosol precursors. We conducted a series of reaction chamber experiments that quantified the total organic nitrate and secondary organic aerosol yield from the OH-radical-initiated oxidation of ocimene, and also measured their hydrolysis lifetimes in the aqueous phase, as a function of pH.
András Hoffer, Beatrix Jancsek-Turóczi, Ádám Tóth, Gyula Kiss, Anca Naghiu, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 20, 16135–16144, https://doi.org/10.5194/acp-20-16135-2020, https://doi.org/10.5194/acp-20-16135-2020, 2020
Short summary
Short summary
Emission factors for PM10 and polycyclic aromatic hydrocarbons (PAHs) are reported for the first time ever for the indoor combustion of 12 common types of municipal solid waste that are frequently burned in households worldwide. We have found that waste burning emits up to 40 times more PM10 and 800 times more PAHs than the combustion of dry firewood. Our finding highlights the need for coordinated actions against illegal waste combustion and the extreme health hazard associated with it.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, https://doi.org/10.5194/acp-20-15513-2020, 2020
Short summary
Short summary
This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1216, https://doi.org/10.5194/acp-2020-1216, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight at aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, and a model consistent with the data is developed, and aerosol production of HONO in the atmosphere is shown to be significant.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
Short summary
Short summary
Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Li Wu, Clara Becote, Sophie Sobanska, Pierre-Marie Flaud, Emilie Perraudin, Eric Villenave, Young-Chul Song, and Chul-Un Ro
Atmos. Chem. Phys., 20, 14103–14122, https://doi.org/10.5194/acp-20-14103-2020, https://doi.org/10.5194/acp-20-14103-2020, 2020
Short summary
Short summary
MBTCA (3-methyl-1,2,3-butanetricarboxylic acid), a second-generation product of monoterpenes, is one of the most relevant tracer compounds for biogenic secondary organic aerosols (SOAs). Laboratory-generated, micrometer-sized, pure-MBTCA, mono-/di-/trisodium MBTCA salts and MBTCA–NaCl mixture aerosol particles were examined systematically to observe their hygroscopic behavior, and it was also observed that the monosodium MBTCA salt aerosols were formed through a reaction between MBTCA and NaCl.
Mingjie Xie, Zhenzhen Zhao, Amara L. Holder, Michael D. Hays, Xi Chen, Guofeng Shen, James J. Jetter, Wyatt M. Champion, and Qin'geng Wang
Atmos. Chem. Phys., 20, 14077–14090, https://doi.org/10.5194/acp-20-14077-2020, https://doi.org/10.5194/acp-20-14077-2020, 2020
Short summary
Short summary
This study investigated the composition, structures, and light absorption of N-containing aromatic compounds (NACs) in PM2.5 emitted from burning red oak and charcoal in a variety of cookstoves. The results suggest that the identified NACs might have substantial fractions remaining in the gas phase. In comparison to other sources, cookstove emissions from red oak or charcoal fuels did not exhibit unique NAC structural features but had distinct NAC composition.
Yujue Wang, Min Hu, Nan Xu, Yanhong Qin, Zhijun Wu, Liwu Zeng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 20, 13721–13734, https://doi.org/10.5194/acp-20-13721-2020, https://doi.org/10.5194/acp-20-13721-2020, 2020
Short summary
Short summary
Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood. In this study, we designed lab-controlled experiments to comprehensively investigate the emission factors, chemical compositions and light absorption properties of both water-soluble and water-insoluble carbonaceous aerosols emitted from straw burning. The results clearly highlight the significant influences of burning conditions and combustion efficiency on the emissions.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
Short summary
Short summary
We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Clarissa Baldo, Paola Formenti, Sophie Nowak, Servanne Chevaillier, Mathieu Cazaunau, Edouard Pangui, Claudia Di Biagio, Jean-Francois Doussin, Konstantin Ignatyev, Pavla Dagsson-Waldhauserova, Olafur Arnalds, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys., 20, 13521–13539, https://doi.org/10.5194/acp-20-13521-2020, https://doi.org/10.5194/acp-20-13521-2020, 2020
Short summary
Short summary
We showed that Icelandic dust has a fundamentally different chemical and mineralogical composition from low-latitude dust. In particular, magnetite is as high as 1 %–2 % of the total dust mass. Our results suggest that Icelandic dust may have an important impact on the radiation balance in the subpolar and polar regions.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys., 20, 13167–13190, https://doi.org/10.5194/acp-20-13167-2020, https://doi.org/10.5194/acp-20-13167-2020, 2020
Short summary
Short summary
In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work, we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
Short summary
Short summary
Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
Short summary
Short summary
With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Manpreet Takhar, Yunchun Li, and Arthur W. H. Chan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1043, https://doi.org/10.5194/acp-2020-1043, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
Our study highlights the importance of molecular composition in constraining the chemical properties of cooking SOA, as well as understanding the contribution of aldehydes in formation of SOA from cooking emissions. We show that fragmentation reactions are key in atmospheric processing of cooking SOA, and aldehydes emitted from cooking emissions contribute substantially to SOA formation. Our study provides a framework to better predict SOA formation in and downwind of urban atmospheres.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
Short summary
Short summary
In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
Short summary
Short summary
We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-924, https://doi.org/10.5194/acp-2020-924, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
Functional group composition of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
Short summary
Short summary
Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Evangelia Kostenidou, Alvaro Martinez-Valiente, Badr R'Mili, Baptiste Marques, Brice Temime-Roussel, Michel André, Yao Liu, Cédric Louis, Boris Vansevenant, Daniel Ferry, Carine Laffon, Philippe Parent, and Barbara D'Anna
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-842, https://doi.org/10.5194/acp-2020-842, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
Passenger vehicles' emissions can be a significant source of particulate matter in urban areas. In this study the particle phase emissions of seven Euro 5 passenger cars were characterized. Changes in engine technologies and after-treatment devices can alter the chemical composition and the size of the emitted particulate matter. The condition of the Diesel Particle Filter (DPF) plays an important role on the emitted pollutants.
Damon M. Smith, Tianqu Cui, Marc N. Fiddler, Rudra P. Pokhrel, Jason D. Surratt, and Solomon Bililign
Atmos. Chem. Phys., 20, 10169–10191, https://doi.org/10.5194/acp-20-10169-2020, https://doi.org/10.5194/acp-20-10169-2020, 2020
Short summary
Short summary
Biomass fuels used for domestic purposes in east Africa produce a significant atmospheric burden of aerosols and volatile organic compounds. The chemical properties and composition of these aerosols have not been investigated in the laboratory. In this work methanol extracts from filter samples of aerosol collected from an indoor smog chamber were analyzed to determine the chemical composition and identify the light absorption properties of organic aerosol constituents.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
Short summary
Short summary
Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
Short summary
Short summary
Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Santosh Kumar Verma, Kimitaka Kawamura, Fei Yang, Pingqing Fu, Yugo Kanaya, and Zifa Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-734, https://doi.org/10.5194/acp-2020-734, 2020
Revised manuscript accepted for ACP
Short summary
Short summary
We studied aerosol samples collected in Autumn 2007 with day/night intervals in a rural site of Mangshan, north of Beijing, for sugar compounds (SCs) that are abundant organic aerosol components and can influence the air quality and climate. We found higher concentrations of biomass burning (BB) products at night- than daytime, whereas pollen tracers and other SCs showed an opposite diurnal trend. Because this site is meteorologically characterized by mountain/valley breeze.
David O. De Haan, Lelia N. Hawkins, Kevin Jansen, Hannah G. Welsh, Raunak Pednekar, Alexia de Loera, Natalie G. Jimenez, Margaret A. Tolbert, Mathieu Cazaunau, Aline Gratien, Antonin Bergé, Edouard Pangui, Paola Formenti, and Jean-François Doussin
Atmos. Chem. Phys., 20, 9581–9590, https://doi.org/10.5194/acp-20-9581-2020, https://doi.org/10.5194/acp-20-9581-2020, 2020
Short summary
Short summary
When exposed to glyoxal in chamber experiments, dry ammonium or methylammonium sulfate particles turn brown immediately and reversibly without increasing in size. Much less browning was observed on wet aerosol particles, and no browning was observed with sodium sulfate aerosol. While estimated dry aerosol light absorption caused by background glyoxal (70 ppt) is insignificant compared to that of secondary brown carbon overall, in polluted regions this process could be a source of brown carbon.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
Short summary
Short summary
A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
Short summary
Short summary
Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
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
Short summary
Short summary
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.
Deep Sengupta, Vera Samburova, Chiranjivi Bhattarai, Adam C. Watts, Hans Moosmüller, and Andrey Y. Khlystov
Atmos. Chem. Phys., 20, 8227–8250, https://doi.org/10.5194/acp-20-8227-2020, https://doi.org/10.5194/acp-20-8227-2020, 2020
Short summary
Short summary
This paper presents important results on the atmospheric chemistry of combustion emissions. Organic compounds from these emissions can contribute significantly to chemical and physical properties of atmospheric aerosols. In this paper, a detailed chemical analysis of gas- and particle-phase polar organic compounds from the laboratory combustion of globally important fuels is presented. The aging experiments were performed to understand the fate of biomass-burning organics in the atmosphere.
Junling Li, Weigang Wang, Kun Li, Wenyu Zhang, Chao Peng, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 20, 8123–8137, https://doi.org/10.5194/acp-20-8123-2020, https://doi.org/10.5194/acp-20-8123-2020, 2020
Short summary
Short summary
Long-chain alkanes (a large fraction of diesel fuel and its exhaust) are important potential contributors of SOA. Through the analysis of the components of formed SOA, we found that low-temperature conditions promote the oligomerization of n-dodecane, and the degree of oligomerization can reach tetramerization. The presence of the oligomers enhances the light extinction of the particles. UV-scattering particles in the boundary layer can accelerate photochemical reactions and haze production.
Minli Wang, Yiqun Chen, Heyun Fu, Xiaolei Qu, Bengang Li, Shu Tao, and Dongqiang Zhu
Atmos. Chem. Phys., 20, 7941–7954, https://doi.org/10.5194/acp-20-7941-2020, https://doi.org/10.5194/acp-20-7941-2020, 2020
Short summary
Short summary
The mechanism and factors controlling the hygroscopicity of black-carbon-containing particles (BCPs) from different carbon sources are not well understood. We thoroughly characterized the chemical and compositional properties of 15 samples of BCPs from different sources (wood, herb, and soot) and further investigated their hygroscopicity. Depending on the carbon source, organic carbon and dissolved mineral contents were key determinants of the equilibrium and kinetics of water uptake by BCPs.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
Short summary
Short summary
To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Gi Young Jeong
Atmos. Chem. Phys., 20, 7411–7428, https://doi.org/10.5194/acp-20-7411-2020, https://doi.org/10.5194/acp-20-7411-2020, 2020
Short summary
Short summary
During long-range transport, mineral dust interacts with the atmosphere, biosphere, cryosphere, and pedosphere, influencing ecosystems, the atmospheric energy balance, and air quality. This study analyzed the mineral and chemical compositions of Asian dust samples collected during 14 years in Korea. The result showed mineralogical and geochemical variation depending on the dust migration path, fractionation, and atmospheric reactions as well as average properties.
Anni Hartikainen, Petri Tiitta, Mika Ihalainen, Pasi Yli-Pirilä, Jürgen Orasche, Hendryk Czech, Miika Kortelainen, Heikki Lamberg, Heikki Suhonen, Hanna Koponen, Liqing Hao, Ralf Zimmermann, Jorma Jokiniemi, Jarkko Tissari, and Olli Sippula
Atmos. Chem. Phys., 20, 6357–6378, https://doi.org/10.5194/acp-20-6357-2020, https://doi.org/10.5194/acp-20-6357-2020, 2020
Short summary
Short summary
Residential wood combustion emits large amounts of organic compounds, which are transformed in the atmosphere via photochemical ageing reactions. We assessed this organic emission at various stages of exposure with an oxidation flow reactor. Ageing led to major changes in both gaseous and particulate phases including increased acidic compounds and transformation of the polycyclic aromatic compounds. Such changes have serious implications for the health- and climate-related effects of combustion.
Nicolás Zabalegui, Malena Manzi, Antoine Depoorter, Nathalie Hayeck, Marie Roveretto, Chunlin Li, Manuela van Pinxteren, Hartmut Herrmann, Christian George, and María Eugenia Monge
Atmos. Chem. Phys., 20, 6243–6257, https://doi.org/10.5194/acp-20-6243-2020, https://doi.org/10.5194/acp-20-6243-2020, 2020
Short summary
Short summary
A new approach to bridging different fields of science by studying the air–sea interface is described. An untargeted ambient mass-spectrometry-based metabolomics method enables the study of enriched organic compounds found on the sea surface for air–water transfer processes. Results from the metabolomics experiments and a lab-to-field approach provide new opportunities for characterizing the seawater organic-matter content and discovering compounds involved in aerosol-formation processes.
Jing Cai, Xiangying Zeng, Guorui Zhi, Sasho Gligorovski, Guoying Sheng, Zhiqiang Yu, Xinming Wang, and Ping'an Peng
Atmos. Chem. Phys., 20, 6115–6128, https://doi.org/10.5194/acp-20-6115-2020, https://doi.org/10.5194/acp-20-6115-2020, 2020
Short summary
Short summary
The composition and light-induced evolution of a water-soluble organic carbon mixture from fresh biomass burning aerosols was investigated with direct infusion electrospray ionisation high-resolution mass spectrometry (HRMS) and liquid chromatography coupled with HRMS. Our findings indicate that the water-soluble organic fraction of combustion-derived aerosols has the potential to form more oxidised organic matter, contributing to the highly oxygenated nature of atmospheric organic aerosols.
Jienan Li, Seanna M. Forrester, and Daniel A. Knopf
Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, https://doi.org/10.5194/acp-20-6055-2020, 2020
Short summary
Short summary
Organic aerosol is ubiquitous in the atmosphere and can change its phase state from liquid to solid in response to temperature. Our laboratory measurements demonstrate that the chemical reactivity of typical organic aerosol species with atmospheric oxidants is modulated by the species’ phase state. We find that under temperatures typical of the middle and upper troposphere the chemical lifetime of organic aerosol can be significantly extended due to the reduced reactive uptake of gas oxidants.
Abdoulaye Samaké, Aurélie Bonin, Jean-Luc Jaffrezo, Pierre Taberlet, Samuël Weber, Gaëlle Uzu, Véronique Jacob, Sébastien Conil, and Jean M. F. Martins
Atmos. Chem. Phys., 20, 5609–5628, https://doi.org/10.5194/acp-20-5609-2020, https://doi.org/10.5194/acp-20-5609-2020, 2020
Short summary
Short summary
Despite being a major source of coarse organic matter, primary biogenic organic aerosols (PBOAs) remain poorly implemented in source-resolved chemical transport models. This study, based on an intensive field sampling of aerosols, combined physicochemical characterizations of PM10 with DNA high-throughput sequencing to provide a comprehensive understanding of the microbial fingerprints associated with primary sugar compounds (tracers of PBOAs) and their main surrounding environmental sources.
Yonghong Wang, Matthieu Riva, Hongbin Xie, Liine Heikkinen, Simon Schallhart, Qiaozhi Zha, Chao Yan, Xu-Cheng He, Otso Peräkylä, and Mikael Ehn
Atmos. Chem. Phys., 20, 5145–5155, https://doi.org/10.5194/acp-20-5145-2020, https://doi.org/10.5194/acp-20-5145-2020, 2020
Short summary
Short summary
Chamber experiments were conducted with alpha-pinene and chlorine under low- and high-nitrogen-oxide (NOX) conditions. We estimated the HOM yields from chlorine-initiated oxidation of alpha-pinene under low-NOX conditions to be around 1.8 %, though with a uncertainty range (0.8 %–4 %) due to lack of suitable calibration methods. Our study clearly demonstrates that the chlorine-atom-initiated oxidation of alpha-pinene can produce low-volatility organic compounds.
Jack J. Lin, Kamal Raj R, Stella Wang, Esko Kokkonen, Mikko-Heikki Mikkelä, Samuli Urpelainen, and Nønne L. Prisle
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-330, https://doi.org/10.5194/acp-2020-330, 2020
Revised manuscript accepted for ACP
Xingjun Fan, Tao Cao, Xufang Yu, Yan Wang, Xin Xiao, Feiyue Li, Yue Xie, Wenchao Ji, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 20, 4593–4605, https://doi.org/10.5194/acp-20-4593-2020, https://doi.org/10.5194/acp-20-4593-2020, 2020
Short summary
Short summary
A particle-phase O3 oxidation of biomass burning (BB) smoke particles was conducted to investigate the evolution of brown carbon (BrC) therein. The O3 aging induced the decomposition of chromophores and fluorophores. EEM–PARAFAC showed a predominant decomposition of protein-like substances and a gradual increase proportion of humic-like substances for BB BrC during O3 aging. The dynamic spectral behavior of chromophores and functional groups within BrC was further explored by 2D-COS.
Elena Ali McKnight, Nicole P. Kretekos, Demi Owusu, and Rebecca Lyn LaLonde
Atmos. Chem. Phys., 20, 4241–4254, https://doi.org/10.5194/acp-20-4241-2020, https://doi.org/10.5194/acp-20-4241-2020, 2020
Short summary
Short summary
This report describes a simple, safe and effective method to prepare nitrate esters of terpenes (carene, limonene, perillic alcohol, beta-pinene and alpha-pinene) which are key oxidation products in the atmosphere. These compounds are implicated in the formation of secondary organic aerosols. A compilation of the relevant spectroscopic data has been presented. The availability of these compounds and their characterization data will enable further study of the structure–reactivity relationships.
Rongshuang Xu, Hoi Ki Lam, Kevin R. Wilson, James F. Davies, Mijung Song, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 20, 3879–3893, https://doi.org/10.5194/acp-20-3879-2020, https://doi.org/10.5194/acp-20-3879-2020, 2020
Short summary
Short summary
Atmospheric particles, a complex mixture of inorganic salts, organic compounds and water, can continually undergo heterogeneous oxidation initiated by gas-phase oxidants at the particle surface. We found that ammonium sulfate can decelerate the rate of heterogeneous OH reaction with 2-methyltetrols when the inorganic-to-organic mass ratio increases. These results would suggest 2-methyltetrols are likely chemically stable against heterogeneous OH oxidation in the atmosphere.
Md. Robiul Islam, Thilina Jayarathne, Isobel J. Simpson, Benjamin Werden, John Maben, Ashley Gilbert, Puppala S. Praveen, Sagar Adhikari, Arnico K. Panday, Maheswar Rupakheti, Donald R. Blake, Robert J. Yokelson, Peter F. DeCarlo, William C. Keene, and Elizabeth A. Stone
Atmos. Chem. Phys., 20, 2927–2951, https://doi.org/10.5194/acp-20-2927-2020, https://doi.org/10.5194/acp-20-2927-2020, 2020
Short summary
Short summary
The Kathmandu Valley experiences high levels of air pollution. In this study, atmospheric gases and particulate matter were characterized by online and off-line measurements, with an emphasis on understanding their sources. The major sources of particulate matter and trace gases were identified as garbage burning, biomass burning, and vehicles. The majority of secondary organic aerosol was attributed to anthropogenic precursors, while a minority was attributed to biogenic gases.
Cited articles
Alfarra, M. R., Hamilton, J. F., Wyche, K. P., Good, N., Ward, M. W., Carr,
T., Barley, M. H., Monks, P. S., Jenkin, M. E., Lewis, A. C., and McFiggans,
G. B.: The effect of photochemical ageing and initial precursor concentration
on the composition and hygroscopic properties of β-caryophyllene
secondary organic aerosol, Atmos. Chem. Phys., 12, 6417–6436,
https://doi.org/10.5194/acp-12-6417-2012, 2012.
Anglada, J. M., Gonzalez, J., and Torrent-Sucarrat, M.: Effects of the
substituents on the reactivity of carbonyl oxides. A theoretical study on the
reaction of substituted carbonyl oxides with water, Phys. Chem. Chem. Phys.,
13, 13034–13045, https://doi.org/10.1039/c1cp20872a, 2011.
Bateman, A. P., Bertram, A. K., and Martin, S. T.: Hygroscopic Influence on
the Semisolid-to-Liquid Transition of Secondary Organic Materials, J. Phys.
Chem. A, 119, 4386–4395, https://doi.org/10.1021/jp508521c, 2015.
Berndt, T., Kaethner, R., Voigtlander, J., Stratmann, F., Pfeifle, M.,
Reichle, P., Sipila, M., Kulmala, M., and Olzmann, M.: Kinetics of the
unimolecular reaction of CH2OO and the bimolecular reactions with the
water monomer, acetaldehyde and acetone under atmospheric conditions, Phys.
Chem. Chem. Phys., 17, 19862–19873, https://doi.org/10.1039/c5cp02224j, 2015.
Birdsall, A. W., Zentner, C. A., and Elrod, M. J.: Study of the kinetics and
equilibria of the oligomerization reactions of 2-methylglyceric acid, Atmos.
Chem. Phys., 13, 3097–3109, https://doi.org/10.5194/acp-13-3097-2013, 2013.
Bones, D. L., Reid, J. P., Lienhard, D. M., and Krieger, U. K.: Comparing the
mechanism of water condensation and evaporation in glassy aerosol, P. Natl.
Acad. Sci. USA, 109, 11613–11618, 2012.
Bonn, B. and Moortgat, G. K.: Sesquiterpene ozonolysis: Origin of atmospheric
new particle formation from biogenic hydrocarbons, Geophys. Res. Lett., 30,
1585, https://doi.org/10.1029/2003GL017000, 2003.
Bonn, B., Kulmala, M., Riipinen, I., Sihto, S. L., and Ruuskanen, T. M.: How
biogenic terpenes govern the correlation between sulfuric acid concentrations
and new particle formation, J. Geophys. Res., 113, D12209,
https://doi.org/10.1029/2007jd009327, 2008.
Bouvier-Brown, N. C., Goldstein, A. H., Gilman, J. B., Kuster, W. C., and de
Gouw, J. A.: In-situ ambient quantification of monoterpenes, sesquiterpenes,
and related oxygenated compounds during BEARPEX 2007: implications for gas-
and particle-phase chemistry, Atmos. Chem. Phys., 9, 5505–5518,
https://doi.org/10.5194/acp-9-5505-2009, 2009.
Boy, M., Karl, T., Turnipseed, A., Mauldin, R. L., Kosciuch, E., Greenberg,
J., Rathbone, J., Smith, J., Held, A., Barsanti, K., Wehner, B., Bauer, S.,
Wiedensohler, A., Bonn, B., Kulmala, M., and Guenther, A.: New particle
formation in the Front Range of the Colorado Rocky Mountains, Atmos. Chem.
Phys., 8, 1577–1590, https://doi.org/10.5194/acp-8-1577-2008, 2008.
Bruns, E. A., Perraud, V., Zelenyuk, A., Ezell, M. J., Johnson, S. N., Yu,
Y., Imre, D., Finlayson-Pitts, B. J., and Alexander, M. L.: Comparison of
FTIR and particle mass spectrometry for the measurement of particulate
organic nitrates, Environ. Sci. Technol., 44, 1056–1061,
https://doi.org/10.1021/Es9029864, 2010.
Canagaratna, M. R., Jimenez, J. L., Kroll, J. H., Chen, Q., Kessler, S. H.,
Massoli, P., Hildebrandt Ruiz, L., Fortner, E., Williams, L. R., Wilson, K.
R., Surratt, J. D., Donahue, N. M., Jayne, J. T., and Worsnop, D. R.:
Elemental ratio measurements of organic compounds using aerosol mass
spectrometry: characterization, improved calibration, and implications,
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, 2015.
Cappa, C. D. and Wilson, K. R.: Evolution of organic aerosol mass spectra
upon heating: implications for OA phase and partitioning behavior, Atmos.
Chem. Phys., 11, 1895–1911, https://doi.org/10.5194/acp-11-1895-2011, 2011.
Chan, M. N., Surratt, J. D., Chan, A. W. H., Schilling, K., Offenberg, J. H.,
Lewandowski, M., Edney, E. O., Kleindienst, T. E., Jaoui, M., Edgerton, E.
S., Tanner, R. L., Shaw, S. L., Zheng, M., Knipping, E. M., and Seinfeld, J.
H.: Influence of aerosol acidity on the chemical composition of secondary
organic aerosol from β-caryophyllene, Atmos. Chem. Phys., 11,
1735–1751, https://doi.org/10.5194/acp-11-1735-2011, 2011.
Chan, M. N., Zhang, H. F., Goldstein, A. H., and Wilson, K. R.: Role of water
and phase in the heterogeneous oxidation of solid and aqueous succinic acid
aerosol by hydroxyl radicals, J. Phys. Chem. C, 118, 28978–28992,
https://doi.org/10.1021/jp5012022, 2014.
Chao, W., Hsieh, J. T., Chang, C. H., and Lin, J. J. M.: Direct kinetic
measurement of the reaction of the simplest Criegee intermediate with water
vapor, Science, 347, 751–754, https://doi.org/10.1126/science.1261549, 2015.
Chen, Q., Li, Y. L., McKinney, K. A., Kuwata, M., and Martin, S. T.: Particle
mass yield from β-caryophyllene ozonolysis, Atmos. Chem. Phys., 12,
3165–3179, https://doi.org/10.5194/acp-12-3165-2012, 2012.
Cody, R. B., Laramee, J. A., and Durst, H. D.: Versatile new ion source for
the analysis of materials in open air under ambient conditions, Anal. Chem.,
77, 2297–2302, https://doi.org/10.1021/ac050162j, 2005.
Compernolle, S., Ceulemans, K., and Müller, J.-F.: EVAPORATION: a new
vapour pressure estimation methodfor organic molecules including
non-additivity and intramolecular interactions, Atmos. Chem. Phys., 11,
9431–9450, https://doi.org/10.5194/acp-11-9431-2011, 2011.
Crank, J.: The mathematics of diffusion, 2nd Edn., Clarendon Press, Oxford,
1975.
Crounse, J. D., Nielsen, L. B., Jorgensen, S., Kjaergaard, H. G., and
Wennberg, P. O.: Autoxidation of organic compounds in the atmosphere, J.
Phys. Chem. Lett., 4, 3513–3520, 2013.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T.,
Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop,
D. R., and Jimenez, J. L.: Field-deployable, high-resolution, time-of-flight
aerosol mass spectrometer, Anal. Chem., 78, 8281–8289, 2006.
DePalma, J. W., Horan, A. J., Hall, W. A., and Johnston, M. V.:
Thermodynamics of oligomer formation: implications for secondary organic
aerosol formation and reactivity, Phys. Chem. Chem. Phys., 15, 6935–6944,
2013.
Ding, X., He, Q. F., Shen, R. Q., Yu, Q. Q., and Wang, X. M.: Spatial
distributions of secondary organic aerosols from isoprene, monoterpenes,
beta-caryophyllene, and aromatics over China during summer, J. Geophys. Res.,
119, 11877–11891, https://doi.org/10.1002/2014jd021748, 2014.
Docherty, K. S., Wu, W., Lim, Y. B., and Ziemann, P. J.: Contributions of
organic peroxides to secondary aerosol formed from reactions of monoterpenes
with O3, Environ. Sci. Technol., 39, 4049–4059, 2005.
Donahue, N. M., Drozd, G. T., Epstein, S. A., Presto, A. A., and Kroll, J.
H.: Adventures in ozoneland: down the rabbit-hole, Phys. Chem. Chem. Phys.,
13, 10848–10857, https://doi.org/10.1039/c0cp02564j, 2011.
Donahue, N. M., Ortega, I. K., Chuang, W., Riipinen, I., Riccobono, F.,
Schobesberger, S., Dommen, J., Baltensperger, U., Kulmala, M., Worsnop, D.
R., and Vehkamaki, H.: How do organic vapors contribute to new-particle
formation?, Faraday Discuss., 165, 91–104, https://doi.org/10.1039/c3fd00046j, 2013.
Duhl, T. R., Helmig, D., and Guenther, A.: Sesquiterpene emissions from
vegetation: a review, Biogeosciences, 5, 761–777, https://doi.org/10.5194/bg-5-761-2008,
2008.
Ehn, M., Thornton, J. A., Kleist, E., Sipila, M., Junninen, H., Pullinen, I.,
Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres,
S., Acir, I. H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma,
J., Kontkanen, J., Nieminen, T., Kurten, T., Nielsen, L. B., Jorgensen, S.,
Kjaergaard, H. G., Canagaratna, M., Dal Maso, M., Berndt, T., Petaja, T.,
Wahner, A., Kerminen, V. M., Kulmala, M., Worsnop, D. R., Wildt, J., and
Mentel, T. F.: A large source of low-volatility secondary organic aerosol,
Nature, 506, 476–479, 2014.
Finlayson-Pitts, B. J. and Pitts, J. N.: Chemistry of the upper and lower
atmosphere: theory, experiments, and applications, Academic Press, San Diego,
2000.
Gao, Y. Q., Hall, W. A., and Johnston, M. V.: Molecular composition of
monoterpene secondary organic aerosol at low mss loading, Environ. Sci.
Technol., 44, 7897–7902, https://doi.org/10.1021/Es101861k, 2010.
Goldstein, A. H. and Galbally, I. E.: Known and unexplored organic
constituents in the earth's atmosphere, Environ. Sci. Technol., 41,
1514–1521, https://doi.org/10.1021/Es072476p, 2007.
Greaves, J. and Roboz, J.: Mass spectrometry for the novice, CRC Press, Boca
Raton, F. L., USA, 2013.
Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T.,
Harley, P., Klinger, L., Lerdau, M., Mckay, W. A., Pierce, T., Scholes, B.,
Steinbrecher, R., Tallamraju, R., Taylor, J., and Zimmerman, P.: A
global-model of natural volatile organic compound emissions, J. Geophys.
Res., 100, 8873–8892, https://doi.org/10.1029/94jd02950, 1995.
Hall, W. A. and Johnston, M. V.: Oligomer formation pathways in secondary
organic aerosol from MS and MS/MS measurements with high mass accuracy and
resolving power, J. Am. Soc. Mass Spectrom., 23, 1097–1108, 2012.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D.,
Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H.,
Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M.
E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel,
Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D.,
Szmigielski, R., and Wildt, J.: The formation, properties and impact of
secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys.,
9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Harrick, N. J.: Internal reflection spectroscopy, Interscience Publishers,
New York, 1967.
Heaton, K. J., Sleighter, R. L., Hatcher, P. G., Hall, W. A., and Johnston,
M. V.: Composition domains in monoterpene secondary organic aerosol, Environ.
Sci. Technol., 43, 7797–7802, 2009.
Helmig, D., Ortega, J., Duhl, T., Tanner, D., Guenther, A., Harley, P.,
Wiedinmyer, C., Milford, J., and Sakulyanontvittaya, T.: Sesquiterpene
emissions from pine trees – Identifications, emission rates and flux
estimates for the contiguous United States, Environ. Sci. Technol., 41,
1545–1553, https://doi.org/10.1021/Es0618907, 2007.
Hodas, N., Zuend, A., Mui, W., Flagan, R. C., and Seinfeld, J. H.: Influence
of particle-phase state on the hygroscopic behavior of mixed
organic–inorganic aerosols, Atmos. Chem. Phys., 15, 5027–5045,
https://doi.org/10.5194/acp-15-5027-2015, 2015.
Hoffmann, T., Odum, J. R., Bowman, F., Collins, D., Klockow, D., Flagan, R.
C., and Seinfeld, J. H.: Formation of organic aerosols from the oxidation of
biogenic hydrocarbons, J. Atmos. Chem., 26, 189–222,
https://doi.org/10.1023/A:1005734301837, 1997.
Hoffmann, T., Bandur, R., Marggraf, U., and Linscheid, M.: Molecular
composition of organic aerosols formed in the alpha-pinene/O3 reaction:
Implications for new particle formation processes, J. Geophys. Res., 103,
25569–25578, 1998.
Hu, D., Bian, Q., Li, T. W. Y., Lau, A. K. H., and Yu, J. Z.: Contributions
of isoprene, monoterpenes, beta-caryophyllene, and toluene to secondary
organic aerosols in Hong Kong during the summer of 2006, J. Geophys. Res.,
113, D22206, https://doi.org/10.1029/2008jd010437, 2008.
IPCC: Summary for Policymakers, in: Climate Change 2013: The Physical Science
Basis. Contribution of Working Group I to the Fifth Assessment Report of the
Intergovernmental Panel on Climate Change, edited by: Stocker, T. F., Qin,
D., Plattner, G.-K., Tignor, M., Allen, S. K., Boschung, J., Nauels, A., Xia,
Y., Bex, V., and Midgley, P. M., Cambridge University Press, Cambridge,
United Kingdom and New York, NY, USA, 2013.
Jaoui, M., Sexton, K. G., and Kamens, R. M.: Reaction of alpha-cedrene with
ozone: mechanism, gas and particulate products distribution, Atmos. Environ.,
38, 2709–2725, 2004.
Jaoui, M., Kleindienst, T. E., Docherty, K. S., Lewandowski, M., and
Offenberg, J. H.: Secondary organic aerosol formation from the oxidation of a
series of sesquiterpenes: alpha-cedrene, beta-caryophyllene, alpha-humulene
and alpha-farnesene with O3, OH and NO3 radicals, Environ. Chem.,
10, 178–193, https://doi.org/10.1071/En13025, 2013.
Jokinen, T., Berndt, T., Makkonen, R., Kerminen, V. M., Junninen, H.,
Paasonen, P., Stratmann, F., Herrmann, H., Guenther, A. B., Worsnop, D. R.,
Kulmala, M., Ehn, M., and Sipila, M.: Production of extremely low volatile
organic compounds from biogenic emissions: Measured yields and atmospheric
implications, P. Natl. Acad. Sci. USA, 112, 7123–7128,
https://doi.org/10.1073/pnas.1423977112, 2015.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J.,
Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J.,
Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat,
G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E.,
Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate
modelling: a review, Atmos. Chem. Phys., 5, 1053–1123,
https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kanawati, B., Herrmann, F., Joniec, S., Winterhalter, R., and Moortgat, G.
K.: Mass spectrometric characterization of beta-caryophyllene ozonolysis
products in the aerosol studied using an electrospray triple quadrupole and
time-of-flight analyzer hybrid system and density functional theory, Rapid
Commun. Mass Sp., 22, 165–186, https://doi.org/10.1002/Rcm.3340, 2008.
Kidd, C., Perraud, V., and Finlayson-Pitts, B. J.: New insights into
secondary organic aerosol from the ozonolysis of alpha-pinene from combined
infrared spectroscopy and mass spectrometry measurements, Phys. Chem. Chem.
Phys., 16, 22706–22716, 2014a.
Kidd, C., Perraud, V., Wingen, L. M., and Finlayson-Pitts, B. J.: Integrating
phase and composition of secondary organic aerosol from the ozonolysis of
alpha-pinene, P. Natl. Acad. Sci. USA, 111, 7552–7557, 2014b.
Kim, H., Liu, S., Russell, L. M., and Paulson, S. E.: Dependence of real
refractive indices on O : C, H : C and mass fragments of secondary
organic aerosol generated from ozonolysis and photooxidation of limonene and
alpha-pinene, Aerosol Sci. Tech., 48, 498–507,
https://doi.org/10.1080/02786826.2014.893278, 2014.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition
and phase state of organic compounds: dependency on molecular properties and
implications for secondary organic aerosols in the atmosphere, Phys. Chem.
Chem. Phys., 13, 19238–19255, 2011.
Kristensen, K., Enggrob, K. L., King, S. M., Worton, D. R., Platt, S. M.,
Mortensen, R., Rosenoern, T., Surratt, J. D., Bilde, M., Goldstein, A. H.,
and Glasius, M.: Formation and occurrence of dimer esters of pinene oxidation
products in atmospheric aerosols, Atmos. Chem. Phys., 13, 3763–3776,
https://doi.org/10.5194/acp-13-3763-2013, 2013.
Kristensen, K., Cui, T., Zhang, H., Gold, A., Glasius, M., and Surratt, J.
D.: Dimers in α-pinene secondary organic aerosol: effect of hydroxyl
radical, ozone, relative humidity and aerosol acidity, Atmos. Chem. Phys.,
14, 4201–4218, https://doi.org/10.5194/acp-14-4201-2014, 2014.
Kroll, J. H. and Seinfeld, J. H.: Chemistry of secondary organic aerosol:
Formation and evolution of low-volatility organics in the atmosphere, Atmos.
Environ., 42, 3593–3624, 2008.
Lambe, A. T., Cappa, C. D., Massoli, P., Onasch, T. B., Forestieri, S. D.,
Martin, A. T., Cummings, M. J., Croasdale, D. R., Brune, W. H., Worsnop, D.
R., and Davidovits, P.: Relationship between oxidation level and optical
properties of secondary organic aerosol, Environ. Sci. Technol., 47,
6349–6357, 2013.
Lee, A., Goldstein, A. H., Keywood, M. D., Gao, S., Varutbangkul, V.,
Bahreini, R., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.: Gas-phase
products and secondary aerosol yields from the ozonolysis of ten different
terpenes, J. Geophys. Res., 111, D07302, https://doi.org/10.1029/2005JD006437, 2006.
Lee, C. T. and Kamens, R. M.: Particle nucleation from the reaction of
α−pinene and O3, Atmos. Environ., 39, 6822–6832, 2005.
Lewis, T. R., Blitz, M. A., Heard, D. E., and Seakins, P. W.: Direct evidence
for a substantive reaction between the Criegee intermediate, CH2OO, and
the water vapour dimer, Phys. Chem. Chem. Phys., 17, 4859–4863,
https://doi.org/10.1039/c4cp04750h, 2015.
Lignell, H., Hinks, M. L., and Nizkorodov, S. A.: Exploring matrix effects on
photochemistry of organic aerosols, P. Natl. Acad. Sci. USA, 111,
13780–13785, 2014.
Mauderly, J. L. and Chow, J. C.: Health effects of organic aerosols, Inhal.
Toxicol., 20, 257–288, https://doi.org/10.1080/08958370701866008, 2008.
Mehrer, H.: Diffusion in solids: fundamentals, methods, materials,
diffusion-controlled processes, Springer Series, solid state science, 155,
Springer, Berlin, New York, 2007.
Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.:
Amorphous and crystalline aerosol particles interacting with water vapor:
conceptual framework and experimental evidence for restructuring, phase
transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491–9522,
https://doi.org/10.5194/acp-9-9491-2009, 2009.
Müller, L., Reinnig, M.-C., Warnke, J., and Hoffmann, Th.: Unambiguous
identification of esters as oligomers in secondary organic aerosol formed
from cyclohexene and cyclohexene/a-pinene ozonolysis, Atmos. Chem. Phys., 8,
1423–1433, https://doi.org/10.5194/acp-8-1423-2008, 2008.
Müller, L., Reinnig, M. C., Hayen, H., and Hoffmann, T.: Characterization of
oligomeric compounds in secondary organic aerosol using liquid chromatography
coupled to electrospray ionization Fourier transform ion cyclotron resonance
mass spectrometry, Rapid Commun. Mass Sp., 23, 971–979, 2009.
Nah, T., Chan, M., Leone, S. R., and Wilson, K. R.: Real time in situ
chemical characterization of submicrometer organic particles using direct
analysis in real time-mass spectrometry, Anal. Chem., 85, 2087–2095,
https://doi.org/10.1021/ac302560c, 2013.
Ng, N. L., Kroll, J. H., Keywood, M. D., Bahreini, R., Varutbangkul, V.,
Flagan, R. C., Seinfeld, J. H., Lee, A., and Goldstein, A. H.: Contribution
of first- versus second-generation products to secondary organic aerosols
formed in the oxidation of biogenic hydrocarbons, Environ. Sci. Technol., 40,
2283–2297, https://doi.org/10.1021/Es052269u, 2006.
Pajunoja, A., Lambe, A. T., Hakala, J., Rastak, N., Cummings, M. J., Brogan,
J. F., Hao, L. Q., Paramonov, M., Hong, J., Prisle, N. L., Malila, J.,
Romakkaniemi, S., Lehtinen, K. E. J., Laaksonen, A., Kulmala, M., Massoli,
P., Onasch, T. B., Donahue, N. M., Riipinen, I., Davidovits, P., Worsnop, D.
R., Petaja, T., and Virtanen, A.: Adsorptive uptake of water by semisolid
secondary organic aerosols, Geophys. Res. Lett., 42, 3063–3068,
https://doi.org/10.1002/2015GL063142, 2015.
Pankow, J. F. and Asher, W. E.: SIMPOL.1: a simple group contribution method
for predicting vapor pressures and enthalpies of vaporization of
multifunctional organic compounds, Atmos. Chem. Phys., 8, 2773–2796,
https://doi.org/10.5194/acp-8-2773-2008, 2008.
Perraud, V., Bruns, E. A., Ezell, M. J., Johnson, S. N., Yu, Y., Alexander,
M. L., Zelenyuk, A., Imre, D., Chang, W. L., Dabdub, D., Pankow, J. F., and
Finlayson-Pitts, B. J.: Nonequilibrium atmospheric secondary organic aerosol
formation and growth, P. Natl. Acad. Sci. USA, 109, 2836–2841, 2012.
Reinnig, M. C., Warnke, J., and Hoffmann, T.: Identification of organic
hydroperoxides and hydroperoxy acids in secondary organic aerosol formed
during the ozonolysis of different monoterpenes and sesquiterpenes by on-line
analysis using atmospheric pressure chemical ionization ion trap mass
spectrometry, Rapid Commun. Mass Sp., 23, 1735–1741, https://doi.org/10.1002/Rcm.4065,
2009.
Renbaum, L. H. and Smith, G. D.: The importance of phase in the
radical-initiated oxidation of model organic aerosols: reactions of solid and
liquid brassidic acid particles, Phys. Chem. Chem. Phys., 11, 2441–2451,
https://doi.org/10.1039/b816799k, 2009.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M.,
Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity
of alpha-pinene secondary organic material and implications for particle
growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019, 2013.
Richters, S., Herrmann, H., and Berndt, T.: Gas-phase rate coefficients of
the reaction of ozone with four sesquiterpenes at 295 ± 2 K, Phys.
Chem. Chem. Phys., 17, 11658–11669, https://doi.org/10.1039/c4cp05542j, 2015.
Riipinen, I., Pierce, J. R., Yli-Juuti, T., Nieminen, T., Häkkinen, S.,
Ehn, M., Junninen, H., Lehtipalo, K., Petäjä, T., Slowik, J., Chang,
R., Shantz, N. C., Abbatt, J., Leaitch, W. R., Kerminen, V.-M., Worsnop, D.
R., Pandis, S. N., Donahue, N. M., and Kulmala, M.: Organic condensation: a
vital link connecting aerosol formation to cloud condensation nuclei (CCN)
concentrations, Atmos. Chem. Phys., 11, 3865–3878,
https://doi.org/10.5194/acp-11-3865-2011, 2011.
Rissanen, M. P., Kurten, T., Sipila, M., Thornton, J. A., Kausiala, O.,
Garmash, O., Kjaergaard, H. G., Petaja, T., Worsnop, D. R., Ehn, M., and
Kulmala, M.: Effects of chemical complexity on the autoxidation mechanisms of
endocyclic alkene ozonolysis products: from methylcyclohexenes toward
understanding alpha-pinene, J. Phys. Chem. A, 119, 4633–4650,
https://doi.org/10.1021/jp510966g, 2015.
Ruscic, B.: Active thermochemical tables: water and water dimer, J. Phys.
Chem. A, 117, 11940–11953, https://doi.org/10.1021/jp403197t, 2013.
Ryzhkov, A. B. and Ariya, P. A.: A theoretical study of the reactions of
parent and substituted Criegee intermediates with water and the water dimer,
Phys. Chem. Chem. Phys., 6, 5042–5050, https://doi.org/10.1039/b408414d, 2004.
Sadezky, A., Winterhalter, R., Kanawati, B., Römpp, A., Spengler, B.,
Mellouki, A., Le Bras, G., Chaimbault, P., and Moortgat, G. K.: Oligomer
formation during gas-phase ozonolysis of small alkenes and enol ethers: new
evidence for the central role of the Criegee Intermediate as oligomer chain
unit, Atmos. Chem. Phys., 8, 2667–2699, https://doi.org/10.5194/acp-8-2667-2008, 2008.
Sakulyanontvittaya, T., Duhl, T., Wiedinmyer, C., Helmig, D., Matsunaga, S.,
Potosnak, M., Milford, J., and Guenther, A.: Monoterpene and sesquiterpene
emission estimates for the United States, Environ. Sci. Technol., 42,
1623–1629, https://doi.org/10.1021/Es702274e, 2008a.
Sakulyanontvittaya, T., Guenther, A., Helmig, D., Milford, J., and
Wiedinmyer, C.: Secondary organic aerosol from sesquiterpene and monoterpene
emissions in the United States, Environ. Sci. Technol., 42, 8784–8790,
https://doi.org/10.1021/Es800817r, 2008b.
Saukko, E., Lambe, A. T., Massoli, P., Koop, T., Wright, J. P., Croasdale, D.
R., Pedernera, D. A., Onasch, T. B., Laaksonen, A., Davidovits, P., Worsnop,
D. R., and Virtanen, A.: Humidity-dependent phase state of SOA particles from
biogenic and anthropogenic precursors, Atmos. Chem. Phys., 12, 7517–7529,
https://doi.org/10.5194/acp-12-7517-2012, 2012.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from
air pollution to climate change, 2nd Edn., J. Wiley, Hoboken, N.J., 2006.
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric
secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801,
https://doi.org/10.1029/2012GL054008, 2012.
Shiraiwa, M., Ammann, M., Koop, T., and Poschl, U.: Gas uptake and chemical
aging of semisolid organic aerosol particles, P. Natl. Acad. Sci. USA, 108,
11003–11008, 2011.
Shiraiwa, M., Selzle, K., and Pöschl, U.: Hazardous components and health
effects of atmospheric aerosol particles: reactive oxygen species, soot,
polycyclic aromatic compounds and allergenic proteins, Free Radical Res., 46,
927–939, https://doi.org/10.3109/10715762.2012.663084, 2012.
Shu, Y. G. and Atkinson, R.: Rate constants for the gas-phase reactions of
O3 with a series of terpenes and OH radical formation from the O3
reactions with sesquiterpenes at 296 ± 2 K, Int. J. Chem. Kinet., 26,
1193–1205, 1994.
Slade, J. H. and Knopf, D. A.: Multiphase OH oxidation kinetics of organic
aerosol: The role of particle phase state and relative humidity, Geophys.
Res. Lett., 41, 5297–5306, https://doi.org/10.1002/2014GL060582, 2014.
Socrates, G.: Infrared and Raman characteristic group frequencies: tables and
charts, 3rd Edn., Wiley, Chichester, New York, 2001.
Taatjes, C. A., Welz, O., Eskola, A. J., Savee, J. D., Scheer, A. M.,
Shallcross, D. E., Rotavera, B., Lee, E. P. F., Dyke, J. M., Mok, D. K. W.,
Osborn, D. L., and Percival, C. J.: Direct measurements of
conformer-dependent reactivity of the criegee intermediate CH3CHOO,
Science, 340, 177–180, 2013.
Tasoglou, A. and Pandis, S. N.: Formation and chemical aging of secondary
organic aerosol during the β-caryophyllene oxidation, Atmos. Chem.
Phys., 15, 6035–6046, https://doi.org/10.5194/acp-15-6035-2015, 2015.
Tolocka, M. P., Jang, M., Ginter, J. M., Cox, F. J., Kamens, R. M., and
Johnston, M. V.: Formation of oligomers in secondary organic aerosol,
Environ. Sci. Technol., 38, 1428–1434, 2004.
Vereecken, L., Muller, J. F., and Peeters, J.: Low-volatility poly-oxygenates
in the OH-initiated atmospheric oxidation of alpha-pinene: impact of
non-traditional peroxyl radical chemistry, Phys. Chem. Chem. Phys., 9,
5241–5248, 2007.
Vereecken, L., Harder, H., and Novelli, A.: The reaction of Criegee
intermediates with NO, RO2, and SO2, and their fate in the
atmosphere, Phys. Chem. Chem. Phys., 14, 14682–14695, 2012.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirila, P.,
Leskinen, J., Makela, J. M., Holopainen, J. K., Poschl, U., Kulmala, M.,
Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic
secondary organic aerosol particles, Nature, 467, 824–827,
https://doi.org/10.1038/nature09455, 2010.
Welz, O., Eskola, A. J., Sheps, L., Rotavera, B., Savee, J. D., Scheer, A.
M., Osborn, D. L., Lowe, D., Booth, A. M., Xiao, P., Khan, M. A. H.,
Percival, C. J., Shallcross, D. E., and Taatjes, C. A.: Rate coefficients of
C1 and C2 Criegee intermediate reactions with formic and acetic acid near the
collision limit: direct kinetics measurements and atmospheric implications,
Angew. Chem.-Int. Ed., 53, 4547–4550, 2014.
Winkler, P. M., Ortega, J., Karl, T., Cappellin, L., Friedli, H. R.,
Barsanti, K., McMurry, P. H., and Smith, J. N.: Identification of the
biogenic compounds responsible for size-dependent nanoparticle growth,
Geophys. Res. Lett., 39, L20815, https://doi.org/10.1029/2012gl053253, 2012.
Winterhalter, R., Herrmann, F., Kanawati, B., Nguyen, T. L., Peeters, J.,
Vereecken, L., and Moortgat, G. K.: The gas-phase ozonolysis of
beta-caryophyllene (C15H24). Part I: an experimental study, Phys.
Chem. Chem. Phys., 11, 4152–4172, https://doi.org/10.1039/B817824k, 2009.
Witkowski, B. and Gierczak, T.: Analysis of alpha-acyloxyhydroperoxy
aldehydes with electrospray ionization-tandem mass spectrometry
(ESI-MSn), J. Mass Spectrom., 48, 79–88, https://doi.org/10.1002/jms.3130, 2013.
Witkowski, B. and Gierczak, T.: Early stage composition of SOA produced by
alpha-pinene/ozone reaction: alpha-Acyloxyhydroperoxy aldehydes and acidic
dimers, Atmos. Environ., 95, 59–70, 2014.
Yao, L., Ma, Y., Wang, L., Zheng, J., Khalizov, A., Chen, M. D., Zhou, Y. Y.,
Qi, L., and Cui, F. P.: Role of stabilized Criegee intermediate in secondary
organic aerosol formation from the ozonolysis of alpha-cedrene, Atmos.
Environ., 94, 448–457, 2014.
Yasmeen, F., Vermeylen, R., Szmigielski, R., Iinuma, Y., Boge, O., Herrmann,
H., Maenhaut, W., and Claeys, M.: Terpenylic acid and related compounds:
precursors for dimers in secondary organic aerosol from the ozonolysis of
alpha- and beta-pinene, Atmos. Chem. Phys., 10, 9383–9392, 2010.
Ying, Q., Li, J. Y., and Kota S. H.: Significant contributions of isoprene to
summertime secondary organic aerosol in eastern United States, Environ. Sci.
Technol., 49, 7834–7842, 2015.
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.
Zhang, R. Y., Wang, G. H., Guo, S., Zarnora, M. L., Ying, Q., Lin, Y., Wang,
W. G., Hu, M., and Wang, Y.: Formation of urban fine particulate matter,
Chem. Rev., 115, 3803–3855, https://doi.org/10.1021/acs.chemrev.5b00067, 2015.
Zhang, X., McVay, R. C., Huang, D. D., Dalleska, N. F., Aumont, B., Flagan,
R. C., and Seinfeld, J. H.: Formation and evolution of molecular products in
α-pinene secondary organic aerosol, P. Natl. Acad. Sci. USA, 112,
14168–14173, https://doi.org/10.1073/pnas.1517742112, 2015.
Zhao, J., Ortega, J., Chen, M., McMurry, P. H., and Smith, J. N.: Dependence
of particle nucleation and growth on high-molecular-weight gas-phase products
during ozonolysis of α-pinene, Atmos. Chem. Phys., 13, 7631–7644,
https://doi.org/10.5194/acp-13-7631-2013, 2013.
Zhao, Y., Wingen, L. M., Perraud, V., Greaves, J., and Finlayson-Pitts, B.
J.: Role of the reaction of stabilized Criegee intermediates with peroxy
radicals in particle formation and growth in air, Phys. Chem. Chem. Phys.,
17, 12500–12514, https://doi.org/10.1039/C5cp01171j, 2015.
Ziemann, P. J. and Atkinson, R.: Kinetics, products, and mechanisms of
secondary organic aerosol formation, Chem. Soc. Rev., 41, 6582–6605, 2012.
Short summary
A significant fraction of airborne particles, which have significant impacts on human health, visibility, and climate, are formed from the oxidation of gaseous precursors to generate low-volatility products. We show here that a sesquiterpene, α-cedrene, efficiently forms high-viscosity semisolid particles with complex composition via mechanisms that involve the highly reactive Criegee intermediate and that high molecular weight products play an important role in new particle formation.
A significant fraction of airborne particles, which have significant impacts on human health,...
Altmetrics
Final-revised paper
Preprint