Articles | Volume 13, issue 9
https://doi.org/10.5194/acp-13-5017-2013
© Author(s) 2013. 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-13-5017-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Modeling organic aerosol from the oxidation of α-pinene in a Potential Aerosol Mass (PAM) chamber
S. Chen
Department of Meteorology, Pennsylvania State University, University Park, PA, USA
W. H. Brune
Department of Meteorology, Pennsylvania State University, University Park, PA, USA
A. T. Lambe
Chemistry Department, Boston College, Chestnut Hill, MA, USA
Aerodyne Research Inc., Billerica, MA, USA
P. Davidovits
Chemistry Department, Boston College, Chestnut Hill, MA, USA
T. B. Onasch
Chemistry Department, Boston College, Chestnut Hill, MA, USA
Aerodyne Research Inc., Billerica, MA, USA
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Chenjie Yu, Edouard Pangui, Kevin Tu, Mathieu Cazaunau, Maxime Feingesicht, Landsheere Xavier, Thierry Bourrianne, Vincent Michoud, Christopher Cantrell, Timothy B. Onasch, Andrew Freedman, and Paola Formenti
Atmos. Meas. Tech., 17, 3419–3437, https://doi.org/10.5194/amt-17-3419-2024, https://doi.org/10.5194/amt-17-3419-2024, 2024
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To meet the requirements for measuring aerosol optical properties on airborne platforms and conducting dual-wavelength measurements, we introduced A2S2, an airborne dual-wavelength cavity-attenuated phase-shift single monitor. This study reports the results in the laboratory and an aircraft campaign over Paris and its surrounding regions. The results demonstrate A2S2's reliability in measuring aerosol optical properties at both wavelengths and its suitability for future aircraft campaigns.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
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Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
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.
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.
Patrick Weber, Andreas Petzold, Oliver F. Bischof, Benedikt Fischer, Marcel Berg, Andrew Freedman, Timothy B. Onasch, and Ulrich Bundke
Atmos. Meas. Tech., 15, 3279–3296, https://doi.org/10.5194/amt-15-3279-2022, https://doi.org/10.5194/amt-15-3279-2022, 2022
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In our laboratory closure study, we measured the full set of aerosol optical properties for different light-absorbing aerosols using a set of instruments.
Our key finding is that the extensive and intensive aerosol optical properties obtained agree with data from reference instruments, except the absorption Ångström exponent of externally mixed aerosols. The reported uncertainty in the single-scattering albedo fulfils the defined goals for Global Climate Observing System applications of 10 %.
Mariam Fawaz, Anita Avery, Timothy B. Onasch, Leah R. Williams, and Tami C. Bond
Atmos. Chem. Phys., 21, 15605–15618, https://doi.org/10.5194/acp-21-15605-2021, https://doi.org/10.5194/acp-21-15605-2021, 2021
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Biomass burning is responsible for 90 % of the emissions of primary organic aerosols to the atmosphere. Emissions from biomass burning sources are considered chaotic. In this work, we developed a controlled experimental approach to understand the controlling factors in emission. Our results showed that emissions are repeatable and deterministic and that emissions from wood can be constrained.
Anna L. Hodshire, Emily Ramnarine, Ali Akherati, Matthew L. Alvarado, Delphine K. Farmer, Shantanu H. Jathar, Sonia M. Kreidenweis, Chantelle R. Lonsdale, Timothy B. Onasch, Stephen R. Springston, Jian Wang, Yang Wang, Lawrence I. Kleinman, Arthur J. Sedlacek III, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 6839–6855, https://doi.org/10.5194/acp-21-6839-2021, https://doi.org/10.5194/acp-21-6839-2021, 2021
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Biomass burning emits particles and vapors that can impact both health and climate. Here, we investigate the role of dilution in the evolution of aerosol size and composition in observed US wildfire smoke plumes. Centers of plumes dilute more slowly than edges. We see differences in concentrations and composition between the centers and edges both in the first measurement and in subsequent measurements. Our findings support the hypothesis that plume dilution influences smoke aging.
Julia Perim de Faria, Ulrich Bundke, Andrew Freedman, Timothy B. Onasch, and Andreas Petzold
Atmos. Meas. Tech., 14, 1635–1653, https://doi.org/10.5194/amt-14-1635-2021, https://doi.org/10.5194/amt-14-1635-2021, 2021
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An evaluation of the performance and accuracy of a Cavity Attenuated Phase-Shift Single Scattering Albedo Monitor (CAPS PMSSA; Aerodyne Research, Inc.) was conducted in an optical-closure study with proven technologies for aerosol particle optical-property measurements. This study demonstrates that the CAPS PMSSA is a robust and reliable instrument for the direct measurement of the particle scattering and extinction coefficients and thus single-scattering albedo.
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.
Lawrence I. Kleinman, Arthur J. Sedlacek III, Kouji Adachi, Peter R. Buseck, Sonya Collier, Manvendra K. Dubey, Anna L. Hodshire, Ernie Lewis, Timothy B. Onasch, Jeffery R. Pierce, John Shilling, Stephen R. Springston, Jian Wang, Qi Zhang, Shan Zhou, and Robert J. Yokelson
Atmos. Chem. Phys., 20, 13319–13341, https://doi.org/10.5194/acp-20-13319-2020, https://doi.org/10.5194/acp-20-13319-2020, 2020
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Aerosols from wildfires affect the Earth's temperature by absorbing light or reflecting it back into space. This study investigates time-dependent chemical, microphysical, and optical properties of aerosols generated by wildfires in the Pacific Northwest, USA. Wildfire smoke plumes were traversed by an instrumented aircraft at locations near the fire and up to 3.5 h travel time downwind. Although there was no net aerosol production, aerosol particles grew and became more efficient scatters.
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
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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.
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.
Sara D. Forestieri, Taylor M. Helgestad, Andrew T. Lambe, Lindsay Renbaum-Wolff, Daniel A. Lack, Paola Massoli, Eben S. Cross, Manvendra K. Dubey, Claudio Mazzoleni, Jason S. Olfert, Arthur J. Sedlacek III, Andrew Freedman, Paul Davidovits, Timothy B. Onasch, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 12141–12159, https://doi.org/10.5194/acp-18-12141-2018, https://doi.org/10.5194/acp-18-12141-2018, 2018
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We characterized optical properties of flame-derived black carbon particles and interpret our observations through the use of Mie theory and Rayleigh–Debye–Gans theory. We determined that the mass absorption coefficient is independent of particle collapse and use this to derive theory- and wavelength-specific refractive indices for black carbon (BC). We demonstrate the inadequacy of Mie theory and suggest an alternative approach for atmospheric models to better represent light absorption by BC.
Arthur J. Sedlacek III, Peter R. Buseck, Kouji Adachi, Timothy B. Onasch, Stephen R. Springston, and Lawrence Kleinman
Atmos. Chem. Phys., 18, 11289–11301, https://doi.org/10.5194/acp-18-11289-2018, https://doi.org/10.5194/acp-18-11289-2018, 2018
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This paper presents the first direct atmospheric observations of the formation and evolution of tar balls (TBs) in forest fires collected during the Department of Energy’s Biomass Burning Observation Project (BBOP). We quantify, for the first time, the TB mass fraction in the BB plumes and show that this mass fraction increases from less than 1 % to 50 % within the first couple of hours of plume aging. Using Mie theory we find that TBs are consistent with being weak light absorbers.
Xiangyu Pei, Mattias Hallquist, Axel C. Eriksson, Joakim Pagels, Neil M. Donahue, Thomas Mentel, Birgitta Svenningsson, William Brune, and Ravi Kant Pathak
Atmos. Chem. Phys., 18, 9845–9860, https://doi.org/10.5194/acp-18-9845-2018, https://doi.org/10.5194/acp-18-9845-2018, 2018
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The findings in this study show that morphological transformation of soot occurs via two key complementary and sequential processes, i.e., void filling in the particle and its diameter growth. To quantify the state of morphological transformation, i.e., the utilization of material for filling and growth during the condensation processes, a framework was developed which can further be utilized to quantify the effect of condensed material on the optical and hygroscopic properties of soot.
Yue Zhang, Shachi Katira, Andrew Lee, Andrew T. Lambe, Timothy B. Onasch, Wen Xu, William A. Brooks, Manjula R. Canagaratna, Andrew Freedman, John T. Jayne, Doug R. Worsnop, Paul Davidovits, David Chandler, and Charles E. Kolb
Atmos. Meas. Tech., 11, 3479–3490, https://doi.org/10.5194/amt-11-3479-2018, https://doi.org/10.5194/amt-11-3479-2018, 2018
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We have adopted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols at submicron sizes and relatively low mass concentrations. Aerosol particles are deposited in the form of a thin film with interdigitated electrodes using electrostatic precipitation. Broadband dielectric spectroscopy is used to measure the kinetically controlled glass transition temperatures of glycerol and citric acid aerosols with three atmospheric relevant cooling rates.
Eben S. Cross, Leah R. Williams, David K. Lewis, Gregory R. Magoon, Timothy B. Onasch, Michael L. Kaminsky, Douglas R. Worsnop, and John T. Jayne
Atmos. Meas. Tech., 10, 3575–3588, https://doi.org/10.5194/amt-10-3575-2017, https://doi.org/10.5194/amt-10-3575-2017, 2017
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Low-cost air quality sensor technologies offer new opportunities for fast and distributed measurements of air pollution, but a persistent characterization gap remains when it comes to evaluating sensor performance under realistic environmental sampling conditions. We present results from a newly developed integrated AQ-sensor system (ARISense) and demonstrate the utility of using high-dimensional model representation to improve the conversion of raw sensor signal to ambient concentration.
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
Ellis Shipley Robinson, Timothy B. Onasch, Douglas Worsnop, and Neil M. Donahue
Atmos. Meas. Tech., 10, 1139–1154, https://doi.org/10.5194/amt-10-1139-2017, https://doi.org/10.5194/amt-10-1139-2017, 2017
Shan Zhou, Sonya Collier, Daniel A. Jaffe, Nicole L. Briggs, Jonathan Hee, Arthur J. Sedlacek III, Lawrence Kleinman, Timothy B. Onasch, and Qi Zhang
Atmos. Chem. Phys., 17, 2477–2493, https://doi.org/10.5194/acp-17-2477-2017, https://doi.org/10.5194/acp-17-2477-2017, 2017
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Wildfire plumes in the western US were sampled at a high-elevation site in summer 2013. Three distinct BBOA types were identified, representing biomass burning OA with different degrees of atmospheric processing. Analysis of consecutive BB plumes transported from the same fire source showed that photooxidation led to enhanced mass fractions of aged BBOAs but negligible net OA production. A possible reason is that SOA formation was almost entirely balanced by BBOA volatilization during transport.
Janarjan Bhandari, Swarup China, Timothy Onasch, Lindsay Wolff, Andrew Lambe, Paul Davidovits, Eben Cross, Adam Ahern, Jason Olfert, Manvendra Dubey, and Claudio Mazzoleni
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2016-270, https://doi.org/10.5194/amt-2016-270, 2016
Revised manuscript not accepted
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Soot particles emitted during the incomplete burning activities, absorb solar radiation and contribute to global warming. Light absorption by soot is also affected by its structure. To investigate whether the soot particle changes its structure or not, we used thermodenuding technique in which soot particles were passed through a heated tube (275 0C). Our study found only minor restructuring of soot suggesting no significant biases in absorption by the modification of soot structure alone.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
S. Carbone, T. Onasch, S. Saarikoski, H. Timonen, K. Saarnio, D. Sueper, T. Rönkkö, L. Pirjola, A. Häyrinen, D. Worsnop, and R. Hillamo
Atmos. Meas. Tech., 8, 4803–4815, https://doi.org/10.5194/amt-8-4803-2015, https://doi.org/10.5194/amt-8-4803-2015, 2015
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The purpose of this study was to develop a method for the quantification of trace metal content in black carbon aerosol in real time, such as combustion-related emissions, by using the SP-AMS. The properties of 13 different trace metals (Na, Al, Ca, V, Cr, Fe, Mn, Ni, Cu, Zn, Rb, Sr and Ba) were investigated in a controlled laboratory experiment. The results from the laboratory tests were applied to study fine particles in emissions of a heavy-fuel-oil-fired heating station.
A. T. Lambe, P. S. Chhabra, T. B. Onasch, W. H. Brune, J. F. Hunter, J. H. Kroll, M. J. Cummings, J. F. Brogan, Y. Parmar, D. R. Worsnop, C. E. Kolb, and P. Davidovits
Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, https://doi.org/10.5194/acp-15-3063-2015, 2015
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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
A. K. Y. Lee, M. D. Willis, R. M. Healy, T. B. Onasch, and J. P. D. Abbatt
Atmos. Chem. Phys., 15, 1823–1841, https://doi.org/10.5194/acp-15-1823-2015, https://doi.org/10.5194/acp-15-1823-2015, 2015
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Understanding the impact of black carbon (BC) particles on human health and radiative forcing requires knowledge of the BC mixing state. This work investigates the mixing state of BC and other aerosol species in a typical urban area using a single particle mass spectrometry technique. Our results provide quantitative insight into the physical and chemical nature of BC-containing particles near emission and can be used as a basis for our developing understanding of BC evolution in the atmosphere.
P. F. Liu, N. Abdelmalki, H.-M. Hung, Y. Wang, W. H. Brune, and S. T. Martin
Atmos. Chem. Phys., 15, 1435–1446, https://doi.org/10.5194/acp-15-1435-2015, https://doi.org/10.5194/acp-15-1435-2015, 2015
I. Nuaaman, S.-M. Li, K. L. Hayden, T. B. Onasch, P. Massoli, D. Sueper, D. R. Worsnop, T. S. Bates, P. K. Quinn, and R. McLaren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-2085-2015, https://doi.org/10.5194/acpd-15-2085-2015, 2015
Revised manuscript has not been submitted
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In this paper, we focus on the measurement and reporting of mass concentrations of particulate chloride and sea salt in a marine area off the coast of California using a High Resolution Aerosol Mass Spectrometer. We outline a method of deconvolving the total aerosol chloride mass into refractory and non-refractory components, previously not reported in the literature. This can be important in regions where refractory sea salt aerosols can contribute to the aerosol chloride signal measured with t
P. S. Chhabra, A. T. Lambe, M. R. Canagaratna, H. Stark, J. T. Jayne, T. B. Onasch, P. Davidovits, J. R. Kimmel, and D. R. Worsnop
Atmos. Meas. Tech., 8, 1–18, https://doi.org/10.5194/amt-8-1-2015, https://doi.org/10.5194/amt-8-1-2015, 2015
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Authors of this publication used acetate chemical ionization mass spectrometry (acetate-CIMS) to measure experimental products of alpha-pinene and naphthalene oxidation formed in a flow reactor. Acetate-CIMS instrumentation is selective toward carboxylic acid compounds which are readily formed in atmospheric photooxidation processes. Spectral information was used to identify previously measured products of both systems and to estimate their volatilities.
M. D. Willis, A. K. Y. Lee, T. B. Onasch, E. C. Fortner, L. R. Williams, A. T. Lambe, D. R. Worsnop, and J. P. D. Abbatt
Atmos. Meas. Tech., 7, 4507–4516, https://doi.org/10.5194/amt-7-4507-2014, https://doi.org/10.5194/amt-7-4507-2014, 2014
T. R. Dallmann, T. B. Onasch, T. W. Kirchstetter, D. R. Worton, E. C. Fortner, S. C. Herndon, E. C. Wood, J. P. Franklin, D. R. Worsnop, A. H. Goldstein, and R. A. Harley
Atmos. Chem. Phys., 14, 7585–7599, https://doi.org/10.5194/acp-14-7585-2014, https://doi.org/10.5194/acp-14-7585-2014, 2014
A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, and Q. Zhang
Atmos. Chem. Phys., 14, 6477–6494, https://doi.org/10.5194/acp-14-6477-2014, https://doi.org/10.5194/acp-14-6477-2014, 2014
S. E. Pusede, D. R. Gentner, P. J. Wooldridge, E. C. Browne, A. W. Rollins, K.-E. Min, A. R. Russell, J. Thomas, L. Zhang, W. H. Brune, S. B. Henry, J. P. DiGangi, F. N. Keutsch, S. A. Harrold, J. A. Thornton, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, J. Sanders, X. Ren, T. C. VandenBoer, M. Z. Markovic, A. Guha, R. Weber, A. H. Goldstein, and R. C. Cohen
Atmos. Chem. Phys., 14, 3373–3395, https://doi.org/10.5194/acp-14-3373-2014, https://doi.org/10.5194/acp-14-3373-2014, 2014
J. C. Corbin, B. Sierau, M. Gysel, M. Laborde, A. Keller, J. Kim, A. Petzold, T. B. Onasch, U. Lohmann, and A. A. Mensah
Atmos. Chem. Phys., 14, 2591–2603, https://doi.org/10.5194/acp-14-2591-2014, https://doi.org/10.5194/acp-14-2591-2014, 2014
G. M. Buffaloe, D. A. Lack, E. J. Williams, D. Coffman, K. L. Hayden, B. M. Lerner, S.-M. Li, I. Nuaaman, P. Massoli, T. B. Onasch, P. K. Quinn, and C. D. Cappa
Atmos. Chem. Phys., 14, 1881–1896, https://doi.org/10.5194/acp-14-1881-2014, https://doi.org/10.5194/acp-14-1881-2014, 2014
C. D. Cappa, E. J. Williams, D. A. Lack, G. M. Buffaloe, D. Coffman, K. L. Hayden, S. C. Herndon, B. M. Lerner, S.-M. Li, P. Massoli, R. McLaren, I. Nuaaman, T. B. Onasch, and P. K. Quinn
Atmos. Chem. Phys., 14, 1337–1352, https://doi.org/10.5194/acp-14-1337-2014, https://doi.org/10.5194/acp-14-1337-2014, 2014
L. R. Williams, L. A. Gonzalez, J. Peck, D. Trimborn, J. McInnis, M. R. Farrar, K. D. Moore, J. T. Jayne, W. A. Robinson, D. K. Lewis, T. B. Onasch, M. R. Canagaratna, A. Trimborn, M. T. Timko, G. Magoon, R. Deng, D. Tang, E. de la Rosa Blanco, A. S. H. Prévôt, K. A. Smith, and D. R. Worsnop
Atmos. Meas. Tech., 6, 3271–3280, https://doi.org/10.5194/amt-6-3271-2013, https://doi.org/10.5194/amt-6-3271-2013, 2013
A. M. Ortega, D. A. Day, M. J. Cubison, W. H. Brune, D. Bon, J. A. de Gouw, and J. L. Jimenez
Atmos. Chem. Phys., 13, 11551–11571, https://doi.org/10.5194/acp-13-11551-2013, https://doi.org/10.5194/acp-13-11551-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
A. Petzold, T. Onasch, P. Kebabian, and A. Freedman
Atmos. Meas. Tech., 6, 1141–1151, https://doi.org/10.5194/amt-6-1141-2013, https://doi.org/10.5194/amt-6-1141-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
The surface tension and CCN activation of sea spray aerosol particles
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain: Insights from six-year simulations
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Exploring the processes controlling secondary inorganic aerosol: Evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Critical Load Exceedances for North America and Europe using an Ensemble of Models and an Investigation of Causes for Environmental Impact Estimate Variability: An AQMEII4 Study
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
EGUsphere, https://doi.org/10.5194/egusphere-2024-2838, https://doi.org/10.5194/egusphere-2024-2838, 2024
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We model the CCN activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updrafts.
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2704, https://doi.org/10.5194/egusphere-2024-2704, 2024
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This study use the WRF-Chem model to assess how meteorological conditions and unexpected emission reductions affected PM2.5 in the North China Plain (NCP). It highlights regional disparities: in the Northern NCP, adverse weather negated emission reduction effects. In contrast, the Southern NCP with PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology and air quality.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Olivia G. Norman, Colette L. Heald, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz-Ozdemir, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Iannis Koutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark Shephard, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2024-2226, https://doi.org/10.5194/egusphere-2024-2226, 2024
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The large range of sulphur and nitrogen deposition estimates from air-quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulphur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by droplets, rain, snow, etc., aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, and gas deposition via plant cuticles and soil.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters, is improved.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1579, https://doi.org/10.5194/egusphere-2024-1579, 2024
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol-radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are -0.11 and +0.17 W/m², respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Cited articles
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Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012b.
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Kang, E., Root, M. J., Toohey, D. W., and Brune, W. H.: Introducing the concept of Potential Aerosol Mass (PAM), Atmos. Chem. Phys., 7, 5727–5744, https://doi.org/10.5194/acp-7-5727-2007, 2007.
Kroll, J. H., Chan, A. W. H., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.: Reactions of Semivolatile Organics and Their Effects on Secondary Organic Aerosol Formation, Environ. Sci. Technol., 41, 3545–3550, 2007.
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Kroll, J. H., Donahue, N. M., Jimenez, J. L., Kessler, S. H., Canagaratna, M. R., Wilson, K. R., Altieri, K. E., Mazzoleni, L. R., Wozniak, A. S., Bluhm, H., Mysak, E. R., Smith, J. D., Kolb, C. E., and Worsnop, D. R.: Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol, Nat. Chem., 3, 133–139, 2011.
Lambe, A. T., Ahern, A. T., Williams, L. R., Slowik, J. G., Wong, J. P. S., Abbatt, J. P. D., Brune, W. H., Ng, N. L., Wright, J. P., Croasdale, D. R., Worsnop, D. R., Davidovits, P., and Onasch, T. B.: Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements, Atmos. Meas. Tech., 4, 445–461, https://doi.org/10.5194/amt-4-445-2011, 2011.
Lambe, A. T., Onasch, T. B., Croasdale, D. R., Wright, J. P., Martin, A. T., Franklin, J. P., Massoli, P., Kroll, J. H., Canagaratna, M. R., Brune, W. H., Worsnop, D. R., and Davidovits, P.: Transitions from Functionalization to Fragmentation Reactions of Laboratory Secondary Organic Aerosol (SOA) Generated from the OH Oxidation of Alkane Precursors, Environ. Sci. Technol., 46, 5430–5437, 2012.
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Mao, J., Ren, X., Brune, W. H., Olson, J. R., Crawford, J. H., Fried, A., Huey, L. G., Cohen, R. C., Heikes, B., Singh, H. B., Blake, D. R., Sachse, G. W., Diskin, G. S., Hall, S. R., and Shetter, R. E.: Airborne measurement of OH reactivity during INTEX-B, Atmos. Chem. Phys., 9, 163–173, https://doi.org/10.5194/acp-9-163-2009, 2009.
Massoli, P., Lambe, A. T., Ahern, A. T., Williams, L. R., Ehn, M., Mikkilä, J., Canagaratna, M. R., Brune, W. H., Onasch, T. B., Jayne, J. T., Petäjä, T., Kulmala, M., Laaksonen, A., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles, Geophys. Res. Lett., 37, L24801, https://doi.org/10.1029/2010GL045258, 2010.
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