Articles | Volume 15, issue 24
https://doi.org/10.5194/acp-15-13915-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-13915-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Biomass burning emissions and potential air quality impacts of volatile organic compounds and other trace gases from fuels common in the US
J. B. Gilman
CORRESPONDING AUTHOR
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
B. M. Lerner
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
W. C. Kuster
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
retired
P. D. Goldan
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
retired
C. Warneke
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
P. R. Veres
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
J. M. Roberts
NOAA Earth System Research Laboratory, Boulder, CO, USA
J. A. de Gouw
CIRES at University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Boulder, CO, USA
I. R. Burling
Department of Chemistry, University of Montana, Missoula, Montana, USA
now at: Cytec Canada, Niagara Falls, Ontario, Canada
R. J. Yokelson
Department of Chemistry, University of Montana, Missoula, Montana, USA
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Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
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Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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Kanako Sekimoto, Abigail R. Koss, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Carsten Warneke, Robert J. Yokelson, James M. Roberts, and Joost de Gouw
Atmos. Chem. Phys., 18, 9263–9281, https://doi.org/10.5194/acp-18-9263-2018, https://doi.org/10.5194/acp-18-9263-2018, 2018
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We found that on average 85 % of the VOC emissions from biomass burning across various fuels representative of the western US (including various coniferous and chaparral fuels) can be explained using only two emission profiles: (i) a high-temperature pyrolysis profile and (ii) a low-temperature pyrolysis profile. The high-temperature profile is quantitatively similar between different fuel types (r2 > 0.84), and likewise for the low-temperature profile.
Roya Bahreini, Ravan Ahmadov, Stu A. McKeen, Kennedy T. Vu, Justin H. Dingle, Eric C. Apel, Donald R. Blake, Nicola Blake, Teresa L. Campos, Chris Cantrell, Frank Flocke, Alan Fried, Jessica B. Gilman, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Brian M. Lerner, Roy L. Mauldin, Simone Meinardi, Denise D. Montzka, Dirk Richter, Jason R. Schroeder, Meghan Stell, David Tanner, James Walega, Peter Weibring, and Andrew Weinheimer
Atmos. Chem. Phys., 18, 8293–8312, https://doi.org/10.5194/acp-18-8293-2018, https://doi.org/10.5194/acp-18-8293-2018, 2018
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We measured organic aerosol (OA) and relevant trace gases during FRAPPÉ in the Colorado Front Range, with the goal of characterizing summertime OA formation. Our results indicate a significant production of secondary OA (SOA) in this region. About 2 μg m−3 of OA was present at background CO levels, suggesting contribution of non-combustion sources to SOA. Contribution of oil- and gas-related activities to anthropogenic SOA was modeled to be ~38 %. Biogenic SOA contributed to >40 % of OA.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Catalina Tsai, Max Spolaor, Santo Fedele Colosimo, Olga Pikelnaya, Ross Cheung, Eric Williams, Jessica B. Gilman, Brian M. Lerner, Robert J. Zamora, Carsten Warneke, James M. Roberts, Ravan Ahmadov, Joost de Gouw, Timothy Bates, Patricia K. Quinn, and Jochen Stutz
Atmos. Chem. Phys., 18, 1977–1996, https://doi.org/10.5194/acp-18-1977-2018, https://doi.org/10.5194/acp-18-1977-2018, 2018
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Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH). Vertical HONO fluxes, observed in the snow-free, wintertime Uintah Basin, Utah, USA, show that chemical formation of HONO on the ground closes the HONO budget. Under high NOx conditions, HONO formation is most likely due to photo-enhanced conversion of NO2 on the ground. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the most likely source of HONO.
Robert C. Rhew, Malte Julian Deventer, Andrew A. Turnipseed, Carsten Warneke, John Ortega, Steve Shen, Luis Martinez, Abigail Koss, Brian M. Lerner, Jessica B. Gilman, James N. Smith, Alex B. Guenther, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 13417–13438, https://doi.org/10.5194/acp-17-13417-2017, https://doi.org/10.5194/acp-17-13417-2017, 2017
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Alkenes emanate from both natural and anthropogenic sources and can contribute to atmospheric ozone production. This study measured
lightalkene (ethene, propene and butene) fluxes from a ponderosa pine forest using a novel relaxed eddy accumulation method, revealing much larger emissions than previously estimated and accounting for a significant fraction of OH reactivity. Emissions have a diurnal cycle related to sunlight and temperature, and the forest canopy appears to be the source.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313, https://doi.org/10.5194/amt-10-291-2017, https://doi.org/10.5194/amt-10-291-2017, 2017
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Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Bin Yuan, Abigail Koss, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Harald Stark, and Joost A. de Gouw
Atmos. Meas. Tech., 9, 2735–2752, https://doi.org/10.5194/amt-9-2735-2016, https://doi.org/10.5194/amt-9-2735-2016, 2016
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We present the development of a hydronium (H3O+) time of flight chemical ionization mass spectrometer (H3O+ ToF-CIMS). We characterize the humidity dependence of the reagent ions and VOC signals in details. The low mass cutoff issue of RF-only quadrupole leads to unusual humidity dependence of reagent ions. The new H3O+ ToF-CIMS was successfully deployed on the NOAA WP-3D research aircraft for the SONGNEX campaign in 2015 and some initial results from the SONGNEX campaign are presented.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
Bin Yuan, John Liggio, Jeremy Wentzell, Shao-Meng Li, Harald Stark, James M. Roberts, Jessica Gilman, Brian Lerner, Carsten Warneke, Rui Li, Amy Leithead, Hans D. Osthoff, Robert Wild, Steven S. Brown, and Joost A. de Gouw
Atmos. Chem. Phys., 16, 2139–2153, https://doi.org/10.5194/acp-16-2139-2016, https://doi.org/10.5194/acp-16-2139-2016, 2016
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We describe high-resolution measurements of nitrated phenols using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS). Strong diurnal profiles were observed for nitrated phenols, with concentration maxima at night. Box model simulations were able to reproduce the measured nitrated phenols.
R. J. Wild, P. M. Edwards, T. S. Bates, R. C. Cohen, J. A. de Gouw, W. P. Dubé, J. B. Gilman, J. Holloway, J. Kercher, A. R. Koss, L. Lee, B. M. Lerner, R. McLaren, P. K. Quinn, J. M. Roberts, J. Stutz, J. A. Thornton, P. R. Veres, C. Warneke, E. Williams, C. J. Young, B. Yuan, K. J. Zarzana, and S. S. Brown
Atmos. Chem. Phys., 16, 573–583, https://doi.org/10.5194/acp-16-573-2016, https://doi.org/10.5194/acp-16-573-2016, 2016
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High wintertime ozone levels have been observed in the Uintah Basin, Utah, a sparsely populated rural region with intensive oil and gas operations. The reactive nitrogen budget plays an important role in tropospheric ozone formation, and we find that nighttime chemistry has a large effect on its partitioning. Much of the oxidation of reactive nitrogen during a high-ozone year occurred via heterogeneous uptake onto aerosol at night, keeping NOx at concentrations comparable to a low-ozone year.
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
A. R. Koss, J. de Gouw, C. Warneke, J. B. Gilman, B. M. Lerner, M. Graus, B. Yuan, P. Edwards, S. S. Brown, R. Wild, J. M. Roberts, T. S. Bates, and P. K. Quinn
Atmos. Chem. Phys., 15, 5727–5741, https://doi.org/10.5194/acp-15-5727-2015, https://doi.org/10.5194/acp-15-5727-2015, 2015
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Extraction of natural gas and oil is associated with a range of possible atmospheric environmental issues. Here we present an analysis of gas-phase hydrocarbon measurements taken in an oil and natural gas extraction area in Utah during a period of high wintertime ozone. We are able to constrain important chemical parameters related to emission sources and rates, hydrocarbon photochemistry, and VOC composition.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
L. Lee, P. J. Wooldridge, J. B. Gilman, C. Warneke, J. de Gouw, and R. C. Cohen
Atmos. Chem. Phys., 14, 12441–12454, https://doi.org/10.5194/acp-14-12441-2014, https://doi.org/10.5194/acp-14-12441-2014, 2014
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Alkyl nitrate formation is known to be an important sink of NOx in a wide range of environments. In a study in the Uintah basin in 2012, we find that formation of these compounds represents a more rapid NOx (NO + NO2) sink than does nitric acid formation. This rapid formation is in large part due to the low mean temperature (~0°C) during the study and is consistent with laboratory observations.
C. Warneke, F. Geiger, P. M. Edwards, W. Dube, G. Pétron, J. Kofler, A. Zahn, S. S. Brown, M. Graus, J. B. Gilman, B. M. Lerner, J. Peischl, T. B. Ryerson, J. A. de Gouw, and J. M. Roberts
Atmos. Chem. Phys., 14, 10977–10988, https://doi.org/10.5194/acp-14-10977-2014, https://doi.org/10.5194/acp-14-10977-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
T. P. Riedel, G. M. Wolfe, K. T. Danas, J. B. Gilman, W. C. Kuster, D. M. Bon, A. Vlasenko, S.-M. Li, E. J. Williams, B. M. Lerner, P. R. Veres, J. M. Roberts, J. S. Holloway, B. Lefer, S. S. Brown, and J. A. Thornton
Atmos. Chem. Phys., 14, 3789–3800, https://doi.org/10.5194/acp-14-3789-2014, https://doi.org/10.5194/acp-14-3789-2014, 2014
C. J. Young, R. A. Washenfelder, P. M. Edwards, D. D. Parrish, J. B. Gilman, W. C. Kuster, L. H. Mielke, H. D. Osthoff, C. Tsai, O. Pikelnaya, J. Stutz, P. R. Veres, J. M. Roberts, S. Griffith, S. Dusanter, P. S. Stevens, J. Flynn, N. Grossberg, B. Lefer, J. S. Holloway, J. Peischl, T. B. Ryerson, E. L. Atlas, D. R. Blake, and S. S. Brown
Atmos. Chem. Phys., 14, 3427–3440, https://doi.org/10.5194/acp-14-3427-2014, https://doi.org/10.5194/acp-14-3427-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 2014
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
D. A. Lack, R. Bahreini, J. M. Langridge, J. B. Gilman, and A. M. Middlebrook
Atmos. Chem. Phys., 13, 2415–2422, https://doi.org/10.5194/acp-13-2415-2013, https://doi.org/10.5194/acp-13-2415-2013, 2013
R. J. Yokelson, I. R. Burling, J. B. Gilman, C. Warneke, C. E. Stockwell, J. de Gouw, S. K. Akagi, S. P. Urbanski, P. Veres, J. M. Roberts, W. C. Kuster, J. Reardon, D. W. T. Griffith, T. J. Johnson, S. Hosseini, J. W. Miller, D. R. Cocker III, H. Jung, and D. R. Weise
Atmos. Chem. Phys., 13, 89–116, https://doi.org/10.5194/acp-13-89-2013, https://doi.org/10.5194/acp-13-89-2013, 2013
Samiha Binte Shahid, Forrest G. Lacey, Christine Wiedinmyer, Robert J. Yokelson, and Kelley C. Barsanti
Geosci. Model Dev., 17, 7679–7711, https://doi.org/10.5194/gmd-17-7679-2024, https://doi.org/10.5194/gmd-17-7679-2024, 2024
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The Next-generation Emissions InVentory expansion of Akagi (NEIVA) v.1.0 is a comprehensive biomass burning emissions database that allows integration of new data and flexible querying. Data are stored in connected datasets, including recommended averages of ~1500 constituents for 14 globally relevant fire types. Individual compounds were mapped to common model species to allow better attribution of emissions in modeling studies that predict the effects of fires on air quality and climate.
Michael F. Link, Megan S. Claflin, Christina E. Cecelski, Ayomide A. Akande, Delaney Kilgour, Paul A. Heine, Matthew Coggon, Chelsea E. Stockwell, Andrew Jensen, Jie Yu, Han N. Huynh, Jenna C. Ditto, Carsten Warneke, William Dresser, Keighan Gemmell, Spiro Jorga, Rileigh L. Robertson, Joost de Gouw, Timothy Bertram, Jonathan P. D. Abbatt, Nadine Borduas-Dedekind, and Dustin Poppendieck
EGUsphere, https://doi.org/10.5194/egusphere-2024-3132, https://doi.org/10.5194/egusphere-2024-3132, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Proton-transfer-reaction mass spectrometry (PTR-MS) is widely used for the measurement of volatile organic compounds (VOCs) both indoors and outdoors. An analytical challenge for PTR-MS measurements is the formation of unintended measurement interferences, product ion distributions (PIDs), that may appear in the data as VOCs of interest. We developed a method for quantifying PID formation and use interlaboratory comparison data to put quantitative constraints on PID formation.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
EGUsphere, https://doi.org/10.5194/egusphere-2024-2752, https://doi.org/10.5194/egusphere-2024-2752, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
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High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
Edward J. Strobach, Sunil Baidar, Brian J. Carroll, Steven S. Brown, Kristen Zuraski, Matthew Coggon, Chelsea E. Stockwell, Lu Xu, Yelena L. Pichugina, W. Alan Brewer, Carsten Warneke, Jeff Peischl, Jessica Gilman, Brandi McCarty, Maxwell Holloway, and Richard Marchbanks
Atmos. Chem. Phys., 24, 9277–9307, https://doi.org/10.5194/acp-24-9277-2024, https://doi.org/10.5194/acp-24-9277-2024, 2024
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Large-scale weather patterns are isolated from local patterns to study the impact that different weather scales have on air quality measurements. While impacts from large-scale meteorology were evaluated by separating ozone (O3) exceedance (>70 ppb) and non-exceedance (<70 ppb) days, we developed a technique that allows direct comparisons of small temporal variations between chemical and dynamics measurements under rapid dynamical transitions.
Alexander C. Bradley, Barbara Dix, Fergus Mackenzie, J. Pepijn Veefkind, and Joost A. de Gouw
EGUsphere, https://doi.org/10.5194/egusphere-2024-2352, https://doi.org/10.5194/egusphere-2024-2352, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Currently measurement of methane from the TROPOMI satellite is biased with respect to surface reflectance. This study demonstrates a new method of correcting for this bias on a seasonal timescale to allow for differences in surface reflectance in areas of intense agriculture where growing seasons may introduce a reflectance bias. We have successfully implemented this technique in the Denver-Julesburg basin where agriculture and methane extraction infrastructure is often co-located.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1899, https://doi.org/10.5194/egusphere-2024-1899, 2024
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking are important sources that impact air quality. This study used a model to evaluate how these emissions impact ozone in the Los Angeles Basin, and quantifies the impact of gaseous cooking emissions for the first time. Accurate representation of these and other man-made sources in inventories is crucial to inform effective air quality policies.
Zachary Finewax, Aparajeo Chattopadhyay, J. Andrew Neuman, James Roberts, and James Burkholder
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-94, https://doi.org/10.5194/amt-2024-94, 2024
Revised manuscript accepted for AMT
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This work provides a comprehensive sensitivity calibration of a chemical ionization instrument commonly used in field measurements for the measurement of the toxic isomers methyl isocyanate and hydroxyacetonitrile that are found in the atmosphere. The results from this work has demonstrated that the hydroyacetonitrile isomer was observed in previous field studies rather than the stated identification of methyl isocyanate.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
Atmos. Chem. Phys., 24, 3729–3742, https://doi.org/10.5194/acp-24-3729-2024, https://doi.org/10.5194/acp-24-3729-2024, 2024
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOCs generated by the ozonolysis of surface seawater are competitive with biological VOC production and emission.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
Atmos. Chem. Phys., 24, 3421–3443, https://doi.org/10.5194/acp-24-3421-2024, https://doi.org/10.5194/acp-24-3421-2024, 2024
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We measured cyanogen bromide (BrCN) in the troposphere for the first time. BrCN is a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments and is a previously unrecognized sink for active Br compounds. BrCN has an apparent lifetime against heterogeneous loss in the range 1–10 d, so it serves as a cumulative marker of Br-radical chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Andrew R. Jensen, Abigail R. Koss, Ryder B. Hales, and Joost A. de Gouw
Atmos. Meas. Tech., 16, 5261–5285, https://doi.org/10.5194/amt-16-5261-2023, https://doi.org/10.5194/amt-16-5261-2023, 2023
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Quantification of a wide range of volatile organic compounds by proton-transfer-reaction mass spectrometry (PTR-MS) can be achieved with direct calibration of only a subset of compounds, characterization of instrument response, and simple reaction kinetics. We characterized our Vocus PTR-MS and developed a toolkit as a guide through this process. A catalytic zero air generator provided the lowest detection limits, and short, frequent calibrations informed variability in instrument response.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
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The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Michael P. Vermeuel, Gordon A. Novak, Delaney B. Kilgour, Megan S. Claflin, Brian M. Lerner, Amy M. Trowbridge, Jonathan Thom, Patricia A. Cleary, Ankur R. Desai, and Timothy H. Bertram
Atmos. Chem. Phys., 23, 4123–4148, https://doi.org/10.5194/acp-23-4123-2023, https://doi.org/10.5194/acp-23-4123-2023, 2023
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Reactive carbon species emitted from natural sources such as forests play an important role in the chemistry of the atmosphere. Predictions of these emissions are based on plant responses during the growing season and do not consider potential effects from seasonal changes. To address this, we made measurements of reactive carbon over a forest during the summer to autumn transition. We learned that observed concentrations and emissions for some key species are larger than model predictions.
John W. Halfacre, Jordan Stewart, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Michael Flynn, Stephen J. Andrews, Steven S. Brown, Patrick R. Veres, and Pete M. Edwards
Atmos. Meas. Tech., 16, 1407–1429, https://doi.org/10.5194/amt-16-1407-2023, https://doi.org/10.5194/amt-16-1407-2023, 2023
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This study details a new sampling method for the optical detection of hydrogen chloride (HCl). HCl is an important atmospheric reservoir for chlorine atoms, which can affect nitrogen oxide cycling and the lifetimes of volatile organic compounds and ozone. However, HCl has a high affinity for interacting with surfaces, thereby preventing fast, quantitative measurements. The sampling technique in this study minimizes these surface interactions and provides a high-quality measurement of HCl.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Sungwoo Kim, Brian M. Lerner, Donna T. Sueper, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 15, 5061–5075, https://doi.org/10.5194/amt-15-5061-2022, https://doi.org/10.5194/amt-15-5061-2022, 2022
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Atmospheric samples can be complex, and current analysis methods often require substantial human interaction and discard potentially important information. To improve analysis accuracy and computational cost of these large datasets, we developed an automated analysis algorithm that utilizes a factor analysis approach coupled with a decision tree. We demonstrate that this algorithm cataloged approximately 10 times more analytes compared to a manual analysis and in a quarter of the analysis time.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
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California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Robert J. Yokelson, Bambang H. Saharjo, Chelsea E. Stockwell, Erianto I. Putra, Thilina Jayarathne, Acep Akbar, Israr Albar, Donald R. Blake, Laura L. B. Graham, Agus Kurniawan, Simone Meinardi, Diah Ningrum, Ati D. Nurhayati, Asmadi Saad, Niken Sakuntaladewi, Eko Setianto, Isobel J. Simpson, Elizabeth A. Stone, Sigit Sutikno, Andri Thomas, Kevin C. Ryan, and Mark A. Cochrane
Atmos. Chem. Phys., 22, 10173–10194, https://doi.org/10.5194/acp-22-10173-2022, https://doi.org/10.5194/acp-22-10173-2022, 2022
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Fire plus non-fire GHG emissions associated with draining peatlands are the largest per area of any land use change considered by the IPCC. To characterize average and variability for tropical peat fire emissions, highly mobile smoke sampling teams were deployed across four Indonesian provinces to explore an extended interannual, climatic, and spatial range. Large adjustments to IPCC-recommended emissions are suggested. Lab data bolster an extensive emissions database for tropical peat fires.
Michael A. Robinson, J. Andrew Neuman, L. Gregory Huey, James M. Roberts, Steven S. Brown, and Patrick R. Veres
Atmos. Meas. Tech., 15, 4295–4305, https://doi.org/10.5194/amt-15-4295-2022, https://doi.org/10.5194/amt-15-4295-2022, 2022
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Iodide chemical ionization mass spectrometry (CIMS) is commonly used in atmospheric chemistry laboratory studies and field campaigns. Deployment of the NOAA iodide CIMS instrument in the summer of 2021 indicated a significant and overlooked temperature dependence of the instrument sensitivity. This work explores which analytes are influenced by this phenomena. Additionally, we recommend controls to reduce this effect for future field deployments.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Kun Zhang, Zhiqiang Liu, Xiaojuan Zhang, Qing Li, Andrew Jensen, Wen Tan, Ling Huang, Yangjun Wang, Joost de Gouw, and Li Li
Atmos. Chem. Phys., 22, 4853–4866, https://doi.org/10.5194/acp-22-4853-2022, https://doi.org/10.5194/acp-22-4853-2022, 2022
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A significant increase in O3 concentrations was found during the lockdown period of COVID-19 in most areas of China. By field measurements coupled with machine learning, an observation-based model (OBM) and sensitivity analysis, we found the changes in the NOx / VOC ratio were a key reason for the significant rise in O3. To restrain O3 pollution, more efforts should be devoted to the control of anthropogenic OVOCs, alkenes and aromatics.
Martin Breitenlechner, Gordon A. Novak, J. Andrew Neuman, Andrew W. Rollins, and Patrick R. Veres
Atmos. Meas. Tech., 15, 1159–1169, https://doi.org/10.5194/amt-15-1159-2022, https://doi.org/10.5194/amt-15-1159-2022, 2022
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We coupled a new ion source to a commercially available state-of-the-art trace gas analyzer. The instrument is particularly well suited for conducting high-altitude observations, addressing the challenges of low ambient pressures and a complex sample matrix. The new instrument and ion source provides significant advantages to more traditional modes of operation, without sacrificing the sensitivity and flexibility of this technique.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
James M. Roberts
Atmos. Chem. Phys., 21, 16793–16795, https://doi.org/10.5194/acp-21-16793-2021, https://doi.org/10.5194/acp-21-16793-2021, 2021
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This comment provides evidence that recently reported measurements of the isotope composition of wildfire-derived oxides of nitrogen have a significant interference from other nitrogen compounds. In addition, the conceptual model used to interpret the results was missing several key reactions.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Teles C. Furlani, Patrick R. Veres, Kathryn E. R. Dawe, J. Andrew Neuman, Steven S. Brown, Trevor C. VandenBoer, and Cora J. Young
Atmos. Meas. Tech., 14, 5859–5871, https://doi.org/10.5194/amt-14-5859-2021, https://doi.org/10.5194/amt-14-5859-2021, 2021
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This study characterized and validated a commercial spectroscopic instrument for the measurement of hydrogen chloride (HCl) in the atmosphere. Near the Earth’s surface, HCl acts as the dominant reservoir for other chlorine-containing reactive chemicals that play an important role in atmospheric chemistry. The properties of HCl make it challenging to measure. This instrument can overcome many of these challenges, enabling reliable HCl measurements.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
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.
Melodie Lao, Leigh R. Crilley, Leyla Salehpoor, Teles C. Furlani, Ilann Bourgeois, J. Andrew Neuman, Andrew W. Rollins, Patrick R. Veres, Rebecca A. Washenfelder, Caroline C. Womack, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 13, 5873–5890, https://doi.org/10.5194/amt-13-5873-2020, https://doi.org/10.5194/amt-13-5873-2020, 2020
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Nitrous acid (HONO) is a key intermediate in the generation of oxidants and fate of nitrogen oxides in the atmosphere. High-purity calibration sources that produce stable atmospherically relevant levels under field conditions have not been made to date, reducing measurement accuracy. In this study a simple salt-coated tube humidified with water vapor is demonstrated to produce pure stable low levels of HONO, with modifications allowing the generation of higher amounts.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
James M. Roberts, Chelsea E. Stockwell, Robert J. Yokelson, Joost de Gouw, Yong Liu, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, Kyle J. Zarzana, Steven S. Brown, Cristina Santin, Stefan H. Doerr, and Carsten Warneke
Atmos. Chem. Phys., 20, 8807–8826, https://doi.org/10.5194/acp-20-8807-2020, https://doi.org/10.5194/acp-20-8807-2020, 2020
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We measured total reactive nitrogen, Nr, in lab fires from western North American fuels, along with measurements of individual nitrogen compounds. We measured the amount of N that gets converted to inactive compounds (avg. 70 %), and the amount that is accounted for by individual species (85 % of remaining N). We provide guidelines for how the reactive nitrogen is distributed among individual compounds such as NOx and ammonia. This will help estimates and predictions of wildfire emissions.
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.
Yi Ji, L. Gregory Huey, David J. Tanner, Young Ro Lee, Patrick R. Veres, J. Andrew Neuman, Yuhang Wang, and Xinming Wang
Atmos. Meas. Tech., 13, 3683–3696, https://doi.org/10.5194/amt-13-3683-2020, https://doi.org/10.5194/amt-13-3683-2020, 2020
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A common way of measuring trace gases in the atmosphere is chemical ionization mass spectrometry. One large drawback of these instruments is that they require radioactive ion sources. In this work we demonstrate a simple ion source that uses a small krypton lamp that can be used to replace a radioactive source.
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
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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.
Lauren T. Fleming, Peng Lin, James M. Roberts, Vanessa Selimovic, Robert Yokelson, Julia Laskin, Alexander Laskin, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, https://doi.org/10.5194/acp-20-1105-2020, 2020
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We have explored the nature and stability of molecules that give biomass burning smoke its faint brown color. Different types of biomass fuels were burned and the resulting smoke was collected for a detailed chemical analysis. We found that brown molecules in smoke become less colored when they are irradiated by sunlight, but this photobleaching process is very slow. This means that biomass burning smoke will remain brown-colored for a long time and efficiently warm up the atmosphere.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Jiajue Chai, David J. Miller, Eric Scheuer, Jack Dibb, Vanessa Selimovic, Robert Yokelson, Kyle J. Zarzana, Steven S. Brown, Abigail R. Koss, Carsten Warneke, and Meredith Hastings
Atmos. Meas. Tech., 12, 6303–6317, https://doi.org/10.5194/amt-12-6303-2019, https://doi.org/10.5194/amt-12-6303-2019, 2019
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Isotopic analysis offers a potential tool to distinguish between sources and interpret transformation pathways of atmospheric species. We applied recently developed techniques in our lab to characterize the isotopic composition of reactive nitrogen species (NOx, HONO, HNO3, pNO3-) in fresh biomass burning emissions. Intercomparison with other techniques confirms the suitability of our methods, allowing for future applications of our techniques in a variety of environments.
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
Benjamin L. Deming, Demetrios Pagonis, Xiaoxi Liu, Douglas A. Day, Ranajit Talukdar, Jordan E. Krechmer, Joost A. de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 12, 3453–3461, https://doi.org/10.5194/amt-12-3453-2019, https://doi.org/10.5194/amt-12-3453-2019, 2019
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Losses or measurement delays of gas-phase compounds sampled through tubing are important to atmospheric science. Here we characterize 14 tubing materials by measuring the effects on step changes in organic compound concentration. We find that polymeric tubings exhibit absorptive partitioning behaviour while glass and metal tubings show adsorptive partitioning. Adsorptive materials impart complex humidity, concentration, and VOC–VOC interaction dependencies that absorptive tubings do not.
Min Zhong, Eri Saikawa, Alexander Avramov, Chen Chen, Boya Sun, Wenlu Ye, William C. Keene, Robert J. Yokelson, Thilina Jayarathne, Elizabeth A. Stone, Maheswar Rupakheti, and Arnico K. Panday
Atmos. Chem. Phys., 19, 8209–8228, https://doi.org/10.5194/acp-19-8209-2019, https://doi.org/10.5194/acp-19-8209-2019, 2019
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Air pollution is one of the most pressing environmental issues in the Kathmandu Valley, the capital city of Nepal. We estimated emissions from two of the major source types in the valley (vehicles and brick kilns) and found that they have significant impacts on air quality surrounding the valley. Our results highlight the importance of improving local emissions estimates for air quality modeling.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
James M. Roberts and Yong Liu
Atmos. Chem. Phys., 19, 4419–4437, https://doi.org/10.5194/acp-19-4419-2019, https://doi.org/10.5194/acp-19-4419-2019, 2019
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Condensed-phase reactions are important removal processes for reduced nitrogen species, isocyanic acid (HNCO), methyl isocyanate (CH3NCO), and cyanogen halides (XCN, X = Cl, Br, I). This chemistry is not well understood, so we measured aqueous-phase solubilities and reaction rates under a range of temperatures and conditions and in n-octanol, a proxy for non-polar media and biological membranes. The results were used to estimate atmospheric removal rates and fates of these nitrogen compounds.
Vanessa Selimovic, Robert J. Yokelson, Gavin R. McMeeking, and Sarah Coefield
Atmos. Chem. Phys., 19, 3905–3926, https://doi.org/10.5194/acp-19-3905-2019, https://doi.org/10.5194/acp-19-3905-2019, 2019
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A massive wildfire smoke episode impacted the western US and Canada in summer 2017. We measured CO, other trace gases, PM, BC, and aerosol optical properties at a heavily impacted, ground-based site affected by this event. Brown carbon diminished as smoke aged but was a persistent component of the regional smoke, accounting for about half of aerosol absorption at 401 nm on average. The PM / CO ratios suggested aerosol evaporation was dominant at the surface at smoke ages of up to ~ 1–2 days.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Daniel C. Anderson, Jessica Pavelec, Conner Daube, Scott C. Herndon, Walter B. Knighton, Brian M. Lerner, J. Robert Roscioli, Tara I. Yacovitch, and Ezra C. Wood
Atmos. Chem. Phys., 19, 2845–2860, https://doi.org/10.5194/acp-19-2845-2019, https://doi.org/10.5194/acp-19-2845-2019, 2019
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San Antonio is one of the largest cities in the United States and is in non-attainment of the 8 h ozone standard. Using the Aerodyne Mobile Laboratory, we made observations of ozone and its precursors at three sites in the San Antonio region to determine the main drivers of its production. We found that compounds produced by plants were the dominant organic compound for ozone production and that to limit ozone production at the study site, emissions of nitrogen oxides should be reduced.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Coty N. Jen, Lindsay E. Hatch, Vanessa Selimovic, Robert J. Yokelson, Robert Weber, Arantza E. Fernandez, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 19, 1013–1026, https://doi.org/10.5194/acp-19-1013-2019, https://doi.org/10.5194/acp-19-1013-2019, 2019
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Wildfires in the western US are occurring more frequently and burning larger land areas. Smoke from these fires will play a greater role in regional air quality and atmospheric chemistry than in the past. To help fire and climate modelers and atmospheric experimentalists better understand how smoke impacts the environment, we have separated, identified, classified, and quantified the thousands of organic compounds found in smoke and related their amounts emitted to fire conditions.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Kyle J. Zarzana, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, William P. Dubé, Robert J. Yokelson, Carsten Warneke, Joost A. de Gouw, James M. Roberts, and Steven S. Brown
Atmos. Chem. Phys., 18, 15451–15470, https://doi.org/10.5194/acp-18-15451-2018, https://doi.org/10.5194/acp-18-15451-2018, 2018
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Emissions of glyoxal and methylglyoxal from fuels common to the western United States were measured using cavity-enhanced spectroscopy, which provides a more selective measurement of those compounds than was previously available. Primary emissions of glyoxal were lower than previously reported and showed variability between the different fuel groups. However, emissions of glyoxal relative to formaldehyde were constant across almost all the fuel groups at 6 %–7 %.
J. Douglas Goetz, Michael R. Giordano, Chelsea E. Stockwell, Ted J. Christian, Rashmi Maharjan, Sagar Adhikari, Prakash V. Bhave, Puppala S. Praveen, Arnico K. Panday, Thilina Jayarathne, Elizabeth A. Stone, Robert J. Yokelson, and Peter F. DeCarlo
Atmos. Chem. Phys., 18, 14653–14679, https://doi.org/10.5194/acp-18-14653-2018, https://doi.org/10.5194/acp-18-14653-2018, 2018
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Size distributions and emission factors of submicron aerosol were quantified using online techniques for a variety of common but under-sampled combustion sources in South Asia: wood and dung cooking fires, groundwater pumps, brick kilns, trash burning, and open burning of crop residues. Optical properties (brown carbon light absorption and the absorption Ångström exponent, AAE) of the emissions were also investigated. Contextual comparisons to the literature and other NAMaSTE results were made.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Kanako Sekimoto, Abigail R. Koss, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Carsten Warneke, Robert J. Yokelson, James M. Roberts, and Joost de Gouw
Atmos. Chem. Phys., 18, 9263–9281, https://doi.org/10.5194/acp-18-9263-2018, https://doi.org/10.5194/acp-18-9263-2018, 2018
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We found that on average 85 % of the VOC emissions from biomass burning across various fuels representative of the western US (including various coniferous and chaparral fuels) can be explained using only two emission profiles: (i) a high-temperature pyrolysis profile and (ii) a low-temperature pyrolysis profile. The high-temperature profile is quantitatively similar between different fuel types (r2 > 0.84), and likewise for the low-temperature profile.
Roya Bahreini, Ravan Ahmadov, Stu A. McKeen, Kennedy T. Vu, Justin H. Dingle, Eric C. Apel, Donald R. Blake, Nicola Blake, Teresa L. Campos, Chris Cantrell, Frank Flocke, Alan Fried, Jessica B. Gilman, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Brian M. Lerner, Roy L. Mauldin, Simone Meinardi, Denise D. Montzka, Dirk Richter, Jason R. Schroeder, Meghan Stell, David Tanner, James Walega, Peter Weibring, and Andrew Weinheimer
Atmos. Chem. Phys., 18, 8293–8312, https://doi.org/10.5194/acp-18-8293-2018, https://doi.org/10.5194/acp-18-8293-2018, 2018
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We measured organic aerosol (OA) and relevant trace gases during FRAPPÉ in the Colorado Front Range, with the goal of characterizing summertime OA formation. Our results indicate a significant production of secondary OA (SOA) in this region. About 2 μg m−3 of OA was present at background CO levels, suggesting contribution of non-combustion sources to SOA. Contribution of oil- and gas-related activities to anthropogenic SOA was modeled to be ~38 %. Biogenic SOA contributed to >40 % of OA.
Si-Wan Kim, Vijay Natraj, Seoyoung Lee, Hyeong-Ahn Kwon, Rokjin Park, Joost de Gouw, Gregory Frost, Jhoon Kim, Jochen Stutz, Michael Trainer, Catalina Tsai, and Carsten Warneke
Atmos. Chem. Phys., 18, 7639–7655, https://doi.org/10.5194/acp-18-7639-2018, https://doi.org/10.5194/acp-18-7639-2018, 2018
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Formaldehyde (HCHO) is a hazardous air pollutant and is associated with tropospheric ozone production. HCHO has been monitored from space. In this study, to acquire high-quality satellite-based HCHO observations, we utilize fine-resolution atmospheric chemistry model results as an input to the computer code for satellite retrievals over the Los Angeles Basin. Our study indicates that the use of fine-resolution profile shapes helps to identify HCHO plumes from space.
Chelsea E. Stockwell, Agnieszka Kupc, Bartłomiej Witkowski, Ranajit K. Talukdar, Yong Liu, Vanessa Selimovic, Kyle J. Zarzana, Kanako Sekimoto, Carsten Warneke, Rebecca A. Washenfelder, Robert J. Yokelson, Ann M. Middlebrook, and James M. Roberts
Atmos. Meas. Tech., 11, 2749–2768, https://doi.org/10.5194/amt-11-2749-2018, https://doi.org/10.5194/amt-11-2749-2018, 2018
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This work investigates the total conversion of particle-bound nitrogen and organic carbon across platinum and molybdenum catalysts followed by NO–O3 chemiluminescence and nondispersive infrared CO2 detection. We show the instrument is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation through comparisons with a calibrated particle-into-liquid sampler coupled to an electrospray ionization source of a mass spectrometer.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Vanessa Selimovic, Robert J. Yokelson, Carsten Warneke, James M. Roberts, Joost de Gouw, James Reardon, and David W. T. Griffith
Atmos. Chem. Phys., 18, 2929–2948, https://doi.org/10.5194/acp-18-2929-2018, https://doi.org/10.5194/acp-18-2929-2018, 2018
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We burned fuels representing western US wildfires in large-scale laboratory simulations to generate relevant emissions as confirmed by lab–field comparison. We report emission factors (EFs) for light scattering and absorption and BC along with SSA at 870 and 401 nm and AAE. We report EF for 22 trace gases that are major inorganic and organic emissions from flaming and smoldering. We report trace gas EF for species rarely (NH3) or not yet measured (e.g., HONO, acetic acid) for real US wildfires.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Thilina Jayarathne, Chelsea E. Stockwell, Ashley A. Gilbert, Kaitlyn Daugherty, Mark A. Cochrane, Kevin C. Ryan, Erianto I. Putra, Bambang H. Saharjo, Ati D. Nurhayati, Israr Albar, Robert J. Yokelson, and Elizabeth A. Stone
Atmos. Chem. Phys., 18, 2585–2600, https://doi.org/10.5194/acp-18-2585-2018, https://doi.org/10.5194/acp-18-2585-2018, 2018
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Fine particulate matter (PM2.5) emissions from Indonesian peat burning were measured in situ. Fuel-based emission factors from 6.0–29.6 gPM kg-1. Detailed chemical analysis revealed high levels of organic carbon that was primarily water insoluble, little to no detectable elemental carbon, and alkane contributions to organic carbon in the range of 6 %. These data were used to estimate that 3.2–11 Tg of PM2.5 were emitted by the 2015 peat burning episodes in Indonesia.
Jingyi Li, Jingqiu Mao, Arlene M. Fiore, Ronald C. Cohen, John D. Crounse, Alex P. Teng, Paul O. Wennberg, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Jeff Peischl, Ilana B. Pollack, Thomas B. Ryerson, Patrick Veres, James M. Roberts, J. Andrew Neuman, John B. Nowak, Glenn M. Wolfe, Thomas F. Hanisco, Alan Fried, Hanwant B. Singh, Jack Dibb, Fabien Paulot, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2341–2361, https://doi.org/10.5194/acp-18-2341-2018, https://doi.org/10.5194/acp-18-2341-2018, 2018
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We present the first comprehensive model evaluation of summertime reactive oxidized nitrogen using a high-resolution chemistry–climate model with up-to-date isoprene oxidation chemistry, along with a series of observations from aircraft campaigns and ground measurement networks from 2004 to 2013 over the Southeast US. We investigate the impact of NOx emission reductions on changes in reactive nitrogen speciation and export efficiency as well as ozone in the past and future decade.
Thilina Jayarathne, Chelsea E. Stockwell, Prakash V. Bhave, Puppala S. Praveen, Chathurika M. Rathnayake, Md. Robiul Islam, Arnico K. Panday, Sagar Adhikari, Rashmi Maharjan, J. Douglas Goetz, Peter F. DeCarlo, Eri Saikawa, Robert J. Yokelson, and Elizabeth A. Stone
Atmos. Chem. Phys., 18, 2259–2286, https://doi.org/10.5194/acp-18-2259-2018, https://doi.org/10.5194/acp-18-2259-2018, 2018
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Emissions of fine particulate matter and its constituents were quantified for a variety of under-sampled combustion sources in South Asia: wood and dung cooking fires, generators, groundwater pumps, brick kilns, trash burning, and open burning of biomasses. Garbage burning and three-stone cooking fires were among the highest emitters, while servicing of motor vehicles significantly reduced PM. These data may be used in source apportionment and to update regional and global emission inventories.
Catalina Tsai, Max Spolaor, Santo Fedele Colosimo, Olga Pikelnaya, Ross Cheung, Eric Williams, Jessica B. Gilman, Brian M. Lerner, Robert J. Zamora, Carsten Warneke, James M. Roberts, Ravan Ahmadov, Joost de Gouw, Timothy Bates, Patricia K. Quinn, and Jochen Stutz
Atmos. Chem. Phys., 18, 1977–1996, https://doi.org/10.5194/acp-18-1977-2018, https://doi.org/10.5194/acp-18-1977-2018, 2018
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Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH). Vertical HONO fluxes, observed in the snow-free, wintertime Uintah Basin, Utah, USA, show that chemical formation of HONO on the ground closes the HONO budget. Under high NOx conditions, HONO formation is most likely due to photo-enhanced conversion of NO2 on the ground. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the most likely source of HONO.
Katherine M. Manfred, Rebecca A. Washenfelder, Nicholas L. Wagner, Gabriela Adler, Frank Erdesz, Caroline C. Womack, Kara D. Lamb, Joshua P. Schwarz, Alessandro Franchin, Vanessa Selimovic, Robert J. Yokelson, and Daniel M. Murphy
Atmos. Chem. Phys., 18, 1879–1894, https://doi.org/10.5194/acp-18-1879-2018, https://doi.org/10.5194/acp-18-1879-2018, 2018
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In this study, we use a new laser imaging nephelometer to measure the bulk aerosol scattering phase function for biomass burning aerosol from controlled fires. By comparing measurements to models for spherical and fractal particles, we demonstrate that the dominant morphology varies by fuel type. This instrument has unique capabilities to directly measure how morphology affects optical properties, and can be used in the future for important validations of remote sensing retrievals.
Demetrios Pagonis, Jordan E. Krechmer, Joost de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 10, 4687–4696, https://doi.org/10.5194/amt-10-4687-2017, https://doi.org/10.5194/amt-10-4687-2017, 2017
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Laboratory studies were conducted to investigate gas-wall partitioning of atmospheric organic compounds in Teflon tubing and inside an instrument used to monitor concentrations. Rapid partitioning caused time delays in instrument response that vary with tubing length and diameter, flow rate, and compound volatility. Tubing delay times of seconds to hours were described using a model that also included effects of instrument surfaces. The results can enable better design of air sampling systems.
Robert C. Rhew, Malte Julian Deventer, Andrew A. Turnipseed, Carsten Warneke, John Ortega, Steve Shen, Luis Martinez, Abigail Koss, Brian M. Lerner, Jessica B. Gilman, James N. Smith, Alex B. Guenther, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 13417–13438, https://doi.org/10.5194/acp-17-13417-2017, https://doi.org/10.5194/acp-17-13417-2017, 2017
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Alkenes emanate from both natural and anthropogenic sources and can contribute to atmospheric ozone production. This study measured
lightalkene (ethene, propene and butene) fluxes from a ponderosa pine forest using a novel relaxed eddy accumulation method, revealing much larger emissions than previously estimated and accounting for a significant fraction of OH reactivity. Emissions have a diurnal cycle related to sunlight and temperature, and the forest canopy appears to be the source.
Guido R. van der Werf, James T. Randerson, Louis Giglio, Thijs T. van Leeuwen, Yang Chen, Brendan M. Rogers, Mingquan Mu, Margreet J. E. van Marle, Douglas C. Morton, G. James Collatz, Robert J. Yokelson, and Prasad S. Kasibhatla
Earth Syst. Sci. Data, 9, 697–720, https://doi.org/10.5194/essd-9-697-2017, https://doi.org/10.5194/essd-9-697-2017, 2017
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Fires occur in many vegetation types and are sometimes natural but often ignited by humans for various purposes. We have estimated how much area they burn globally and what their emissions are. Total burned area is roughly equivalent to the size of the EU with most fires burning in tropical savannas. Their emissions vary substantially from year to year and contribute to the atmospheric burdens of many trace gases and aerosols. The 20-year dataset is mostly suited for large-scale assessments.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Shantanu H. Jathar, Christopher Heppding, Michael F. Link, Delphine K. Farmer, Ali Akherati, Michael J. Kleeman, Joost A. de Gouw, Patrick R. Veres, and James M. Roberts
Atmos. Chem. Phys., 17, 8959–8970, https://doi.org/10.5194/acp-17-8959-2017, https://doi.org/10.5194/acp-17-8959-2017, 2017
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Our work makes novel emissions measurements of isocyanic acid, a toxic gas, from a modern-day diesel engine and finds that diesel engines emit isocyanic acid but the emissions control devices do not enhance or destroy the isocyanic acid. Air quality model calculations suggest that diesel engines are possibly important sources of isocyanic acid in urban environments although the isocyanic acid levels are ten times lower than levels linked to adverse human health effects.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
Caroline C. Womack, J. Andrew Neuman, Patrick R. Veres, Scott J. Eilerman, Charles A. Brock, Zachary C. J. Decker, Kyle J. Zarzana, William P. Dube, Robert J. Wild, Paul J. Wooldridge, Ronald C. Cohen, and Steven S. Brown
Atmos. Meas. Tech., 10, 1911–1926, https://doi.org/10.5194/amt-10-1911-2017, https://doi.org/10.5194/amt-10-1911-2017, 2017
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The accurate detection of reactive nitrogen species (NOy) is key to understanding tropospheric ozone production. Typically, NOy is detected by thermal conversion to NO2, followed by NO2 detection. Here, we assess the conversion efficiency of several NOy species to NO2 in a thermal dissociation cavity ring-down spectrometer and discuss how this conversion efficiency is affected by certain experimental conditions, such as oven residence time, and interferences from non-NOy species.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Rudra P. Pokhrel, Eric R. Beamesderfer, Nick L. Wagner, Justin M. Langridge, Daniel A. Lack, Thilina Jayarathne, Elizabeth A. Stone, Chelsea E. Stockwell, Robert J. Yokelson, and Shane M. Murphy
Atmos. Chem. Phys., 17, 5063–5078, https://doi.org/10.5194/acp-17-5063-2017, https://doi.org/10.5194/acp-17-5063-2017, 2017
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This study investigates enhancement of black carbon (BC) absorption in biomass burning emissions due to absorbing and non-absorbing coatings. The fraction of absorption due to BC, brown carbon (BrC), and lensing is estimated using different approaches. The similarities and differences between the results from these approaches are discussed. Absorption by BrC is shown to have good correlation with the elemental to organic carbon ratio (EC / OC) and AAE.
Bin Yuan, Matthew M. Coggon, Abigail R. Koss, Carsten Warneke, Scott Eilerman, Jeff Peischl, Kenneth C. Aikin, Thomas B. Ryerson, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 4945–4956, https://doi.org/10.5194/acp-17-4945-2017, https://doi.org/10.5194/acp-17-4945-2017, 2017
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In this study, we measured emissions of volatile organic compounds (VOCs) from concentrated animal feeding operations (CAFOs) using both mobile laboratory and aircraft measurements. We will use this data set to investigate chemical compositions of VOC emissions and sources apportionment for these VOC emissions in different facilities.
Lindsay E. Hatch, Robert J. Yokelson, Chelsea E. Stockwell, Patrick R. Veres, Isobel J. Simpson, Donald R. Blake, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 17, 1471–1489, https://doi.org/10.5194/acp-17-1471-2017, https://doi.org/10.5194/acp-17-1471-2017, 2017
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The most comprehensive database of gaseous biomass burning emissions to date was compiled. Four complementary instruments were deployed together during laboratory fires. The results generally compared within experimental uncertainty and highlighted that a range of measurement approaches are required for adequate characterization of smoke composition. Observed compounds were binned based on volatility, and priority recommendations were made to improve secondary organic aerosol predictions.
Anusha P. S. Hettiyadura, Thilina Jayarathne, Karsten Baumann, Allen H. Goldstein, Joost A. de Gouw, Abigail Koss, Frank N. Keutsch, Kate Skog, and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, https://doi.org/10.5194/acp-17-1343-2017, 2017
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Organosulfates are components of secondary organic aerosol (SOA) formed in the presence of sulfate. Herein, their abundance, identity, and potential to form as sampling artifacts were studied in Centreville, AL, USA. The 10 most abundant signals accounted for 58–78 % of the total, with at least 20–200 other species accounting for the remainder. These major species were largely associated with biogenic gases, like isoprene and monoterpenes, and are proposed targets for future standard development.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313, https://doi.org/10.5194/amt-10-291-2017, https://doi.org/10.5194/amt-10-291-2017, 2017
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Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, John J. Remedios, Carsten Warneke, James M. Roberts, Glenn S. Diskin, Lewis G. Huey, Armin Wisthaler, Eric C. Apel, Peter F. Bernath, and Wuhu Feng
Atmos. Chem. Phys., 16, 13541–13559, https://doi.org/10.5194/acp-16-13541-2016, https://doi.org/10.5194/acp-16-13541-2016, 2016
Chelsea E. Stockwell, Thilina Jayarathne, Mark A. Cochrane, Kevin C. Ryan, Erianto I. Putra, Bambang H. Saharjo, Ati D. Nurhayati, Israr Albar, Donald R. Blake, Isobel J. Simpson, Elizabeth A. Stone, and Robert J. Yokelson
Atmos. Chem. Phys., 16, 11711–11732, https://doi.org/10.5194/acp-16-11711-2016, https://doi.org/10.5194/acp-16-11711-2016, 2016
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We present the first or rare field measurements of emission factors for Indonesian peat fires made in Borneo during the 2015 El Niño. The data include up to 90 gases, aerosol mass, and aerosol optical properties at two wavelengths (405 and 870 nm). Brown carbon dominates aerosol absorption, revisions to previous values for greenhouse gas emissions are supported and air toxics are assessed.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Chelsea E. Stockwell, Ted J. Christian, J. Douglas Goetz, Thilina Jayarathne, Prakash V. Bhave, Puppala S. Praveen, Sagar Adhikari, Rashmi Maharjan, Peter F. DeCarlo, Elizabeth A. Stone, Eri Saikawa, Donald R. Blake, Isobel J. Simpson, Robert J. Yokelson, and Arnico K. Panday
Atmos. Chem. Phys., 16, 11043–11081, https://doi.org/10.5194/acp-16-11043-2016, https://doi.org/10.5194/acp-16-11043-2016, 2016
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We present the first, or rare, field measurements in South Asia of emission factors for up to 80 gases (pollutants, greenhouse gases, and precursors) and black carbon and aerosol optical properties at 405 and 870 nm for many previously under-sampled sources that are important in developing countries such as cooking with dung and wood, garbage and crop residue burning, brick kilns, motorcycles, generators and pumps, etc. Brown carbon contributes significantly to total aerosol absorption.
Rudra P. Pokhrel, Nick L. Wagner, Justin M. Langridge, Daniel A. Lack, Thilina Jayarathne, Elizabeth A. Stone, Chelsea E. Stockwell, Robert J. Yokelson, and Shane M. Murphy
Atmos. Chem. Phys., 16, 9549–9561, https://doi.org/10.5194/acp-16-9549-2016, https://doi.org/10.5194/acp-16-9549-2016, 2016
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This paper gives first multi-wavelength estimates of SSA and AAE of emissions from combustion of Indonesian peat. In addition, it demonstrates that SSA of biomass burning emissions can be parameterized with EC / (EC+OC) and that this parameterization is quantitatively superior to previously published parameterizations based on MCE. It also shows that EC / (EC+OC) parameterization accurately predicts SSA during the first few hours of aging of a biomass burning plume.
Jan Zörner, Marloes Penning de Vries, Steffen Beirle, Holger Sihler, Patrick R. Veres, Jonathan Williams, and Thomas Wagner
Atmos. Chem. Phys., 16, 9457–9487, https://doi.org/10.5194/acp-16-9457-2016, https://doi.org/10.5194/acp-16-9457-2016, 2016
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We present a top-down approach to infer and quantify rain-induced emission pulses of nitrogen oxides from soils using satellite-borne measurements of NO2. We found strong enhancements of NO2 induced by the first intense precipitation after prolonged droughts in many semi-arid regions of the world, in particular in the Sahel. Apart from the clear first-day peak, NO2 VCDs are moderately enhanced compared to background over the following 2 weeks suggesting potential further emissions.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Abigail R. Koss, Carsten Warneke, Bin Yuan, Matthew M. Coggon, Patrick R. Veres, and Joost A. de Gouw
Atmos. Meas. Tech., 9, 2909–2925, https://doi.org/10.5194/amt-9-2909-2016, https://doi.org/10.5194/amt-9-2909-2016, 2016
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Using laboratory and field experiments, we have explored how the technique of NO+ chemical ionization mass spectrometry can be used to measure volatile organic compounds (VOCs) in the troposphere. Results include the design and operation of the instrument, an evaluation of the technique’s utility for atmospheric measurement, and a guide for data interpretation. Use of this technique will improve our understanding of VOC chemistry.
Bin Yuan, Abigail Koss, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Harald Stark, and Joost A. de Gouw
Atmos. Meas. Tech., 9, 2735–2752, https://doi.org/10.5194/amt-9-2735-2016, https://doi.org/10.5194/amt-9-2735-2016, 2016
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We present the development of a hydronium (H3O+) time of flight chemical ionization mass spectrometer (H3O+ ToF-CIMS). We characterize the humidity dependence of the reagent ions and VOC signals in details. The low mass cutoff issue of RF-only quadrupole leads to unusual humidity dependence of reagent ions. The new H3O+ ToF-CIMS was successfully deployed on the NOAA WP-3D research aircraft for the SONGNEX campaign in 2015 and some initial results from the SONGNEX campaign are presented.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Hannah M. Allen, Benjamin R. Ayres, Steven S. Brown, William H. Brune, John D. Crounse, Joost de Gouw, Danielle C. Draper, Philip A. Feiner, Juliane L. Fry, Allen H. Goldstein, Abigail Koss, Pawel K. Misztal, Tran B. Nguyen, Kevin Olson, Alex P. Teng, Paul O. Wennberg, Robert J. Wild, Li Zhang, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 7623–7637, https://doi.org/10.5194/acp-16-7623-2016, https://doi.org/10.5194/acp-16-7623-2016, 2016
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The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the southeastern United States. At warm temperatures in the daytime boundary layer, NOx interconverts rapidly with both PAN and alkyl and multifunctional nitrates (RONO2), and the relevant lifetime is the combined lifetime of these three classes. We find that the production of RONO2, followed by hydrolysis to produce nitric acid, is the dominant pathway for NOx removal in an isoprene dominated forest.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Chun Zhao, Maoyi Huang, Jerome D. Fast, Larry K. Berg, Yun Qian, Alex Guenther, Dasa Gu, Manish Shrivastava, Ying Liu, Stacy Walters, Gabriele Pfister, Jiming Jin, John E. Shilling, and Carsten Warneke
Geosci. Model Dev., 9, 1959–1976, https://doi.org/10.5194/gmd-9-1959-2016, https://doi.org/10.5194/gmd-9-1959-2016, 2016
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In this study, the latest version of MEGAN is coupled within CLM4 in WRF-Chem. In this implementation, MEGAN shares a consistent vegetation map with CLM4. This improved modeling framework is used to investigate the impact of two land surface schemes on BVOCs and examine the sensitivity of BVOCs to vegetation distributions in California. This study indicates that more effort is needed to obtain the most appropriate and accurate land cover data sets for climate and air quality models.
Markus Müller, Bruce E. Anderson, Andreas J. Beyersdorf, James H. Crawford, Glenn S. Diskin, Philipp Eichler, Alan Fried, Frank N. Keutsch, Tomas Mikoviny, Kenneth L. Thornhill, James G. Walega, Andrew J. Weinheimer, Melissa Yang, Robert J. Yokelson, and Armin Wisthaler
Atmos. Chem. Phys., 16, 3813–3824, https://doi.org/10.5194/acp-16-3813-2016, https://doi.org/10.5194/acp-16-3813-2016, 2016
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Atmospheric emissions from small forest fires and their impact on regional air quality are still poorly characterized. We used an instrumented NASA P-3B aircraft to study emissions from a small forest understory fire in Georgia (USA) and to investigate chemical transformations in the fire plume in the 1 h downwind region. A state-of-the-art chemical model was able to accurately simulate key chemical processes in the aging plume.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
Bin Yuan, John Liggio, Jeremy Wentzell, Shao-Meng Li, Harald Stark, James M. Roberts, Jessica Gilman, Brian Lerner, Carsten Warneke, Rui Li, Amy Leithead, Hans D. Osthoff, Robert Wild, Steven S. Brown, and Joost A. de Gouw
Atmos. Chem. Phys., 16, 2139–2153, https://doi.org/10.5194/acp-16-2139-2016, https://doi.org/10.5194/acp-16-2139-2016, 2016
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We describe high-resolution measurements of nitrated phenols using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS). Strong diurnal profiles were observed for nitrated phenols, with concentration maxima at night. Box model simulations were able to reproduce the measured nitrated phenols.
R. J. Wild, P. M. Edwards, T. S. Bates, R. C. Cohen, J. A. de Gouw, W. P. Dubé, J. B. Gilman, J. Holloway, J. Kercher, A. R. Koss, L. Lee, B. M. Lerner, R. McLaren, P. K. Quinn, J. M. Roberts, J. Stutz, J. A. Thornton, P. R. Veres, C. Warneke, E. Williams, C. J. Young, B. Yuan, K. J. Zarzana, and S. S. Brown
Atmos. Chem. Phys., 16, 573–583, https://doi.org/10.5194/acp-16-573-2016, https://doi.org/10.5194/acp-16-573-2016, 2016
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High wintertime ozone levels have been observed in the Uintah Basin, Utah, a sparsely populated rural region with intensive oil and gas operations. The reactive nitrogen budget plays an important role in tropospheric ozone formation, and we find that nighttime chemistry has a large effect on its partitioning. Much of the oxidation of reactive nitrogen during a high-ozone year occurred via heterogeneous uptake onto aerosol at night, keeping NOx at concentrations comparable to a low-ozone year.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
C. Huang, H. L. Wang, L. Li, Q. Wang, Q. Lu, J. A. de Gouw, M. Zhou, S. A. Jing, J. Lu, and C. H. Chen
Atmos. Chem. Phys., 15, 11081–11096, https://doi.org/10.5194/acp-15-11081-2015, https://doi.org/10.5194/acp-15-11081-2015, 2015
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SOA formations from vehicle exhausts and gas evaporation contribute 40% and 60% of total organic aerosols observed in summer and winter in urban Shanghai. Diesel vehicles, which accounted for less than 20% of vehicle kilometers of travel, contribute the most to vehicular POA emissions and SOA production in urban Shanghai. Intermediate-volatile organic compounds (IVOCs) in vehicle exhausts contribute greatly to SOA formation in the urban atmosphere of China.
L. Lee, P. J. Wooldridge, J. deGouw, S. S. Brown, T. S. Bates, P. K. Quinn, and R. C. Cohen
Atmos. Chem. Phys., 15, 9313–9325, https://doi.org/10.5194/acp-15-9313-2015, https://doi.org/10.5194/acp-15-9313-2015, 2015
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Secondary organic aerosol affects both the environment and human health. We characterized the aerosol composition in Uintah Basin by measuring the concentration of nitrooxy group moiety which is produced through chemical interaction of volatile organic compounds and NOx emitted largely from local human activity. We found nitrooxy compounds to be a persistent, if not dominant, portion of fine aerosol mass. Similar results may be expected from emissions due to traffic in cities.
P. R. Veres, J. M. Roberts, R. J. Wild, P. M. Edwards, S. S. Brown, T. S. Bates, P. K. Quinn, J. E. Johnson, R. J. Zamora, and J. de Gouw
Atmos. Chem. Phys., 15, 8101–8114, https://doi.org/10.5194/acp-15-8101-2015, https://doi.org/10.5194/acp-15-8101-2015, 2015
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In this paper laboratory work is documented establishing iodide ion chemical ionization mass spectrometry (I- CIMS) as a sensitive method for the unambiguous detection of peroxynitric acid (HO2NO2; PNA). A dynamic calibration source for HO2NO2, HO2, and HONO was developed and calibrated using a novel total NOy detector (NOy CaRDS). The ambient observations of HO2NO2 using I- CIMS made during the 2013 and 2014 Uintah Basin Wintertime Ozone Study (UBWOS) are presented.
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
M. J. Alvarado, C. R. Lonsdale, R. J. Yokelson, S. K. Akagi, H. Coe, J. S. Craven, E. V. Fischer, G. R. McMeeking, J. H. Seinfeld, T. Soni, J. W. Taylor, D. R. Weise, and C. E. Wold
Atmos. Chem. Phys., 15, 6667–6688, https://doi.org/10.5194/acp-15-6667-2015, https://doi.org/10.5194/acp-15-6667-2015, 2015
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Being able to understand and simulate the chemical evolution of biomass burning smoke plumes under a wide variety of conditions is a critical part of forecasting the impact of these fires on air quality, atmospheric composition, and climate. Here we use an improved model of this chemistry to simulate the evolution of ozone and secondary organic aerosol within a young biomass burning smoke plume from the Williams prescribed burn in chaparral, which was sampled over California in November 2009.
A. A. May, T. Lee, G. R. McMeeking, S. Akagi, A. P. Sullivan, S. Urbanski, R. J. Yokelson, and S. M. Kreidenweis
Atmos. Chem. Phys., 15, 6323–6335, https://doi.org/10.5194/acp-15-6323-2015, https://doi.org/10.5194/acp-15-6323-2015, 2015
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Smoke plumes from some prescribed fires in the southeastern United States were sampled via aircraft to observe changes in organic aerosol (OA) with atmospheric transport. These plumes underwent rapid mixing, and, hence, substantial dilution with background air occurred. Dilution-driven evaporation appears to be the primary driver of OA transformations within the sampled plumes rather than photochemistry.
D. B. Millet, M. Baasandorj, D. K. Farmer, J. A. Thornton, K. Baumann, P. Brophy, S. Chaliyakunnel, J. A. de Gouw, M. Graus, L. Hu, A. Koss, B. H. Lee, F. D. Lopez-Hilfiker, J. A. Neuman, F. Paulot, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, B. J. Williams, and J. Xu
Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, https://doi.org/10.5194/acp-15-6283-2015, 2015
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Formic acid (HCOOH) is an abundant atmospheric acid that affects precipitation chemistry and acidity. HCOOH measurements over the USA are 2-3× larger than can be explained by known sources and sinks, revealing a key gap in current understanding. Observations indicate a large biogenic source plus chemical production across a range of precursors. Model simulations cannot capture the HCOOH diurnal amplitude or nocturnal profile, implying a deposition bias and possibly even larger missing source.
P. R. Veres and J. M. Roberts
Atmos. Meas. Tech., 8, 2225–2231, https://doi.org/10.5194/amt-8-2225-2015, https://doi.org/10.5194/amt-8-2225-2015, 2015
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A dynamic system for the calibration of acyl peroxynitrate compounds has been developed to reduce the difficulty, required time, and stability of laboratory standards. We present a photochemical source for the generation of acetyl peroxynitrate (PAN), propionyl peroxynitrate (PPN), acryloyl peroxynitrate (APAN), methacryloyl peroxynitrate (MPAN), and crotonyl peroxynitrate (CPAN). Validation of the APN products was performed using iodide ion chemical ionization mass spectroscopy (I- CIMS).
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
A. R. Koss, J. de Gouw, C. Warneke, J. B. Gilman, B. M. Lerner, M. Graus, B. Yuan, P. Edwards, S. S. Brown, R. Wild, J. M. Roberts, T. S. Bates, and P. K. Quinn
Atmos. Chem. Phys., 15, 5727–5741, https://doi.org/10.5194/acp-15-5727-2015, https://doi.org/10.5194/acp-15-5727-2015, 2015
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Extraction of natural gas and oil is associated with a range of possible atmospheric environmental issues. Here we present an analysis of gas-phase hydrocarbon measurements taken in an oil and natural gas extraction area in Utah during a period of high wintertime ozone. We are able to constrain important chemical parameters related to emission sources and rates, hydrocarbon photochemistry, and VOC composition.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
L. E. Hatch, W. Luo, J. F. Pankow, R. J. Yokelson, C. E. Stockwell, and K. C. Barsanti
Atmos. Chem. Phys., 15, 1865–1899, https://doi.org/10.5194/acp-15-1865-2015, https://doi.org/10.5194/acp-15-1865-2015, 2015
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This work represents the first application of two-dimensional gas chromatography to broadly characterize the gas-phase emissions of biomass burning, including comparisons among the emissions from burns of selected conifer, grass, crop residue, and peat fuel types. In these smoke samples, over 700 compounds were detected, which are discussed in the context of potential secondary organic aerosol formation.
C. Warneke, P. Veres, S. M. Murphy, J. Soltis, R. A. Field, M. G. Graus, A. Koss, S.-M. Li, R. Li, B. Yuan, J. M. Roberts, and J. A. de Gouw
Atmos. Meas. Tech., 8, 411–420, https://doi.org/10.5194/amt-8-411-2015, https://doi.org/10.5194/amt-8-411-2015, 2015
C. E. Stockwell, P. R. Veres, J. Williams, and R. J. Yokelson
Atmos. Chem. Phys., 15, 845–865, https://doi.org/10.5194/acp-15-845-2015, https://doi.org/10.5194/acp-15-845-2015, 2015
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We used a high-resolution proton-transfer-reaction time-of-flight mass spectrometer to measure emissions from peat, crop residue, cooking fires, etc. We assigned > 80% of the mass of gas-phase organic compounds and much of it was secondary organic aerosol precursors. The open cooking emissions were much larger than from advanced cookstoves. Little-studied N-containing organic compounds accounted for 0.1-8.7% of the fuel N and may influence new particle formation.
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
L. Lee, P. J. Wooldridge, J. B. Gilman, C. Warneke, J. de Gouw, and R. C. Cohen
Atmos. Chem. Phys., 14, 12441–12454, https://doi.org/10.5194/acp-14-12441-2014, https://doi.org/10.5194/acp-14-12441-2014, 2014
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Alkyl nitrate formation is known to be an important sink of NOx in a wide range of environments. In a study in the Uintah basin in 2012, we find that formation of these compounds represents a more rapid NOx (NO + NO2) sink than does nitric acid formation. This rapid formation is in large part due to the low mean temperature (~0°C) during the study and is consistent with laboratory observations.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
R. Li, C. Warneke, M. Graus, R. Field, F. Geiger, P. R. Veres, J. Soltis, S.-M. Li, S. M. Murphy, C. Sweeney, G. Pétron, J. M. Roberts, and J. de Gouw
Atmos. Meas. Tech., 7, 3597–3610, https://doi.org/10.5194/amt-7-3597-2014, https://doi.org/10.5194/amt-7-3597-2014, 2014
C. Warneke, F. Geiger, P. M. Edwards, W. Dube, G. Pétron, J. Kofler, A. Zahn, S. S. Brown, M. Graus, J. B. Gilman, B. M. Lerner, J. Peischl, T. B. Ryerson, J. A. de Gouw, and J. M. Roberts
Atmos. Chem. Phys., 14, 10977–10988, https://doi.org/10.5194/acp-14-10977-2014, https://doi.org/10.5194/acp-14-10977-2014, 2014
A. P. Sullivan, A. A. May, T. Lee, G. R. McMeeking, S. M. Kreidenweis, S. K. Akagi, R. J. Yokelson, S. P. Urbanski, and J. L. Collett Jr.
Atmos. Chem. Phys., 14, 10535–10545, https://doi.org/10.5194/acp-14-10535-2014, https://doi.org/10.5194/acp-14-10535-2014, 2014
T. Behrendt, P. R. Veres, F. Ashuri, G. Song, M. Flanz, B. Mamtimin, M. Bruse, J. Williams, and F. X. Meixner
Biogeosciences, 11, 5463–5492, https://doi.org/10.5194/bg-11-5463-2014, https://doi.org/10.5194/bg-11-5463-2014, 2014
W. Ait-Helal, A. Borbon, S. Sauvage, J. A. de Gouw, A. Colomb, V. Gros, F. Freutel, M. Crippa, C. Afif, U. Baltensperger, M. Beekmann, J.-F. Doussin, R. Durand-Jolibois, I. Fronval, N. Grand, T. Leonardis, M. Lopez, V. Michoud, K. Miet, S. Perrier, A. S. H. Prévôt, J. Schneider, G. Siour, P. Zapf, and N. Locoge
Atmos. Chem. Phys., 14, 10439–10464, https://doi.org/10.5194/acp-14-10439-2014, https://doi.org/10.5194/acp-14-10439-2014, 2014
C. E. Stockwell, R. J. Yokelson, S. M. Kreidenweis, A. L. Robinson, P. J. DeMott, R. C. Sullivan, J. Reardon, K. C. Ryan, D. W. T. Griffith, and L. Stevens
Atmos. Chem. Phys., 14, 9727–9754, https://doi.org/10.5194/acp-14-9727-2014, https://doi.org/10.5194/acp-14-9727-2014, 2014
P. R. Veres, T. Behrendt, A. Klapthor, F. X. Meixner, and J. Williams
Biogeosciences Discuss., https://doi.org/10.5194/bgd-11-12009-2014, https://doi.org/10.5194/bgd-11-12009-2014, 2014
Revised manuscript not accepted
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
T. P. Riedel, G. M. Wolfe, K. T. Danas, J. B. Gilman, W. C. Kuster, D. M. Bon, A. Vlasenko, S.-M. Li, E. J. Williams, B. M. Lerner, P. R. Veres, J. M. Roberts, J. S. Holloway, B. Lefer, S. S. Brown, and J. A. Thornton
Atmos. Chem. Phys., 14, 3789–3800, https://doi.org/10.5194/acp-14-3789-2014, https://doi.org/10.5194/acp-14-3789-2014, 2014
C. J. Young, R. A. Washenfelder, P. M. Edwards, D. D. Parrish, J. B. Gilman, W. C. Kuster, L. H. Mielke, H. D. Osthoff, C. Tsai, O. Pikelnaya, J. Stutz, P. R. Veres, J. M. Roberts, S. Griffith, S. Dusanter, P. S. Stevens, J. Flynn, N. Grossberg, B. Lefer, J. S. Holloway, J. Peischl, T. B. Ryerson, E. L. Atlas, D. R. Blake, and S. S. Brown
Atmos. Chem. Phys., 14, 3427–3440, https://doi.org/10.5194/acp-14-3427-2014, https://doi.org/10.5194/acp-14-3427-2014, 2014
K. C. Wells, D. B. Millet, K. E. Cady-Pereira, M. W. Shephard, D. K. Henze, N. Bousserez, E. C. Apel, J. de Gouw, C. Warneke, and H. B. Singh
Atmos. Chem. Phys., 14, 2555–2570, https://doi.org/10.5194/acp-14-2555-2014, https://doi.org/10.5194/acp-14-2555-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 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
C. L. Hagen, B. C. Lee, I. S. Franka, J. L. Rath, T. C. VandenBoer, J. M. Roberts, S. S. Brown, and A. P. Yalin
Atmos. Meas. Tech., 7, 345–357, https://doi.org/10.5194/amt-7-345-2014, https://doi.org/10.5194/amt-7-345-2014, 2014
S. K. Akagi, I. R. Burling, A. Mendoza, T. J. Johnson, M. Cameron, D. W. T. Griffith, C. Paton-Walsh, D. R. Weise, J. Reardon, and R. J. Yokelson
Atmos. Chem. Phys., 14, 199–215, https://doi.org/10.5194/acp-14-199-2014, https://doi.org/10.5194/acp-14-199-2014, 2014
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. S. Brown, W. P. Dubé, R. Bahreini, A. M. Middlebrook, C. A. Brock, C. Warneke, J. A. de Gouw, R. A. Washenfelder, E. Atlas, J. Peischl, T. B. Ryerson, J. S. Holloway, J. P. Schwarz, R. Spackman, M. Trainer, D. D. Parrish, F. C. Fehshenfeld, and A. R. Ravishankara
Atmos. Chem. Phys., 13, 11317–11337, https://doi.org/10.5194/acp-13-11317-2013, https://doi.org/10.5194/acp-13-11317-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
R. J. Yokelson, M. O. Andreae, and S. K. Akagi
Atmos. Meas. Tech., 6, 2155–2158, https://doi.org/10.5194/amt-6-2155-2013, https://doi.org/10.5194/amt-6-2155-2013, 2013
J. Brioude, W. M. Angevine, R. Ahmadov, S.-W. Kim, S. Evan, S. A. McKeen, E.-Y. Hsie, G. J. Frost, J. A. Neuman, I. B. Pollack, J. Peischl, T. B. Ryerson, J. Holloway, S. S. Brown, J. B. Nowak, J. M. Roberts, S. C. Wofsy, G. W. Santoni, T. Oda, and M. Trainer
Atmos. Chem. Phys., 13, 3661–3677, https://doi.org/10.5194/acp-13-3661-2013, https://doi.org/10.5194/acp-13-3661-2013, 2013
D. A. Lack, R. Bahreini, J. M. Langridge, J. B. Gilman, and A. M. Middlebrook
Atmos. Chem. Phys., 13, 2415–2422, https://doi.org/10.5194/acp-13-2415-2013, https://doi.org/10.5194/acp-13-2415-2013, 2013
S. K. Akagi, R. J. Yokelson, I. R. Burling, S. Meinardi, I. Simpson, D. R. Blake, G. R. McMeeking, A. Sullivan, T. Lee, S. Kreidenweis, S. Urbanski, J. Reardon, D. W. T. Griffith, T. J. Johnson, and D. R. Weise
Atmos. Chem. Phys., 13, 1141–1165, https://doi.org/10.5194/acp-13-1141-2013, https://doi.org/10.5194/acp-13-1141-2013, 2013
R. J. Yokelson, I. R. Burling, J. B. Gilman, C. Warneke, C. E. Stockwell, J. de Gouw, S. K. Akagi, S. P. Urbanski, P. Veres, J. M. Roberts, W. C. Kuster, J. Reardon, D. W. T. Griffith, T. J. Johnson, S. Hosseini, J. W. Miller, D. R. Cocker III, H. Jung, and D. R. Weise
Atmos. Chem. Phys., 13, 89–116, https://doi.org/10.5194/acp-13-89-2013, https://doi.org/10.5194/acp-13-89-2013, 2013
Related subject area
Subject: Gases | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Formation of reactive nitrogen species promoted by iron ions through the photochemistry of a neonicotinoid insecticide
Rate coefficients for the reactions of OH radicals with C3–C11 alkanes determined by the relative-rate technique
Formation and temperature dependence of highly oxygenated organic molecules (HOMs) from Δ3-carene ozonolysis
Mechanistic insight into the kinetic fragmentation of norpinonic acid in the gas phase: an experimental and density functional theory (DFT) study
Temperature-dependent rate coefficients for the reaction of OH radicals with selected alkanes, aromatic compounds and monoterpenes
Exploring HONO production from particulate nitrate photolysis in Chinese representative regions: characteristics, influencing factors and environmental implications
Secondary reactions of aromatics-derived oxygenated organic molecules lead to plentiful highly oxygenated organic molecules within an intraday OH exposure
Impact of HO2∕RO2 ratio on highly oxygenated α-pinene photooxidation products and secondary organic aerosol formation potential
Negligible temperature dependence of the ozone–iodide reaction and implications for oceanic emissions of iodine
Extension, development, and evaluation of the representation of the OH-initiated dimethyl sulfide (DMS) oxidation mechanism in the Master Chemical Mechanism (MCM) v3.3.1 framework
On the potential use of highly oxygenated organic molecules (HOMs) as indicators for ozone formation sensitivity
Oxygenated organic molecules produced by low-NOx photooxidation of aromatic compounds: contributions to secondary organic aerosol and steric hindrance
Impact of temperature on the role of Criegee intermediates and peroxy radicals in dimer formation from β-pinene ozonolysis
Atmospheric impact of 2-methylpentanal emissions: kinetics, photochemistry, and formation of secondary pollutants
Quantifying primary oxidation products in the OH-initiated reaction of benzyl alcohol
Technical note: Gas-phase nitrate radical generation via irradiation of aerated ceric ammonium nitrate mixtures
Direct probing of acylperoxy radicals during ozonolysis of α-pinene: constraints on radical chemistry and production of highly oxygenated organic molecules
Atmospheric photooxidation and ozonolysis of sabinene: reaction rate coefficients, product yields, and chemical budget of radicals
Compilation of Henry's law constants (version 5.0.0) for water as solvent
Measurement report: Carbonyl sulfide production during dimethyl sulfide oxidation in the atmospheric simulation chamber SAPHIR
An aldehyde as a rapid source of secondary aerosol precursors: theoretical and experimental study of hexanal autoxidation
Measuring and modeling investigation of the net photochemical ozone production rate via an improved dual-channel reaction chamber technique
Evolution of organic carbon in the laboratory oxidation of biomass-burning emissions
Atmospheric oxidation of new “green” solvents – Part 2: methyl pivalate and pinacolone
On the formation of highly oxidized pollutants by autoxidation of terpenes under low-temperature-combustion conditions: the case of limonene and α-pinene
Selective deuteration as a tool for resolving autoxidation mechanisms in α-pinene ozonolysis
Comparison of isoprene chemical mechanisms under atmospheric night-time conditions in chamber experiments: evidence of hydroperoxy aldehydes and epoxy products from NO3 oxidation
Measurement of Henry's law and liquid-phase loss rate constants of peroxypropionic nitric anhydride (PPN) in deionized water and in n-octanol
Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO2 regimes
Atmospheric breakdown chemistry of the new “green” solvent 2,2,5,5-tetramethyloxolane via gas-phase reactions with OH and Cl radicals
Impact of cooking style and oil on semi-volatile and intermediate volatility organic compound emissions from Chinese domestic cooking
Observations of gas-phase products from the nitrate-radical-initiated oxidation of four monoterpenes
Investigation of the limonene photooxidation by OH at different NO concentrations in the atmospheric simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction Chamber)
Kinetic study of the atmospheric oxidation of a series of epoxy compounds by OH radicals
An experimental study of the reactivity of terpinolene and β-caryophyllene with the nitrate radical
Oxidation product characterization from ozonolysis of the diterpene ent-kaurene
Kinetics of OH + SO2 + M: temperature-dependent rate coefficients in the fall-off regime and the influence of water vapour
Formation of organic sulfur compounds through SO2-initiated photochemistry of PAHs and dimethylsulfoxide at the air-water interface
Stable carbon isotopic composition of biomass burning emissions – implications for estimating the contribution of C3 and C4 plants
Evaluation of the daytime tropospheric loss of 2-methylbutanal
Investigations into the gas-phase photolysis and OH radical kinetics of nitrocatechols: implications of intramolecular interactions on their atmospheric behaviour
Reproducing Arctic springtime tropospheric ozone and mercury depletion events in an outdoor mesocosm sea ice facility
N2O5 uptake onto saline mineral dust: a potential missing source of tropospheric ClNO2 in inland China
NO3 chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO3 radical
Marine gas-phase sulfur emissions during an induced phytoplankton bloom
Biomass burning plume chemistry: OH-radical-initiated oxidation of 3-penten-2-one and its main oxidation product 2-hydroxypropanal
Atmospheric photo-oxidation of myrcene: OH reaction rate constant, gas-phase oxidation products and radical budgets
Characterization of ambient volatile organic compounds, source apportionment, and the ozone–NOx–VOC sensitivities in a heavily polluted megacity of central China: effect of sporting events and emission reductions
Atmospheric oxidation of α,β-unsaturated ketones: kinetics and mechanism of the OH radical reaction
Reactions of NO3 with aromatic aldehydes: gas-phase kinetics and insights into the mechanism of the reaction
Zhu Ran, Yanan Hu, Yuanzhe Li, Xiaoya Gao, Can Ye, Shuai Li, Xiao Lu, Yongming Luo, Sasho Gligorovski, and Jiangping Liu
Atmos. Chem. Phys., 24, 11943–11954, https://doi.org/10.5194/acp-24-11943-2024, https://doi.org/10.5194/acp-24-11943-2024, 2024
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We report enhanced formation of nitrous acid (HONO) and NOx (NO + NO2) triggered by iron ions during photolysis of neonicotinoid insecticides at the air–water interface. This novel previously overlooked source of atmospheric HONO and NOx may be an important contribution to the global nitrogen cycle and affects atmospheric oxidizing capacity and climate change.
Yanyan Xin, Chengtang Liu, Xiaoxiu Lun, Shuyang Xie, Junfeng Liu, and Yujing Mu
Atmos. Chem. Phys., 24, 11409–11429, https://doi.org/10.5194/acp-24-11409-2024, https://doi.org/10.5194/acp-24-11409-2024, 2024
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Rate coefficients for the reactions of OH radicals with C3–C11 alkanes were determined using the multivariate relative-rate technique. A total of 25 relative-rate coefficients at room temperature and 24 Arrhenius expressions in the temperature range of 273–323 K were obtained, which expanded the data available.
Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn
Atmos. Chem. Phys., 24, 9459–9473, https://doi.org/10.5194/acp-24-9459-2024, https://doi.org/10.5194/acp-24-9459-2024, 2024
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∆3-carene is abundantly emitted from vegetation, but its atmospheric oxidation chemistry has received limited attention. We explored highly oxygenated organic molecule (HOM) formation from ∆3-carene ozonolysis in chambers and investigated the impact of temperature and relative humidity on HOM formation. Our findings provide new insights into ∆3-carene oxidation pathways and their potential to impact atmospheric aerosols.
Izabela Kurzydym, Agata Błaziak, Kinga Podgórniak, Karol Kułacz, and Kacper Błaziak
Atmos. Chem. Phys., 24, 9309–9322, https://doi.org/10.5194/acp-24-9309-2024, https://doi.org/10.5194/acp-24-9309-2024, 2024
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This paper outlines a unique scientific strategy for studying the reactivity of atmospherically relevant norpinonic acid (NA). The publication offers a new toolbox, illustrating NA's fragmentation and pattern of kinetic degradation leading to the formation of new small molecules. Furthermore, the research strategy presented here demonstrates how a mass spectrometer can function as a gas-phase reactor and the quantum chemistry method can serve as a reaction model builder.
Florian Berg, Anna Novelli, René Dubus, Andreas Hofzumahaus, Frank Holland, Andreas Wahner, and Hendrik Fuchs
EGUsphere, https://doi.org/10.5194/egusphere-2024-2614, https://doi.org/10.5194/egusphere-2024-2614, 2024
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This study reports temperature dependent reaction rate constants of the reaction of atmospherically relevant hydrocarbons from biogenic sources (MVK, monoterpenes) and anthropogenic sources (alkanes, aromatics). Measurements were done at atmospheric conditions (ambient pressure, temperature range) in air.
Bowen Li, Jian Gao, Chun Chen, Liang Wen, Yuechong Zhang, Junling Li, Yuzhe Zhang, Xiaohui Du, Kai Zhang, and Jiaqi Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2141, https://doi.org/10.5194/egusphere-2024-2141, 2024
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The photolysis rate constants of particulate nitrate for HONO production (JHONO) with PM2.5 samples collected from five representative sites in China varied over a wide range. The parameterization equation between JHONO and OC/NO3− has been established and can be used to estimate JHONO in different environments. Our work provided an important reference for the research in other areas in the world with high proportion of organic components in aerosol samples, such as United States and Europe.
Yuwei Wang, Chuang Li, Ying Zhang, Yueyang Li, Gan Yang, Xueyan Yang, Yizhen Wu, Lei Yao, Hefeng Zhang, and Lin Wang
Atmos. Chem. Phys., 24, 7961–7981, https://doi.org/10.5194/acp-24-7961-2024, https://doi.org/10.5194/acp-24-7961-2024, 2024
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The formation and evolution mechanisms of aromatics-derived highly oxygenated organic molecules (HOMs) are essential to understand the formation of secondary organic aerosol pollution. Our conclusion highlights an underappreciated formation pathway of aromatics-derived HOMs and elucidates detailed formation mechanisms of certain HOMs, which advances our understanding of HOMs and potentially explains the existing gap between model prediction and ambient measurement of the HOMs' concentrations.
Yarê Baker, Sungah Kang, Hui Wang, Rongrong Wu, Jian Xu, Annika Zanders, Quanfu He, Thorsten Hohaus, Till Ziehm, Veronica Geretti, Thomas J. Bannan, Simon P. O'Meara, Aristeidis Voliotis, Mattias Hallquist, Gordon McFiggans, Sören R. Zorn, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 24, 4789–4807, https://doi.org/10.5194/acp-24-4789-2024, https://doi.org/10.5194/acp-24-4789-2024, 2024
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Highly oxygenated organic molecules are important contributors to secondary organic aerosol. Their yield depends on detailed atmospheric chemical composition. One important parameter is the ratio of hydroperoxy radicals to organic peroxy radicals (HO2/RO2), and we show that higher HO2/RO2 ratios lower the secondary organic aerosol yield. This is of importance as laboratory studies are often biased towards organic peroxy radicals.
Lucy V. Brown, Ryan J. Pound, Lyndsay S. Ives, Matthew R. Jones, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 3905–3923, https://doi.org/10.5194/acp-24-3905-2024, https://doi.org/10.5194/acp-24-3905-2024, 2024
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Ozone is deposited from the lower atmosphere to the surface of the ocean; however, the chemical reactions which drive this deposition are currently not well understood. Of particular importance is the reaction between ozone and iodide, and this work measures the kinetics of this reaction and its temperature dependence, which we find to be negligible. We then investigate the subsequent emissions of iodine-containing species from the surface ocean, which can further impact ozone.
Lorrie Simone Denise Jacob, Chiara Giorio, and Alexander Thomas Archibald
Atmos. Chem. Phys., 24, 3329–3347, https://doi.org/10.5194/acp-24-3329-2024, https://doi.org/10.5194/acp-24-3329-2024, 2024
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Recent studies on DMS have provided new challenges to our mechanistic understanding. Here we synthesise a number of recent studies to further develop and extend a state-of-the-art mechanism. Our new mechanism is shown to outperform all existing mechanisms when compared over a wide set of conditions. The development of an improved DMS mechanism will help lead the way to better the understanding the climate impacts of DMS emissions in past, present, and future atmospheric conditions.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
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Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Xi Cheng, Yong Jie Li, Yan Zheng, Keren Liao, Theodore K. Koenig, Yanli Ge, Tong Zhu, Chunxiang Ye, Xinghua Qiu, and Qi Chen
Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, https://doi.org/10.5194/acp-24-2099-2024, 2024
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In this study we conducted laboratory measurements to investigate the formation of gas-phase oxygenated organic molecules (OOMs) from six aromatic volatile organic compounds (VOCs). We provide a thorough analysis on the effects of precursor structure (substituents and ring numbers) on product distribution and highlight from a laboratory perspective that heavy (e.g., double-ring) aromatic VOCs are important in initial particle growth during secondary organic aerosol formation.
Yiwei Gong, Feng Jiang, Yanxia Li, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 167–184, https://doi.org/10.5194/acp-24-167-2024, https://doi.org/10.5194/acp-24-167-2024, 2024
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This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
María Asensio, Sergio Blázquez, María Antiñolo, José Albaladejo, and Elena Jiménez
Atmos. Chem. Phys., 23, 14115–14126, https://doi.org/10.5194/acp-23-14115-2023, https://doi.org/10.5194/acp-23-14115-2023, 2023
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In this work, we focus on the atmospheric chemistry and consequences for air quality of 2-methylpentanal (2MP), which is widely used as a flavoring ingredient and as an intermediate in the synthesis of dyes, resins, and pharmaceuticals. Measurements are presented on how fast 2MP is degraded by sunlight and oxidants like hydroxyl (OH) radicals and chlorine (Cl) atoms and what products are generated. We conclude that 2MP will be degraded in a few hours, affecting local air quality.
Reina S. Buenconsejo, Sophia M. Charan, John H. Seinfeld, and Paul O. Wennberg
EGUsphere, https://doi.org/10.5194/egusphere-2023-2483, https://doi.org/10.5194/egusphere-2023-2483, 2023
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We look at the atmospheric chemistry of a volatile chemical product (VCP), benzyl alcohol. Benzyl alcohol and other VCPs may play a significant role in the formation of urban smog. By better understanding the chemistry of VCPs like benzyl alcohol, we may better understand observed data and how VCPs affect air quality. We identify products formed from benzyl alcohol chemistry and use this chemistry to understand how benzyl alcohol forms a key component of smog, secondary organic aerosol.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Han Zang, Dandan Huang, Jiali Zhong, Ziyue Li, Chenxi Li, Huayun Xiao, and Yue Zhao
Atmos. Chem. Phys., 23, 12691–12705, https://doi.org/10.5194/acp-23-12691-2023, https://doi.org/10.5194/acp-23-12691-2023, 2023
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Acylperoxy radicals (RO2) are key intermediates in the atmospheric oxidation of organic compounds, yet our knowledge of their identities and chemistry remains poor. Using direct measurements and kinetic modeling, we identify the composition and formation pathways of acyl RO2 and quantify their contribution to highly oxygenated organic molecules during α-pinene ozonolysis, which will help to understand oxidation chemistry of monoterpenes and sources of low-volatility organics in the atmosphere.
Jacky Y. S. Pang, Florian Berg, Anna Novelli, Birger Bohn, Michelle Färber, Philip T. M. Carlsson, René Dubus, Georgios I. Gkatzelis, Franz Rohrer, Sergej Wedel, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 12631–12649, https://doi.org/10.5194/acp-23-12631-2023, https://doi.org/10.5194/acp-23-12631-2023, 2023
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In this study, the oxidations of sabinene by OH radicals and ozone were investigated with an atmospheric simulation chamber. Reaction rate coefficients of the OH-oxidation reaction at temperatures between 284 to 340 K were determined for the first time in the laboratory by measuring the OH reactivity. Product yields determined in chamber experiments had good agreement with literature values, but discrepancies were found between experimental yields and expected yields from oxidation mechanisms.
Rolf Sander
Atmos. Chem. Phys., 23, 10901–12440, https://doi.org/10.5194/acp-23-10901-2023, https://doi.org/10.5194/acp-23-10901-2023, 2023
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According to Henry's law, the equilibrium ratio between the abundances in the gas phase and in the aqueous phase is constant for a dilute solution. Henry’s law constants of trace gases of potential importance in environmental chemistry have been collected and converted into a uniform format. The compilation contains 46 434 values of Henry's law constants for 10 173 species, collected from 995 references. It is also available on the internet at https://www.henrys-law.org.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
Shawon Barua, Siddharth Iyer, Avinash Kumar, Prasenjit Seal, and Matti Rissanen
Atmos. Chem. Phys., 23, 10517–10532, https://doi.org/10.5194/acp-23-10517-2023, https://doi.org/10.5194/acp-23-10517-2023, 2023
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This work illustrates how a common volatile hydrocarbon, hexanal, has the potential to undergo atmospheric autoxidation that leads to prompt formation of condensable material that subsequently contributes to aerosol formation, deteriorating the air quality of urban atmospheres. We used the combined state-of-the-art quantum chemical modeling and experimental flow reactor experiments under atmospheric conditions to resolve the autoxidation mechanism of hexanal initiated by a common oxidant.
Yixin Hao, Jun Zhou, Jie-Ping Zhou, Yan Wang, Suxia Yang, Yibo Huangfu, Xiao-Bing Li, Chunsheng Zhang, Aiming Liu, Yanfeng Wu, Yaqing Zhou, Shuchun Yang, Yuwen Peng, Jipeng Qi, Xianjun He, Xin Song, Yubin Chen, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 23, 9891–9910, https://doi.org/10.5194/acp-23-9891-2023, https://doi.org/10.5194/acp-23-9891-2023, 2023
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By employing an improved net photochemical ozone production rate (NPOPR) detection system based on the dual-channel reaction chamber technique, we measured the net photochemical ozone production rate in the Pearl River Delta in China. The photochemical ozone formation mechanisms in the reaction and reference chambers were investigated using the observation-data-constrained box model, which helped us to validate the NPOPR detection system and understand photochemical ozone formation mechanism.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Caterina Mapelli, James K. Donnelly, Úna E. Hogan, Andrew R. Rickard, Abbie T. Robinson, Fergal Byrne, Con Rob McElroy, Basile F. E. Curchod, Daniel Hollas, and Terry J. Dillon
Atmos. Chem. Phys., 23, 7767–7779, https://doi.org/10.5194/acp-23-7767-2023, https://doi.org/10.5194/acp-23-7767-2023, 2023
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Solvents are chemical compounds with countless uses in the chemical industry, and they also represent one of the main sources of pollution in the chemical sector. Scientists are trying to develop new
greensafer solvents which present favourable advantages when compared to traditional solvents. Since the assessment of these green solvents often lacks air quality considerations, this study aims to understand the behaviour of these compounds, investigating their reactivity in the troposphere.
Roland Benoit, Nesrine Belhadj, Zahraa Dbouk, Maxence Lailliau, and Philippe Dagaut
Atmos. Chem. Phys., 23, 5715–5733, https://doi.org/10.5194/acp-23-5715-2023, https://doi.org/10.5194/acp-23-5715-2023, 2023
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We observed a surprisingly similar set of oxidation product chemical formulas from limonene and α-pinene, including oligomers, formed under cool-flame (present experiments) and simulated atmospheric oxidation (literature). Data analysis indicated that a subset of chemical formulas is common to all experiments independently of experimental conditions. Also, this study indicates that many detected chemical formulas can be ascribed to an autooxidation reaction.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
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The investigation of the night-time oxidation of the most abundant hydrocarbon, isoprene, in chamber experiments shows the importance of reaction pathways leading to epoxy products, which could enhance particle formation, that have so far not been accounted for. The chemical lifetime of organic nitrates from isoprene is long enough for the majority to be further oxidized the next day by daytime oxidants.
Kevin D. Easterbrook, Mitchell A. Vona, Kiana Nayebi-Astaneh, Amanda M. Miller, and Hans D. Osthoff
Atmos. Chem. Phys., 23, 311–322, https://doi.org/10.5194/acp-23-311-2023, https://doi.org/10.5194/acp-23-311-2023, 2023
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The trace gas peroxypropionyl nitrate (PPN) is generated in photochemical smog, phytotoxic, a strong eye irritant, and possibly mutagenic. Here, its solubility and reactivity in water and in octanol were investigated using a bubble flow apparatus, yielding its Henry's law constant and octanol–water partition coefficient (Kow). The results allow the fate of PPN to be more accurately constrained in atmospheric chemical transport models, including its uptake on clouds, organic aerosol, and leaves.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Caterina Mapelli, Juliette V. Schleicher, Alex Hawtin, Conor D. Rankine, Fiona C. Whiting, Fergal Byrne, C. Rob McElroy, Claudiu Roman, Cecilia Arsene, Romeo I. Olariu, Iustinian G. Bejan, and Terry J. Dillon
Atmos. Chem. Phys., 22, 14589–14602, https://doi.org/10.5194/acp-22-14589-2022, https://doi.org/10.5194/acp-22-14589-2022, 2022
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Solvents represent an important source of pollution from the chemical industry. New "green" solvents aim to replace toxic solvents with new molecules made from renewable sources and designed to be less harmful. Whilst these new molecules are selected according to toxicity and other characteristics, no consideration has yet been included on air quality. Studying the solvent breakdown in air, we found that TMO has a lower impact on air quality than traditional solvents with similar properties.
Kai Song, Song Guo, Yuanzheng Gong, Daqi Lv, Yuan Zhang, Zichao Wan, Tianyu Li, Wenfei Zhu, Hui Wang, Ying Yu, Rui Tan, Ruizhe Shen, Sihua Lu, Shuangde Li, Yunfa Chen, and Min Hu
Atmos. Chem. Phys., 22, 9827–9841, https://doi.org/10.5194/acp-22-9827-2022, https://doi.org/10.5194/acp-22-9827-2022, 2022
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Emissions from four typical Chinese domestic cooking and fried chicken using four kinds of oils were investigated to illustrate the impact of cooking style and oil. Of the estimated SOA, 10.2 %–32.0 % could be explained by S/IVOC oxidation. Multiway principal component analysis (MPCA) emphasizes the importance of the unsaturated fatty acid-alkadienal volatile product mechanism (oil autoxidation) accelerated by the cooking and heating procedure.
Michelia Dam, Danielle C. Draper, Andrey Marsavin, Juliane L. Fry, and James N. Smith
Atmos. Chem. Phys., 22, 9017–9031, https://doi.org/10.5194/acp-22-9017-2022, https://doi.org/10.5194/acp-22-9017-2022, 2022
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We performed chamber experiments to measure the composition of the gas-phase reaction products of nitrate-radical-initiated oxidation of four monoterpenes. The total organic yield, effective oxygen-to-carbon ratio, and dimer-to-monomer ratio were correlated with the observed particle formation for the monoterpene systems with some exceptions. The Δ-carene system produced the most particles, followed by β-pinene, with the α-pinene and α-thujene systems producing no particles.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip T. M. Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 22, 8497–8527, https://doi.org/10.5194/acp-22-8497-2022, https://doi.org/10.5194/acp-22-8497-2022, 2022
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This study investigates the radical chemical budget during the limonene oxidation at different atmospheric-relevant NO concentrations in chamber experiments under atmospheric conditions. It is found that the model–measurement discrepancies of HO2 and RO2 are very large at low NO concentrations that are typical for forested environments. Possible additional processes impacting HO2 and RO2 concentrations are discussed.
Carmen Maria Tovar, Ian Barnes, Iustinian Gabriel Bejan, and Peter Wiesen
Atmos. Chem. Phys., 22, 6989–7004, https://doi.org/10.5194/acp-22-6989-2022, https://doi.org/10.5194/acp-22-6989-2022, 2022
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This work explores the kinetics and reactivity of epoxides towards the OH radical using two different simulation chambers. Estimation of the rate coefficients has also been made using different structure–activity relationship (SAR) approaches. The results indicate a direct influence of the structural and geometric properties of the epoxides not considered in SAR estimations, influencing the reactivity of these compounds. The outcomes of this work are in very good agreement with previous studies.
Axel Fouqueau, Manuela Cirtog, Mathieu Cazaunau, Edouard Pangui, Jean-François Doussin, and Bénédicte Picquet-Varrault
Atmos. Chem. Phys., 22, 6411–6434, https://doi.org/10.5194/acp-22-6411-2022, https://doi.org/10.5194/acp-22-6411-2022, 2022
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Biogenic volatile organic compounds are intensely emitted by forests and crops and react with the nitrate radical during the nighttime to form functionalized products. The purpose of this study is to furnish kinetic and mechanistic data for terpinolene and β-caryophyllene, using simulation chamber experiments. Rate constants have been measured using both relative and absolute methods, and mechanistic studies have been conducted in order to identify and quantify the main reaction products.
Yuanyuan Luo, Olga Garmash, Haiyan Li, Frans Graeffe, Arnaud P. Praplan, Anssi Liikanen, Yanjun Zhang, Melissa Meder, Otso Peräkylä, Josep Peñuelas, Ana María Yáñez-Serrano, and Mikael Ehn
Atmos. Chem. Phys., 22, 5619–5637, https://doi.org/10.5194/acp-22-5619-2022, https://doi.org/10.5194/acp-22-5619-2022, 2022
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Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and we characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Haoyu Jiang, Yingyao He, Yiqun Wang, Sheng Li, Bin Jiang, Luca Carena, Xue Li, Lihua Yang, Tiangang Luan, Davide Vione, and Sasho Gligorovski
Atmos. Chem. Phys., 22, 4237–4252, https://doi.org/10.5194/acp-22-4237-2022, https://doi.org/10.5194/acp-22-4237-2022, 2022
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Heterogeneous oxidation of SO2 is suggested to be one of the most important pathways for sulfate formation during extreme haze events in China, yet the exact mechanism remains highly uncertain. Our study reveals that ubiquitous compounds at the sea surface PAHS and DMSO, when exposed to SO2 under simulated sunlight irradiation, generate abundant organic sulfur compounds, providing implications for air-sea interaction and secondary organic aerosols formation processes.
Roland Vernooij, Ulrike Dusek, Maria Elena Popa, Peng Yao, Anupam Shaikat, Chenxi Qiu, Patrik Winiger, Carina van der Veen, Thomas Callum Eames, Natasha Ribeiro, and Guido R. van der Werf
Atmos. Chem. Phys., 22, 2871–2890, https://doi.org/10.5194/acp-22-2871-2022, https://doi.org/10.5194/acp-22-2871-2022, 2022
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Landscape fires are a major source of greenhouse gases and aerosols, particularly in sub-tropical savannas. Stable carbon isotopes in emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to greenhouse gases and aerosols if the process is well understood. This helps us to link individual vegetation types to emissions, identify biomass burning emissions in the atmosphere, and improve the reconstruction of historic fire regimes.
María Asensio, María Antiñolo, Sergio Blázquez, José Albaladejo, and Elena Jiménez
Atmos. Chem. Phys., 22, 2689–2701, https://doi.org/10.5194/acp-22-2689-2022, https://doi.org/10.5194/acp-22-2689-2022, 2022
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The diurnal atmospheric degradation of 2-methylbutanal, 2 MB, emitted by sources like vegetation or the poultry industry is evaluated in this work. Sunlight and oxidants like hydroxyl (OH) radicals and chlorine (Cl) atoms initiate this degradation. Measurements of how fast 2 MB is degraded and what products are generated are presented. The lifetime of 2 MB is around 1 h at noon, when the OH reaction dominates. Thus, 2 MB will not be transported far, affecting only local air quality.
Claudiu Roman, Cecilia Arsene, Iustinian Gabriel Bejan, and Romeo Iulian Olariu
Atmos. Chem. Phys., 22, 2203–2219, https://doi.org/10.5194/acp-22-2203-2022, https://doi.org/10.5194/acp-22-2203-2022, 2022
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Gas-phase reaction rate coefficients of OH radicals with four nitrocatechols have been investigated for the first time by using ESC-Q-UAIC chamber facilities. The reactivity of all investigated nitrocatechols is influenced by the formation of the intramolecular H-bonds that are connected to the deactivating electromeric effect of the NO2 group. For the 3-nitrocatechol compounds, the electromeric effect of the
freeOH group is diminished by the deactivating E-effect of the NO2 group.
Zhiyuan Gao, Nicolas-Xavier Geilfus, Alfonso Saiz-Lopez, and Feiyue Wang
Atmos. Chem. Phys., 22, 1811–1824, https://doi.org/10.5194/acp-22-1811-2022, https://doi.org/10.5194/acp-22-1811-2022, 2022
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Every spring in the Arctic, a series of photochemical events occur over the ice-covered ocean, known as bromine explosion events, ozone depletion events, and mercury depletion events. Here we report the re-creation of these events at an outdoor sea ice facility in Winnipeg, Canada, far away from the Arctic. The success provides a new platform with new opportunities to uncover fundamental mechanisms of these Arctic springtime phenomena and how they may change in a changing climate.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Mike J. Newland, Yangang Ren, Max R. McGillen, Lisa Michelat, Véronique Daële, and Abdelwahid Mellouki
Atmos. Chem. Phys., 22, 1761–1772, https://doi.org/10.5194/acp-22-1761-2022, https://doi.org/10.5194/acp-22-1761-2022, 2022
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Wildfires are increasing in extent and severity, driven by climate change. Such fires emit large amounts of volatile organic compounds (VOCs) to the atmosphere. Many of these, such as the furans studied here, are very reactive and are rapidly converted to other VOCs, which are expected to have negative health effects and to further impact the climate. Here, we establish the importance of the nitrate radical for removing these compounds both during the night and during the day.
Delaney B. Kilgour, Gordon A. Novak, Jon S. Sauer, Alexia N. Moore, Julie Dinasquet, Sarah Amiri, Emily B. Franklin, Kathryn Mayer, Margaux Winter, Clare K. Morris, Tyler Price, Francesca Malfatti, Daniel R. Crocker, Christopher Lee, Christopher D. Cappa, Allen H. Goldstein, Kimberly A. Prather, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 1601–1613, https://doi.org/10.5194/acp-22-1601-2022, https://doi.org/10.5194/acp-22-1601-2022, 2022
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We report measurements of gas-phase volatile organosulfur molecules made during a mesocosm phytoplankton bloom experiment. Dimethyl sulfide (DMS), methanethiol (MeSH), and benzothiazole accounted for on average over 90 % of total gas-phase sulfur emissions. This work focuses on factors controlling the production and emission of DMS and MeSH and the role of non-DMS molecules (such as MeSH and benzothiazole) in secondary sulfate formation in coastal marine environments.
Niklas Illmann, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys., 21, 18557–18572, https://doi.org/10.5194/acp-21-18557-2021, https://doi.org/10.5194/acp-21-18557-2021, 2021
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Understanding the chemistry of biomass burning plumes is of global interest. Within this work we investigated the OH radical reaction of 3-penten-2-one, which has been identified in biomass burning emissions. We observed the primary formation of peroxyacetyl nitrate (PAN), a key NOx reservoir species. Besides, PAN precursors were also identified as main oxidation products. 3-Penten-2-one is shown to be an example explaining rapid PAN formation within young biomass burning plumes.
Zhaofeng Tan, Luisa Hantschke, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Changmin Cho, Hans-Peter Dorn, Xin Li, Anna Novelli, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 16067–16091, https://doi.org/10.5194/acp-21-16067-2021, https://doi.org/10.5194/acp-21-16067-2021, 2021
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The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR. The chemical structure of myrcene is partly similar to isoprene. Therefore, it can be expected that hydrogen shift reactions could play a role as observed for isoprene. In this work, their potential impact on the regeneration efficiency of hydroxyl radicals is investigated.
Shijie Yu, Fangcheng Su, Shasha Yin, Shenbo Wang, Ruixin Xu, Bing He, Xiangge Fan, Minghao Yuan, and Ruiqin Zhang
Atmos. Chem. Phys., 21, 15239–15257, https://doi.org/10.5194/acp-21-15239-2021, https://doi.org/10.5194/acp-21-15239-2021, 2021
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This study measured 106 VOC species using a GC-MS/FID. Meanwhile, the WRF-CMAQ model was used to investigate the nonlinearity of the O3 response to precursor reductions. This study highlights the effectiveness of stringent emission controls in relation to solvent utilization and coal combustion. However, unreasonable emission reduction may aggravate ozone pollution during control periods. It is suggested that emission-reduction ratios of the precursors (VOC : NOx) should be more than 2.
Niklas Illmann, Rodrigo Gastón Gibilisco, Iustinian Gabriel Bejan, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys., 21, 13667–13686, https://doi.org/10.5194/acp-21-13667-2021, https://doi.org/10.5194/acp-21-13667-2021, 2021
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Within this work we determined the rate coefficients and products of the reaction of unsaturated ketones with OH radicals in an effort to complete the gaps in the knowledge needed for modelling chemistry in the atmosphere. Both substances are potentially emitted by biomass burning, industrial activities or formed in the troposphere by oxidation of terpenes. As products we identified aldehydes and ketones which in turn are known to be responsible for the transportation of NOx species.
Yangang Ren, Li Zhou, Abdelwahid Mellouki, Véronique Daële, Mahmoud Idir, Steven S. Brown, Branko Ruscic, Robert S. Paton, Max R. McGillen, and A. R. Ravishankara
Atmos. Chem. Phys., 21, 13537–13551, https://doi.org/10.5194/acp-21-13537-2021, https://doi.org/10.5194/acp-21-13537-2021, 2021
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Aromatic aldehydes are a family of compounds emitted into the atmosphere from both anthropogenic and biogenic sources that are formed from the degradation of aromatic hydrocarbons. Their atmospheric degradation may impact air quality. We report on their atmospheric degradation through reaction with NO3, which is useful to estimate their atmospheric lifetimes. We have also attempted to elucidate the mechanism of these reactions via studies of isotopic substitution and quantum chemistry.
Cited articles
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Akagi, S. K., Yokelson, R. J., Wiedinmyer, C., Alvarado, M. J., Reid, J. S., Karl, T., Crounse, J. D., and Wennberg, P. O.: Emission factors for open and domestic biomass burning for use in atmospheric models, Atmos. Chem. Phys., 11, 4039–4072, https://doi.org/10.5194/acp-11-4039-2011, 2011.
Akagi, S. K., Craven, J. S., Taylor, J. W., McMeeking, G. R., Yokelson, R. J., Burling, I. R., Urbanski, S. P., Wold, C. E., Seinfeld, J. H., Coe, H., Alvarado, M. J., and Weise, D. R.: Evolution of trace gases and particles emitted by a chaparral fire in California, Atmos. Chem. Phys., 12, 1397–1421, https://doi.org/10.5194/acp-12-1397-2012, 2012.
Alvarado, M. J. and Prinn, R. G.: Formation of ozone and growth of aerosols in young smoke plumes from biomass burning: 1. Lagrangian parcel studies, J. Geophys. Res.-Atmos., 114, D09306, https://doi.org/10.1029/2008jd011144, 2009.
Alvarado, M. J., Lonsdale, C. R., Yokelson, R. J., Akagi, S. K., Coe, H., Craven, J. S., Fischer, E. V., McMeeking, G. R., Seinfeld, J. H., Soni, T., Taylor, J. W., Weise, D. R., and Wold, C. E.: Investigating the links between ozone and organic aerosol chemistry in a biomass burning plume from a prescribed fire in California chaparral, Atmos. Chem. Phys., 15, 6667–6688, https://doi.org/10.5194/acp-15-6667-2015, 2015.
Alvarez, E. G., Borras, E., Viidanoja, J., and Hjorth, J.: Unsaturated dicarbonyl products from the OH-initiated photo-oxidation of furan, 2-methylfuran and 3-methylfuran, Atmos. Environ., 43, 1603–1612, https://doi.org/10.1016/j.atmosenv.2008.12.019, 2009.
Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, 2001.
Bahreini, R., Middlebrook, A. M., de Gouw, J. A., Warneke, C., Trainer, M., Brock, C. A., Stark, H., Brown, S. S., Dube, W. P., Gilman, J. B., Hall, K., Holloway, J. S., Kuster, W. C., Perring, A. E., Prevot, A. S. H., Schwarz, J. P., Spackman, J. R., Szidat, S., Wagner, N. L., Weber, R. J., Zotter, P., and Parrish, D. D.: Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass, Geophys. Res. Lett., 39, L06805, https://doi.org/10.1029/2011gl050718, 2012.
Bierbach, A., Barnes, I., and Becker, K. H.: Rate Coefficients For The Gas-Phase Reactions Of Hydroxyl Radicals With Furan, 2-Methylfuran, 2-Ethylfuran And 2,5-Dimethylfuran At 300 +/- 2-K, Atmos. Environ., 26, 813–817, 1992.
Bierbach, A., Barnes, I., and Becker, K. H.: Product and kinetic study of the oh-initiated gas-phase oxidation of Furan, 2-methylfuran and furanaldehydes at 300 K, Atmos. Environ., 29, 2651-2660, https://doi.org/10.1016/1352-2310(95)00096-H, 1995.
Burling, I. R., Yokelson, R. J., Griffith, D. W. T., Johnson, T. J., Veres, P., Roberts, J. M., Warneke, C., Urbanski, S. P., Reardon, J., Weise, D. R., Hao, W. M., and de Gouw, J.: Laboratory measurements of trace gas emissions from biomass burning of fuel types from the southeastern and southwestern United States, Atmos. Chem. Phys., 10, 11115–11130, https://doi.org/10.5194/acp-10-11115-2010, 2010.
Burling, I. R., Yokelson, R. J., Akagi, S. K., Urbanski, S. P., Wold, C. E., Griffith, D. W. T., Johnson, T. J., Reardon, J., and Weise, D. R.: Airborne and ground-based measurements of the trace gases and particles emitted by prescribed fires in the United States, Atmos. Chem. Phys., 11, 12197–12216, https://doi.org/10.5194/acp-11-12197-2011, 2011.
Christian, T. J., Kleiss, B., Yokelson, R. J., Holzinger, R., Crutzen, P. J., Hao, W. M., Saharjo, B. H., and Ward, D. E.: Comprehensive laboratory measurements of biomass-burning emissions: 1. Emissions from Indonesian, African, and other fuels, J. Geophys. Res., 108, 4719, https://doi.org/10.1029/2003JD003704, 2003.
Christian, T. J., Kleiss, B., Yokelson, R. J., Holzinger, R., Crutzen, P. J., Hao, W. M., Shirai, T., and Blake, D. R.: Comprehensive laboratory measurements of biomass-burning emissions: 2. First intercomparison of open-path FTIR, PTR-MS, and GC- MS/FID/ECD, J. Geophys. Res., 109, D02311, https://doi.org/10.1029/2003JD003874, 2004.
Crutzen, P. J. and Andreae, M. O.: Biomass burning in the Tropics – impact on atmospheric chemistry and biogeochemical cycles, Science, 250, 1669–1678, https://doi.org/10.1126/science.250.4988.1669, 1990.
de Gouw, J. A., Warneke, C., Parrish, D. D., Holloway, J. S., Trainer, M., and Fehsenfeld, F. C.: Emission sources and ocean uptake of acetonitrile (CH3CN) in the atmosphere, J. Geophys. Res.-Atmos., 108, 4329, https://doi.org/10.1029/2002jd002897, 2003.
de Gouw, J. A., Middlebrook, A. M., Warneke, C., Goldan, P. D., Kuster, W. C., Roberts, J. M., Fehsenfeld, F. C., Worsnop, D. R., Canagaratna, M. R., Pszenny, A. A. P., Keene, W. C., Marchewka, M., Bertman, S. B., and Bates, T. S.: Budget of organic carbon in a polluted atmosphere: Results from the New England Air Quality Study in 2002, J. Geophys. Res.-Atmos., 110, D16305, https://doi.org/10.1029/2004JD005623, 2005.
de Gouw, J. A., Warneke, C., Stohl, A., Wollny, A. G., Brock, C. A., Cooper, O. R., Holloway, J. S., Trainer, M., Fehsenfeld, F. C., Atlas, E. L., Donnelly, S. G., Stroud, V., and Lueb, A.: Volatile organic compounds composition of merged and aged forest fire plumes from Alaska and western Canada, J. Geophys. Res.-Atmos., 111, D10303, https://doi.org/10.1029/2005JD006175, 2006.
Demirbas, M. F. and Demirbas, T.: Hazardous emissions from combustion of biomass, Energ. Source, 31, 527–534, https://doi.org/10.1080/15567030802466953, 2009.
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Short summary
A comprehensive suite of instruments was used to quantify the emissions of over 200 organic and inorganic gases from 56 laboratory burns of 18 different biomass fuel types common in the southeastern, southwestern, or northern United States. Emission ratios relative to carbon monoxide (CO) are used to characterize the composition of gases emitted by mass; OH reactivity; and potential secondary organic aerosol (SOA) precursors for the three different U.S. fuel regions presented here.
A comprehensive suite of instruments was used to quantify the emissions of over 200 organic and...
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