Articles | Volume 13, issue 22
https://doi.org/10.5194/acp-13-11317-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-13-11317-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
22 Nov 2013
Research article |
| 22 Nov 2013
Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX
S. S. Brown
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
W. P. Dubé
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
R. Bahreini
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
now at: Department of Environmental Sciences, University of California, Riverside, CA, 92521, USA
A. M. Middlebrook
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
C. A. Brock
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
C. Warneke
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
J. A. de Gouw
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
R. A. Washenfelder
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
RSMAS/MAC, University of Miami, 4600 Rickenbacker Causeway, Miami, FL 33149, USA
J. Peischl
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
T. B. Ryerson
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
J. S. Holloway
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
J. P. Schwarz
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
R. Spackman
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
M. Trainer
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
D. D. Parrish
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
F. C. Fehshenfeld
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
A. R. Ravishankara
NOAA Earth System Research Laboratory, Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, USA
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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
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Andrew O. Langford, Christoph J. Senff, Raul J. Alvarez II, Ken C. Aikin, Sunil Baidar, Timothy A. Bonin, W. Alan Brewer, Jerome Brioude, Steven S. Brown, Joel D. Burley, Dani J. Caputi, Stephen A. Conley, Patrick D. Cullis, Zachary C. J. Decker, Stéphanie Evan, Guillaume Kirgis, Meiyun Lin, Mariusz Pagowski, Jeff Peischl, Irina Petropavlovskikh, R. Bradley Pierce, Thomas B. Ryerson, Scott P. Sandberg, Chance W. Sterling, Ann M. Weickmann, and Li Zhang
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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.
Quanfu He, Zheng Fang, Ofir Shoshanim, Steven S. Brown, and Yinon Rudich
Atmos. Chem. Phys., 21, 14927–14940, https://doi.org/10.5194/acp-21-14927-2021, https://doi.org/10.5194/acp-21-14927-2021, 2021
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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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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.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Caroline C. Womack, Katherine M. Manfred, Nicholas L. Wagner, Gabriela Adler, Alessandro Franchin, Kara D. Lamb, Ann M. Middlebrook, Joshua P. Schwarz, Charles A. Brock, Steven S. Brown, and Rebecca A. Washenfelder
Atmos. Chem. Phys., 21, 7235–7252, https://doi.org/10.5194/acp-21-7235-2021, https://doi.org/10.5194/acp-21-7235-2021, 2021
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Microscopic particles interact with sunlight and affect the earth's climate in ways that are not fully understood. Aerosols from wildfire smoke present particular challenges due to their complexity in shape and composition. We demonstrate that we can experimentally measure aerosol optical properties for many types of smoke particles, using measurements of smoke from controlled burns, but that the method does not work well for smoke with high soot content.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
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.
Andrew W. Rollins, Pamela S. Rickly, Ru-Shan Gao, Thomas B. Ryerson, Steven S. Brown, Jeff Peischl, and Ilann Bourgeois
Atmos. Meas. Tech., 13, 2425–2439, https://doi.org/10.5194/amt-13-2425-2020, https://doi.org/10.5194/amt-13-2425-2020, 2020
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Nitric oxide (NO) is a key atmospheric constituent controlling atmospheric oxidation chemistry and tropospheric ozone formation. Existing instrumentation capable of quantifying NO at very low mixing ratios is uncommon and typically relies on chemiluminescence. We describe and demonstrate a new laser-based technique (LIF) with significant practical and technical advantages to CL. This technique is expected to allow for advances in understanding of atmospheric radical chemistry.
Chuan Yu, Zhe Wang, Men Xia, Xiao Fu, Weihao Wang, Yee Jun Tham, Tianshu Chen, Penggang Zheng, Hongyong Li, Ye Shan, Xinfeng Wang, Likun Xue, Yan Zhou, Dingli Yue, Yubo Ou, Jian Gao, Keding Lu, Steven S. Brown, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 20, 4367–4378, https://doi.org/10.5194/acp-20-4367-2020, https://doi.org/10.5194/acp-20-4367-2020, 2020
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This study provides a holistic picture of N2O5 heterogeneous uptake on ambient aerosols and the influencing factors under various climatic and chemical conditions in China, and it proposes an observation-based empirical parameterization. The empirical parameterization can be used in air quality models to improve the prediction of PM2.5 and photochemical pollution in China and similar polluted regions of the world.
Alexander Moravek, Jennifer G. Murphy, Amy Hrdina, John C. Lin, Christopher Pennell, Alessandro Franchin, Ann M. Middlebrook, Dorothy L. Fibiger, Caroline C. Womack, Erin E. McDuffie, Randal Martin, Kori Moore, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 15691–15709, https://doi.org/10.5194/acp-19-15691-2019, https://doi.org/10.5194/acp-19-15691-2019, 2019
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Ammonium nitrate is a major component of fine particulate matter of wintertime air pollution in the Great Salt Lake Region (UT, USA). We investigate the sources of ammonia in the region by using aircraft observations and comparing them to modelled ammonia mixing ratios based on emission inventory estimates. The results suggest that ammonia emissions are underestimated, specifically in regions with high agricultural activity, while ammonia in Salt Lake City is mainly of local origin.
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.
Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 9287–9308, https://doi.org/10.5194/acp-19-9287-2019, https://doi.org/10.5194/acp-19-9287-2019, 2019
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Populated mountain basins, including the Salt Lake Valley (SLV) in Utah, suffer from wintertime stagnation events that trap emissions near the surface and cause fine particulate matter (PM2.5) concentrations to reach unhealthy levels. Previously limited by a lack of nighttime measurements, this study uses 2017 UWFPS aircraft campaign data, in combination with a box model, to show that nitrogen chemistry above the surface at night is a major source of PM2.5 during a wintertime event in the SLV.
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.
Nick Jordan, Connie Z. Ye, Satyaki Ghosh, Rebecca A. Washenfelder, Steven S. Brown, and Hans D. Osthoff
Atmos. Meas. Tech., 12, 1277–1293, https://doi.org/10.5194/amt-12-1277-2019, https://doi.org/10.5194/amt-12-1277-2019, 2019
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A new spectrometer to measure abundances of the atmospheric trace gases nitrogen dioxide and iodine is described. The spectrometer uses a light-emitting diode between 470 and 540 nm and two highly reflective mirrors to yield an effective absorption path of 6.3 km. We remeasured scattering cross sections of common atmospheric gases in the cyan region and present sample NO2 measurements that agreed with those made with a laser-based instrument.
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
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We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
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 %.
James M. Mattila, Patrick Brophy, Jeffrey Kirkland, Samuel Hall, Kirk Ullmann, Emily V. Fischer, Steve Brown, Erin McDuffie, Alex Tevlin, and Delphine K. Farmer
Atmos. Chem. Phys., 18, 12315–12327, https://doi.org/10.5194/acp-18-12315-2018, https://doi.org/10.5194/acp-18-12315-2018, 2018
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Molecular acids in the atmosphere have implications for human health and air quality. Measurements of various acidic molecules were performed in the Colorado Front Range. Atmospheric concentrations of many acids increased during the day, indicative of sunlight-related production sources. A surface-level source of many acids persisting throughout day and night was observed. Traffic and agricultural activity were important anthropogenic sources of several acids near the measurement site.
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.
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.
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.
Lihua Wang, Michael J. Newchurch, Raul J. Alvarez II, Timothy A. Berkoff, Steven S. Brown, William Carrion, Russell J. De Young, Bryan J. Johnson, Rene Ganoe, Guillaume Gronoff, Guillaume Kirgis, Shi Kuang, Andrew O. Langford, Thierry Leblanc, Erin E. McDuffie, Thomas J. McGee, Denis Pliutau, Christoph J. Senff, John T. Sullivan, Grant Sumnicht, Laurence W. Twigg, and Andrew J. Weinheimer
Atmos. Meas. Tech., 10, 3865–3876, https://doi.org/10.5194/amt-10-3865-2017, https://doi.org/10.5194/amt-10-3865-2017, 2017
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Intercomparisons have been made between three TOLNet ozone lidars and between the lidars and other ozone instruments during the 2014 DISCOVER-AQ and FRAPPÉ campaigns in Colorado. Overall, the TOLNet lidars are capable of measuring 5 min tropospheric ozone variations with accuracy better than ±15 % in terms of their vertical resolving capability and better than ±5 % in terms of their column average measurement. These results indicate very good measurement accuracy for the three TOLNet lidars.
Bianca C. Baier, William H. Brune, David O. Miller, Donald Blake, Russell Long, Armin Wisthaler, Christopher Cantrell, Alan Fried, Brian Heikes, Steven Brown, Erin McDuffie, Frank Flocke, Eric Apel, Lisa Kaser, and Andrew Weinheimer
Atmos. Chem. Phys., 17, 11273–11292, https://doi.org/10.5194/acp-17-11273-2017, https://doi.org/10.5194/acp-17-11273-2017, 2017
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Ozone production rates were measured using the Measurement of Ozone Production Sensor (MOPS). Measurements are compared to modeled ozone production rates using two different chemical mechanisms. At high nitric oxide levels, observed rates are higher than those modeled, prompting the need to revisit current model photochemistry. These direct measurements can add to our understanding of the ozone chemistry within air quality models and can be used to guide government regulatory strategies.
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.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
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.
Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Amber M. Ortega, Juliane L. Fry, Steven S. Brown, Kyle J. Zarzana, William Dube, Nicholas L. Wagner, Danielle C. Draper, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5331–5354, https://doi.org/10.5194/acp-17-5331-2017, https://doi.org/10.5194/acp-17-5331-2017, 2017
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Ambient forest air was oxidized by OH, O3, or NO3 inside an oxidation flow reactor, leading to formation of particulate matter from any gaseous precursors found in the air. Closure was achieved between the amount of particulate mass formed from O3 and NO3 oxidation and the amount predicted from speciated gaseous precursors, which was in contrast to previous results for OH oxidation (Palm et al., 2016). Elemental analysis of the particulate mass formed in the reactor is presented.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Hendrik Fuchs, Zhaofeng Tan, Keding Lu, Birger Bohn, Sebastian Broch, Steven S. Brown, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Kyung-Eun Min, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinson Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 645–661, https://doi.org/10.5194/acp-17-645-2017, https://doi.org/10.5194/acp-17-645-2017, 2017
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OH reactivity was measured during a 1-month long campaign at a rural site in the North China Plain in 2014. OH reactivity measurements are compared to calculations using OH reactant measurements. Good agreement is found indicating that all important OH reactants were measured. In addition, the chemical OH budget is analyzed. In contrast to previous campaigns in China in 2006, no significant imbalance between OH production and destruction is found.
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.
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.
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.
K.-E. Min, R. A. Washenfelder, W. P. Dubé, A. O. Langford, P. M. Edwards, K. J. Zarzana, J. Stutz, K. Lu, F. Rohrer, Y. Zhang, and S. S. Brown
Atmos. Meas. Tech., 9, 423–440, https://doi.org/10.5194/amt-9-423-2016, https://doi.org/10.5194/amt-9-423-2016, 2016
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We have developed a two-channel broadband cavity enhanced absorption spectrometer for field measurements of glyoxal, methylglyoxal, nitrous acid, nitrogen dioxide, and water. We have successfully deployed this instrument during two aircraft and two ground-based field campaigns. The demonstrated precision (2σ) for retrievals of CHOCHO, HONO, and NO2 are 34, 350, and 80 parts per trillion (pptv) in 5 s, with accuracy of 5.8, 9.0 and 5.0 %.
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.
R. A. Washenfelder, A. R. Attwood, J. M. Flores, K. J. Zarzana, Y. Rudich, and S. S. Brown
Atmos. Meas. Tech., 9, 41–52, https://doi.org/10.5194/amt-9-41-2016, https://doi.org/10.5194/amt-9-41-2016, 2016
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Formaldehyde is the most abundant aldehyde in the atmosphere and plays an important role in photochemistry. Broadband cavity-enhanced absorption spectroscopy uses a high finesse cavity to obtain effective path lengths of kilometers. We use a diode-pumped plasma lamp and custom cavity mirrors to extend this technique further into the ultraviolet spectral region, and we achieve detection limits of hundreds of parts per trillion in 1 min for formaldehyde and nitrogen dioxide.
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.
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
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.
P. A. Cleary, N. Fuhrman, L. Schulz, J. Schafer, J. Fillingham, H. Bootsma, J. McQueen, Y. Tang, T. Langel, S. McKeen, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 15, 5109–5122, https://doi.org/10.5194/acp-15-5109-2015, https://doi.org/10.5194/acp-15-5109-2015, 2015
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This study examines ozone mixing ratios over Lake Michigan as measured on the Lake Express ferry, by shoreline differential optical absorption spectroscopy (DOAS) observations in southeastern Wisconsin, and as predicted by the Community Multiscale Air Quality (CMAQ) model. Over water, ozone was determined to be an average of 3.8ppb higher than shoreline observations but overpredicted by the CMAQ model by as much as 11-16ppb midday.
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.
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
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
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
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
J. L. Fry, D. C. Draper, K. J. Zarzana, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, S. S. Brown, R. C. Cohen, L. Kaser, A. Hansel, L. Cappellin, T. Karl, A. Hodzic Roux, A. Turnipseed, C. Cantrell, B. L. Lefer, and N. Grossberg
Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, https://doi.org/10.5194/acp-13-8585-2013, 2013
H.-P. Dorn, R. L. Apodaca, S. M. Ball, T. Brauers, S. S. Brown, J. N. Crowley, W. P. Dubé, H. Fuchs, R. Häseler, U. Heitmann, R. L. Jones, A. Kiendler-Scharr, I. Labazan, J. M. Langridge, J. Meinen, T. F. Mentel, U. Platt, D. Pöhler, F. Rohrer, A. A. Ruth, E. Schlosser, G. Schuster, A. J. L. Shillings, W. R. Simpson, J. Thieser, R. Tillmann, R. Varma, D. S. Venables, and A. Wahner
Atmos. Meas. Tech., 6, 1111–1140, https://doi.org/10.5194/amt-6-1111-2013, https://doi.org/10.5194/amt-6-1111-2013, 2013
R. A. Washenfelder, J. M. Flores, C. A. Brock, S. S. Brown, and Y. Rudich
Atmos. Meas. Tech., 6, 861–877, https://doi.org/10.5194/amt-6-861-2013, https://doi.org/10.5194/amt-6-861-2013, 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
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.
Audrey Gaudel, Ilann Bourgeois, Meng Li, Kai-Lan Chang, Jerald Ziemke, Bastien Sauvage, Ryan M. Stauffer, Anne M. Thompson, Debra E. Kollonige, Nadia Smith, Daan Hubert, Arno Keppens, Juan Cuesta, Klaus-Peter Heue, Pepijn Veefkind, Kenneth Aikin, Jeff Peischl, Chelsea R. Thompson, Thomas B. Ryerson, Gregory J. Frost, Brian C. McDonald, and Owen R. Cooper
Atmos. Chem. Phys., 24, 9975–10000, https://doi.org/10.5194/acp-24-9975-2024, https://doi.org/10.5194/acp-24-9975-2024, 2024
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The study examines tropical tropospheric ozone changes. In situ data from 1994–2019 display increased ozone, notably over India, Southeast Asia, and Malaysia and Indonesia. Sparse in situ data limit trend detection for the 15-year period. In situ and satellite data, with limited sampling, struggle to consistently detect trends. Continuous observations are vital over the tropical Pacific Ocean, Indian Ocean, western Africa, and South Asia for accurate ozone trend estimation in these regions.
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
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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.
Olivia G. Norman, Colette L. Heald, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
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.
Andrea E. Gordon, Cameron R. Homeyer, Jessica B. Smith, Rei Ueyama, Jonathan M. Dean-Day, Elliot L. Atlas, Kate Smith, Jasna V. Pittman, David S. Sayres, David M. Wilmouth, Apoorva Pandey, Jason M. St. Clair, Thomas F. Hanisco, Jennifer Hare, Reem A. Hannun, Steven Wofsy, Bruce C. Daube, and Stephen Donnelly
Atmos. Chem. Phys., 24, 7591–7608, https://doi.org/10.5194/acp-24-7591-2024, https://doi.org/10.5194/acp-24-7591-2024, 2024
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In situ airborne observations of ongoing tropopause-overshooting convection and an above-anvil cirrus plume from the 31 May 2022 flight of the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are examined. Upper troposphere and lower stratosphere composition changes are evaluated along with possible contributing dynamical and physical processes. Measurements reveal multiple changes in air mass composition and stratospheric hydration throughout the flight.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
EGUsphere, https://doi.org/10.5194/egusphere-2024-1399, https://doi.org/10.5194/egusphere-2024-1399, 2024
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol, and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
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.
Kouji Adachi, Jack E. Dibb, Joseph M. Katich, Joshua P. Schwarz, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Jeff Peischl, Christopher D. Holmes, and James Crawford
EGUsphere, https://doi.org/10.5194/egusphere-2024-880, https://doi.org/10.5194/egusphere-2024-880, 2024
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We examined aerosol particles from wildfires and identified tarballs (TBs) during the FIREX-AQ campaign. This study revealed the compositions, abundance, sizes, and mixing states of TBs and showed that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass burning and ages and enhances the knowledge of TB emissions and our understanding of their climate impact.
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.
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.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn Chipperfield, Wuhu Feng, David Oram, Karina Adcock, Stephen Montzka, Isobel Simpson, Andrea Mazzeo, Amber Leeson, Elliot Atlas, and Charles C.-K. Chou
EGUsphere, https://doi.org/10.5194/egusphere-2024-560, https://doi.org/10.5194/egusphere-2024-560, 2024
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Ethylene dichloride (EDC) is an industrial chemical used to produce polyvinyl chloride (PVC). We analysed EDC production data to estimate global EDC emissions (2002 to 2020). The emissions were included in an atmospheric model and evaluated by comparing simulated EDC to EDC measurements in the troposphere. We show EDC contributes ozone-depleting chlorine to the stratosphere and this has increased with increasing EDC emissions. EDC’s impact on stratospheric ozone is currently small, but non-zero.
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.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
Atmos. Chem. Phys., 23, 15643–15654, https://doi.org/10.5194/acp-23-15643-2023, https://doi.org/10.5194/acp-23-15643-2023, 2023
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We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
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.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Alia L. Khan, Peng Xian, and Joshua P. Schwarz
The Cryosphere, 17, 2909–2918, https://doi.org/10.5194/tc-17-2909-2023, https://doi.org/10.5194/tc-17-2909-2023, 2023
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Ice–albedo feedbacks in the ablation region of the Greenland Ice Sheet are difficult to constrain and model. Surface samples were collected across the 2014 summer melt season from different ice surface colors. On average, concentrations were higher in patches that were visibly dark, compared to medium patches and light patches, suggesting that black carbon aggregation contributed to snow aging, and vice versa. High concentrations are likely due to smoke transport from high-latitude wildfires.
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.
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.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
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.
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.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
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.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Caroline C. Womack, Steven S. Brown, Steven J. Ciciora, Ru-Shan Gao, Richard J. McLaughlin, Michael A. Robinson, Yinon Rudich, and Rebecca A. Washenfelder
Atmos. Meas. Tech., 15, 6643–6652, https://doi.org/10.5194/amt-15-6643-2022, https://doi.org/10.5194/amt-15-6643-2022, 2022
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We present a new miniature instrument to measure nitrogen dioxide (NO2) using cavity-enhanced spectroscopy. NO2 contributes to the formation of pollutants such as ozone and particulate matter, and its concentration can vary widely near sources. We developed this lightweight (3.05 kg) low-power (<35 W) instrument to measure NO2 on uncrewed aircraft vehicles (UAVs) and demonstrate that it has the accuracy and precision needed for atmospheric field measurements.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
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.
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.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219, https://doi.org/10.5194/acp-22-10195-2022, https://doi.org/10.5194/acp-22-10195-2022, 2022
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We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
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.
Eric A. Ray, Elliot L. Atlas, Sue Schauffler, Sofia Chelpon, Laura Pan, Harald Bönisch, and Karen H. Rosenlof
Atmos. Chem. Phys., 22, 6539–6558, https://doi.org/10.5194/acp-22-6539-2022, https://doi.org/10.5194/acp-22-6539-2022, 2022
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The movement of air masses and the trace gases they contain from the Earth’s surface into the upper troposphere and lower stratosphere (UTLS) can have important implications for the radiative and chemical balance of the atmosphere. In this study we build on recent techniques and use new ones to estimate a range of transport diagnostics based on simultaneously measured trace gases in the UTLS during the monsoon season in North America.
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.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
Adam T. Ahern, Frank Erdesz, Nicholas L. Wagner, Charles A. Brock, Ming Lyu, Kyra Slovacek, Richard H. Moore, Elizabeth B. Wiggins, and Daniel M. Murphy
Atmos. Meas. Tech., 15, 1093–1105, https://doi.org/10.5194/amt-15-1093-2022, https://doi.org/10.5194/amt-15-1093-2022, 2022
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Particles in the atmosphere play a significant role in climate change by scattering light back into space, reducing the amount of energy available to be absorbed by greenhouse gases. We built a new instrument to measure what direction light is scattered by particles, e.g., wildfire smoke. This is important because, depending on the angle of the sun, some particles scatter light into space (cooling the planet), but some light is also scattered towards the Earth (not cooling the planet).
Yanan Zhao, Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Astrid Bracher, Elliot L. Atlas, Jonathan Williams, and Hermann W. Bange
Biogeosciences, 19, 701–714, https://doi.org/10.5194/bg-19-701-2022, https://doi.org/10.5194/bg-19-701-2022, 2022
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We present here, for the first time, simultaneously measured dimethylsulfide (DMS) seawater concentrations and DMS atmospheric mole fractions from the Peruvian upwelling region during two cruises in December 2012 and October 2015. Our results indicate low oceanic DMS concentrations and atmospheric DMS molar fractions in surface waters and the atmosphere, respectively. In addition, the Peruvian upwelling region was identified as an insignificant source of DMS emissions during both periods.
Andrew O. Langford, Christoph J. Senff, Raul J. Alvarez II, Ken C. Aikin, Sunil Baidar, Timothy A. Bonin, W. Alan Brewer, Jerome Brioude, Steven S. Brown, Joel D. Burley, Dani J. Caputi, Stephen A. Conley, Patrick D. Cullis, Zachary C. J. Decker, Stéphanie Evan, Guillaume Kirgis, Meiyun Lin, Mariusz Pagowski, Jeff Peischl, Irina Petropavlovskikh, R. Bradley Pierce, Thomas B. Ryerson, Scott P. Sandberg, Chance W. Sterling, Ann M. Weickmann, and Li Zhang
Atmos. Chem. Phys., 22, 1707–1737, https://doi.org/10.5194/acp-22-1707-2022, https://doi.org/10.5194/acp-22-1707-2022, 2022
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The Fires, Asian, and Stratospheric Transport–Las Vegas Ozone Study (FAST-LVOS) combined lidar, aircraft, and in situ measurements with global models to investigate the contributions of stratospheric intrusions, regional and Asian pollution, and wildfires to background ozone in the southwestern US during May and June 2017 and demonstrated that these processes contributed to background ozone levels that exceeded 70 % of the US National Ambient Air Quality Standard during the 6-week campaign.
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.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
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.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Quanfu He, Zheng Fang, Ofir Shoshanim, Steven S. Brown, and Yinon Rudich
Atmos. Chem. Phys., 21, 14927–14940, https://doi.org/10.5194/acp-21-14927-2021, https://doi.org/10.5194/acp-21-14927-2021, 2021
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Rayleigh scattering and absorption cross sections for CO2, N2O, SF6, O2, and CH4 were measured between 307 and 725 nm. New dispersion relations for N2O, SF6, and CH4 in the UV–vis range were derived. This study provides refractive index dispersion relations, scattering, and absorption cross sections which are highly needed for accurate instrument calibration and for improved accuracy of Rayleigh scattering parameterizations for major greenhouse gases in Earth's atmosphere.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Linghan Zeng, Amy P. Sullivan, Rebecca A. Washenfelder, Jack Dibb, Eric Scheuer, Teresa L. Campos, Joseph M. Katich, Ezra Levin, Michael A. Robinson, and Rodney J. Weber
Atmos. Meas. Tech., 14, 6357–6378, https://doi.org/10.5194/amt-14-6357-2021, https://doi.org/10.5194/amt-14-6357-2021, 2021
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Three online systems for measuring water-soluble brown carbon are compared. A mist chamber and two different particle-into-liquid samplers were deployed on separate research aircraft targeting wildfires and followed a similar detection method using a long-path liquid waveguide with a spectrometer to measure the light absorption from 300 to 700 nm. Detection limits, signal hysteresis and other sampling issues are compared, and further improvements of these liquid-based systems are provided.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
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.
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.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Marco Zanatta, Andreas Herber, Zsófia Jurányi, Oliver Eppers, Johannes Schneider, and Joshua P. Schwarz
Atmos. Chem. Phys., 21, 9329–9342, https://doi.org/10.5194/acp-21-9329-2021, https://doi.org/10.5194/acp-21-9329-2021, 2021
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Saline snow samples were collected from the sea ice in the Fram Strait. Laboratory experiments revealed that sea salt can bias the quantification of black carbon with a laser-induced incandescence technique. The maximum underestimation was quantified to reach values of 80 %–90 %. This salt-induced interference is reported here for the first time and should be considered in future studies aiming to quantify black carbon in snow in marine environments.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Caroline C. Womack, Katherine M. Manfred, Nicholas L. Wagner, Gabriela Adler, Alessandro Franchin, Kara D. Lamb, Ann M. Middlebrook, Joshua P. Schwarz, Charles A. Brock, Steven S. Brown, and Rebecca A. Washenfelder
Atmos. Chem. Phys., 21, 7235–7252, https://doi.org/10.5194/acp-21-7235-2021, https://doi.org/10.5194/acp-21-7235-2021, 2021
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Microscopic particles interact with sunlight and affect the earth's climate in ways that are not fully understood. Aerosols from wildfire smoke present particular challenges due to their complexity in shape and composition. We demonstrate that we can experimentally measure aerosol optical properties for many types of smoke particles, using measurements of smoke from controlled burns, but that the method does not work well for smoke with high soot content.
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.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
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.
Reem A. Hannun, Andrew K. Swanson, Steven A. Bailey, Thomas F. Hanisco, T. Paul Bui, Ilann Bourgeois, Jeff Peischl, and Thomas B. Ryerson
Atmos. Meas. Tech., 13, 6877–6887, https://doi.org/10.5194/amt-13-6877-2020, https://doi.org/10.5194/amt-13-6877-2020, 2020
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We have developed a cavity-enhanced absorption instrument to measure ozone in the atmosphere. The detection technique enables highly sensitive measurements in fast averaging times. The compact, robust instrument is suitable for operation in varied field environments, including aboard research aircraft. We have successfully flown the instrument and demonstrated its performance capabilities with measurements of ozone deposition rates over the coastal Pacific Ocean.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
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Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
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.
Wayne M. Angevine, Jeff Peischl, Alice Crawford, Christopher P. Loughner, Ilana B. Pollack, and Chelsea R. Thompson
Atmos. Chem. Phys., 20, 11855–11868, https://doi.org/10.5194/acp-20-11855-2020, https://doi.org/10.5194/acp-20-11855-2020, 2020
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Emissions of air pollutants must be known for a wide variety of applications. Different methods of estimating emissions often disagree substantially. In this study, we apply standard methods to a well-known source, a power plant. We explore the uncertainty implied by the different answers that come from the different methods, different samples taken over several years, and different pollutants. We find that the overall uncertainty of emissions estimates is about 30 %.
Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Kenneth C. Aikin, Teresa Campos, Hannah Clark, Róisín Commane, Bruce Daube, Glenn W. Diskin, James W. Elkins, Ru-Shan Gao, Audrey Gaudel, Eric J. Hintsa, Bryan J. Johnson, Rigel Kivi, Kathryn McKain, Fred L. Moore, David D. Parrish, Richard Querel, Eric Ray, Ricardo Sánchez, Colm Sweeney, David W. Tarasick, Anne M. Thompson, Valérie Thouret, Jacquelyn C. Witte, Steve C. Wofsy, and Thomas B. Ryerson
Atmos. Chem. Phys., 20, 10611–10635, https://doi.org/10.5194/acp-20-10611-2020, https://doi.org/10.5194/acp-20-10611-2020, 2020
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
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.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Susann Tegtmeier, Elliot Atlas, Birgit Quack, Franziska Ziska, and Kirstin Krüger
Atmos. Chem. Phys., 20, 7103–7123, https://doi.org/10.5194/acp-20-7103-2020, https://doi.org/10.5194/acp-20-7103-2020, 2020
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We investigate emissions of brominated gases from the ocean and their contribution to stratospheric ozone depletion. Once in the atmosphere, these gases usually break down in less than 6 months. Their impact on the ozone layer depends on the prevailing atmospheric circulation, since transport to the stratosphere requires uplift. We combine aircraft and ship observations with atmospheric modelling to analyse how, where, and when these gases are transported from the ocean into the stratosphere.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Andrew W. Rollins, Pamela S. Rickly, Ru-Shan Gao, Thomas B. Ryerson, Steven S. Brown, Jeff Peischl, and Ilann Bourgeois
Atmos. Meas. Tech., 13, 2425–2439, https://doi.org/10.5194/amt-13-2425-2020, https://doi.org/10.5194/amt-13-2425-2020, 2020
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Nitric oxide (NO) is a key atmospheric constituent controlling atmospheric oxidation chemistry and tropospheric ozone formation. Existing instrumentation capable of quantifying NO at very low mixing ratios is uncommon and typically relies on chemiluminescence. We describe and demonstrate a new laser-based technique (LIF) with significant practical and technical advantages to CL. This technique is expected to allow for advances in understanding of atmospheric radical chemistry.
Sophia Brilke, Nikolaus Fölker, Thomas Müller, Konrad Kandler, Xianda Gong, Jeff Peischl, Bernadett Weinzierl, and Paul M. Winkler
Atmos. Chem. Phys., 20, 5645–5656, https://doi.org/10.5194/acp-20-5645-2020, https://doi.org/10.5194/acp-20-5645-2020, 2020
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Atmospheric particle size distributions with the focus on freshly nucleated particles were measured during the A-LIFE field experiment in Cyprus. A DMA-train was set up for the first time in an atmospheric environment and captures the sub-10 nm particle dynamics. Several new particle formation (NPF) events are studied in detail, of which some did not show particle growth beyond 10 nm indicating that NPF may occur more frequently than estimated when the sub-10 nm size range is not covered.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Chuan Yu, Zhe Wang, Men Xia, Xiao Fu, Weihao Wang, Yee Jun Tham, Tianshu Chen, Penggang Zheng, Hongyong Li, Ye Shan, Xinfeng Wang, Likun Xue, Yan Zhou, Dingli Yue, Yubo Ou, Jian Gao, Keding Lu, Steven S. Brown, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 20, 4367–4378, https://doi.org/10.5194/acp-20-4367-2020, https://doi.org/10.5194/acp-20-4367-2020, 2020
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This study provides a holistic picture of N2O5 heterogeneous uptake on ambient aerosols and the influencing factors under various climatic and chemical conditions in China, and it proposes an observation-based empirical parameterization. The empirical parameterization can be used in air quality models to improve the prediction of PM2.5 and photochemical pollution in China and similar polluted regions of the world.
Alexander B. Thames, William H. Brune, David O. Miller, Hannah M. Allen, Eric C. Apel, Donald R. Blake, T. Paul Bui, Roisin Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, Joshua P. DiGangi, James W. Elkins, Samuel R. Hall, Thomas F. Hanisco, Reem A. Hannun, Eric Hintsa, Rebecca S. Hornbrook, Michelle J. Kim, Kathryn McKain, Fred L. Moore, Julie M. Nicely, Jeffrey Peischl, Thomas B. Ryerson, Jason M. St. Clair, Colm Sweeney, Alex Teng, Chelsea R. Thompson, Kirk Ullmann, Paul O. Wennberg, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 4013–4029, https://doi.org/10.5194/acp-20-4013-2020, https://doi.org/10.5194/acp-20-4013-2020, 2020
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Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Meinrat O. Andreae, Kazushi Aranami, Elliot Atlas, Max Berkelhammer, Heinz Bingemer, Dennis Booge, Gregory Cutter, Pau Cortes, Stefanie Kremser, Cliff S. Law, Andrew Marriner, Rafel Simó, Birgit Quack, Günther Uher, Huixiang Xie, and Xiaobin Xu
Earth Syst. Sci. Data, 12, 591–609, https://doi.org/10.5194/essd-12-591-2020, https://doi.org/10.5194/essd-12-591-2020, 2020
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Sulfur-containing trace gases in the atmosphere influence atmospheric chemistry and the energy budget of the Earth by forming aerosols. The ocean is an important source of the most abundant sulfur gas in the atmosphere, carbonyl sulfide (OCS) and its most important precursor carbon disulfide (CS2). In order to assess global variability of the sea surface concentrations of both gases to calculate their oceanic emissions, we have compiled a database of existing shipborne measurements.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Alexander Moravek, Jennifer G. Murphy, Amy Hrdina, John C. Lin, Christopher Pennell, Alessandro Franchin, Ann M. Middlebrook, Dorothy L. Fibiger, Caroline C. Womack, Erin E. McDuffie, Randal Martin, Kori Moore, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 15691–15709, https://doi.org/10.5194/acp-19-15691-2019, https://doi.org/10.5194/acp-19-15691-2019, 2019
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Ammonium nitrate is a major component of fine particulate matter of wintertime air pollution in the Great Salt Lake Region (UT, USA). We investigate the sources of ammonia in the region by using aircraft observations and comparing them to modelled ammonia mixing ratios based on emission inventory estimates. The results suggest that ammonia emissions are underestimated, specifically in regions with high agricultural activity, while ammonia in Salt Lake City is mainly of local origin.
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.
Karl D. Froyd, Daniel M. Murphy, Charles A. Brock, Pedro Campuzano-Jost, Jack E. Dibb, Jose-Luis Jimenez, Agnieszka Kupc, Ann M. Middlebrook, Gregory P. Schill, Kenneth L. Thornhill, Christina J. Williamson, James C. Wilson, and Luke D. Ziemba
Atmos. Meas. Tech., 12, 6209–6239, https://doi.org/10.5194/amt-12-6209-2019, https://doi.org/10.5194/amt-12-6209-2019, 2019
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Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with a fast time response applicable to aircraft sampling.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
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.
David D. Parrish and Christine A. Ennis
Atmos. Chem. Phys., 19, 12587–12605, https://doi.org/10.5194/acp-19-12587-2019, https://doi.org/10.5194/acp-19-12587-2019, 2019
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Background ozone transported into cities contributes greatly to urban concentrations. Based on projections of past trends, the largest ozone concentrations on which the 70 ppb National Ambient Air Quality Standard is based will reach that standard by ∼ 2021 in the New York City area but much later (∼ 2050) in the Los Angeles region. The much smaller background contribution in New York City (45.8 ± 1.7 ppb) than in Los Angeles (62.0 ± 2.0 ppb) is the primary reason for this large difference.
Yue Jia, Susann Tegtmeier, Elliot Atlas, and Birgit Quack
Atmos. Chem. Phys., 19, 11089–11103, https://doi.org/10.5194/acp-19-11089-2019, https://doi.org/10.5194/acp-19-11089-2019, 2019
Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 9287–9308, https://doi.org/10.5194/acp-19-9287-2019, https://doi.org/10.5194/acp-19-9287-2019, 2019
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Populated mountain basins, including the Salt Lake Valley (SLV) in Utah, suffer from wintertime stagnation events that trap emissions near the surface and cause fine particulate matter (PM2.5) concentrations to reach unhealthy levels. Previously limited by a lack of nighttime measurements, this study uses 2017 UWFPS aircraft campaign data, in combination with a box model, to show that nitrogen chemistry above the surface at night is a major source of PM2.5 during a wintertime event in the SLV.
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.
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.
Charles A. Brock, Christina Williamson, Agnieszka Kupc, Karl D. Froyd, Frank Erdesz, Nicholas Wagner, Matthews Richardson, Joshua P. Schwarz, Ru-Shan Gao, Joseph M. Katich, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, Bernadett Weinzierl, Maximilian Dollner, ThaoPaul Bui, and Daniel M. Murphy
Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, https://doi.org/10.5194/amt-12-3081-2019, 2019
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From 2016 to 2018 a NASA aircraft profiled the atmosphere from 180 m to ~12 km from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, ATom, sought to sample atmospheric chemical composition to compare with global climate models. We describe the how measurements of particulate matter were made during ATom, and show that the instrument performance was excellent. Data from this project can be used with confidence to evaluate models and compare with satellites.
Daniel M. Murphy, Karl D. Froyd, Huisheng Bian, Charles A. Brock, Jack E. Dibb, Joshua P. DiGangi, Glenn Diskin, Maximillian Dollner, Agnieszka Kupc, Eric M. Scheuer, Gregory P. Schill, Bernadett Weinzierl, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 19, 4093–4104, https://doi.org/10.5194/acp-19-4093-2019, https://doi.org/10.5194/acp-19-4093-2019, 2019
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We present the first data on the concentration of sea-salt aerosol throughout most of the depth of the troposphere and a wide range of latitudes. Sea-salt concentrations in the upper troposphere are very small. This puts stringent limits on how sea-salt aerosol affects halogen and nitric acid chemistry there. With a widely distributed source, sea-salt aerosol provides an excellent test of wet scavenging and vertical transport of aerosols in chemical transport models.
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.
Nick Jordan, Connie Z. Ye, Satyaki Ghosh, Rebecca A. Washenfelder, Steven S. Brown, and Hans D. Osthoff
Atmos. Meas. Tech., 12, 1277–1293, https://doi.org/10.5194/amt-12-1277-2019, https://doi.org/10.5194/amt-12-1277-2019, 2019
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A new spectrometer to measure abundances of the atmospheric trace gases nitrogen dioxide and iodine is described. The spectrometer uses a light-emitting diode between 470 and 540 nm and two highly reflective mirrors to yield an effective absorption path of 6.3 km. We remeasured scattering cross sections of common atmospheric gases in the cyan region and present sample NO2 measurements that agreed with those made with a laser-based instrument.
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.
J. Christopher Kaiser, Johannes Hendricks, Mattia Righi, Patrick Jöckel, Holger Tost, Konrad Kandler, Bernadett Weinzierl, Daniel Sauer, Katharina Heimerl, Joshua P. Schwarz, Anne E. Perring, and Thomas Popp
Geosci. Model Dev., 12, 541–579, https://doi.org/10.5194/gmd-12-541-2019, https://doi.org/10.5194/gmd-12-541-2019, 2019
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The implementation of the aerosol microphysics submodel MADE3 into the global atmospheric chemistry model EMAC is described and evaluated against an extensive pool of observational data, focusing on aerosol mass and number concentrations, size distributions, composition, and optical properties. EMAC (MADE3) is able to reproduce main aerosol properties reasonably well, in line with the performance of other global aerosol models.
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.
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
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We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
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 %.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
James M. Mattila, Patrick Brophy, Jeffrey Kirkland, Samuel Hall, Kirk Ullmann, Emily V. Fischer, Steve Brown, Erin McDuffie, Alex Tevlin, and Delphine K. Farmer
Atmos. Chem. Phys., 18, 12315–12327, https://doi.org/10.5194/acp-18-12315-2018, https://doi.org/10.5194/acp-18-12315-2018, 2018
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Molecular acids in the atmosphere have implications for human health and air quality. Measurements of various acidic molecules were performed in the Colorado Front Range. Atmospheric concentrations of many acids increased during the day, indicative of sunlight-related production sources. A surface-level source of many acids persisting throughout day and night was observed. Traffic and agricultural activity were important anthropogenic sources of several acids near the measurement site.
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.
Christina Williamson, Agnieszka Kupc, James Wilson, David W. Gesler, J. Michael Reeves, Frank Erdesz, Richard McLaughlin, and Charles A. Brock
Atmos. Meas. Tech., 11, 3491–3509, https://doi.org/10.5194/amt-11-3491-2018, https://doi.org/10.5194/amt-11-3491-2018, 2018
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We describe the operating principle, design and performance of the Nucleation Mode Aerosol Size Spectrometer (NMASS), an instrument composed of 5 condensation particle counters measuring size selected particle concentrations between 3 and 60 nm. An inversion to recover size distributions from the data is evaluated. Calibrations of a 2-NMASS system for measuring size distributions on the NASA Atmospheric Tomography Mission, and examples of its in-flight performance are presented.
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.
Richard Newton, Geraint Vaughan, Eric Hintsa, Michal T. Filus, Laura L. Pan, Shawn Honomichl, Elliot Atlas, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 18, 5157–5171, https://doi.org/10.5194/acp-18-5157-2018, https://doi.org/10.5194/acp-18-5157-2018, 2018
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We consider the ozone measurements from aircraft during the CAST/CONTRAST/ATTREX campaigns of 2014. Low concentrations of ozone were found in the layer of 10–15 km altitude, which is indicative of uplift of ozone-poor air from near the sea surface to 10–15 km altitude. Chemicals that have origins in the sea were found in greater abundance when ozone concentrations were low compared to when ozone concentrations were high. The lowest ozone concentrations were found in the Southern Hemisphere.
James D. Lee, Stephen D. Mobbs, Axel Wellpott, Grant Allen, Stephane J.-B. Bauguitte, Ralph R. Burton, Richard Camilli, Hugh Coe, Rebecca E. Fisher, James L. France, Martin Gallagher, James R. Hopkins, Mathias Lanoiselle, Alastair C. Lewis, David Lowry, Euan G. Nisbet, Ruth M. Purvis, Sebastian O'Shea, John A. Pyle, and Thomas B. Ryerson
Atmos. Meas. Tech., 11, 1725–1739, https://doi.org/10.5194/amt-11-1725-2018, https://doi.org/10.5194/amt-11-1725-2018, 2018
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This work describes measurements, made from an aircraft platform, of the emission of methane and other organic gases from an uncontrolled leak from an oil platform in the North Sea (Total Elgin). The measurements made helped the platform operators to devise a strategy for repairing the leak and serve as a methodology for assessing future similar incidents.
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.
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.
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.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Agnieszka Kupc, Christina Williamson, Nicholas L. Wagner, Mathews Richardson, and Charles A. Brock
Atmos. Meas. Tech., 11, 369–383, https://doi.org/10.5194/amt-11-369-2018, https://doi.org/10.5194/amt-11-369-2018, 2018
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
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.
Lihua Wang, Michael J. Newchurch, Raul J. Alvarez II, Timothy A. Berkoff, Steven S. Brown, William Carrion, Russell J. De Young, Bryan J. Johnson, Rene Ganoe, Guillaume Gronoff, Guillaume Kirgis, Shi Kuang, Andrew O. Langford, Thierry Leblanc, Erin E. McDuffie, Thomas J. McGee, Denis Pliutau, Christoph J. Senff, John T. Sullivan, Grant Sumnicht, Laurence W. Twigg, and Andrew J. Weinheimer
Atmos. Meas. Tech., 10, 3865–3876, https://doi.org/10.5194/amt-10-3865-2017, https://doi.org/10.5194/amt-10-3865-2017, 2017
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Intercomparisons have been made between three TOLNet ozone lidars and between the lidars and other ozone instruments during the 2014 DISCOVER-AQ and FRAPPÉ campaigns in Colorado. Overall, the TOLNet lidars are capable of measuring 5 min tropospheric ozone variations with accuracy better than ±15 % in terms of their vertical resolving capability and better than ±5 % in terms of their column average measurement. These results indicate very good measurement accuracy for the three TOLNet lidars.
Jin Liao, Charles A. Brock, Daniel M. Murphy, Donna T. Sueper, André Welti, and Ann M. Middlebrook
Atmos. Meas. Tech., 10, 3801–3820, https://doi.org/10.5194/amt-10-3801-2017, https://doi.org/10.5194/amt-10-3801-2017, 2017
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The Aerodyne aerosol mass spectrometer (AMS) has emerged as a widely used method for measuring the real-time, submicron, nonrefractory aerosol composition. A large uncertainty in accurate measurements with the AMS (the collection efficiency due to particle bounce) is evaluated in this paper using in situ measurements of particle light scattering. Current calculations of the collection efficiency reasonably predict this effect in acidic environments, resulting in more confidence for AMS results.
Bianca C. Baier, William H. Brune, David O. Miller, Donald Blake, Russell Long, Armin Wisthaler, Christopher Cantrell, Alan Fried, Brian Heikes, Steven Brown, Erin McDuffie, Frank Flocke, Eric Apel, Lisa Kaser, and Andrew Weinheimer
Atmos. Chem. Phys., 17, 11273–11292, https://doi.org/10.5194/acp-17-11273-2017, https://doi.org/10.5194/acp-17-11273-2017, 2017
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Ozone production rates were measured using the Measurement of Ozone Production Sensor (MOPS). Measurements are compared to modeled ozone production rates using two different chemical mechanisms. At high nitric oxide levels, observed rates are higher than those modeled, prompting the need to revisit current model photochemistry. These direct measurements can add to our understanding of the ozone chemistry within air quality models and can be used to guide government regulatory strategies.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
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.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Alina Fiehn, Birgit Quack, Helmke Hepach, Steffen Fuhlbrügge, Susann Tegtmeier, Matthew Toohey, Elliot Atlas, and Kirstin Krüger
Atmos. Chem. Phys., 17, 6723–6741, https://doi.org/10.5194/acp-17-6723-2017, https://doi.org/10.5194/acp-17-6723-2017, 2017
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Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. In the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise in the west Indian Ocean, we found an important source region of halogenated VSLSs during the Asian summer monsoon. Modeling the transport from the ocean to the stratosphere we found two main pathways, one over the Indian Ocean and one over northern India.
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.
Ellis Shipley Robinson, Ru-Shan Gao, Joshua P. Schwarz, David W. Fahey, and Anne E. Perring
Atmos. Meas. Tech., 10, 1755–1768, https://doi.org/10.5194/amt-10-1755-2017, https://doi.org/10.5194/amt-10-1755-2017, 2017
Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Amber M. Ortega, Juliane L. Fry, Steven S. Brown, Kyle J. Zarzana, William Dube, Nicholas L. Wagner, Danielle C. Draper, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5331–5354, https://doi.org/10.5194/acp-17-5331-2017, https://doi.org/10.5194/acp-17-5331-2017, 2017
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Ambient forest air was oxidized by OH, O3, or NO3 inside an oxidation flow reactor, leading to formation of particulate matter from any gaseous precursors found in the air. Closure was achieved between the amount of particulate mass formed from O3 and NO3 oxidation and the amount predicted from speciated gaseous precursors, which was in contrast to previous results for OH oxidation (Palm et al., 2016). Elemental analysis of the particulate mass formed in the reactor is presented.
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.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
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.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Hendrik Fuchs, Zhaofeng Tan, Keding Lu, Birger Bohn, Sebastian Broch, Steven S. Brown, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Kyung-Eun Min, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinson Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 645–661, https://doi.org/10.5194/acp-17-645-2017, https://doi.org/10.5194/acp-17-645-2017, 2017
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OH reactivity was measured during a 1-month long campaign at a rural site in the North China Plain in 2014. OH reactivity measurements are compared to calculations using OH reactant measurements. Good agreement is found indicating that all important OH reactants were measured. In addition, the chemical OH budget is analyzed. In contrast to previous campaigns in China in 2006, no significant imbalance between OH production and destruction is found.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliot Atlas, and Kirstin Krüger
Atmos. Chem. Phys., 17, 385–402, https://doi.org/10.5194/acp-17-385-2017, https://doi.org/10.5194/acp-17-385-2017, 2017
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We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577, https://doi.org/10.5194/acp-16-13561-2016, https://doi.org/10.5194/acp-16-13561-2016, 2016
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Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
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
Stephen J. Andrews, Lucy J. Carpenter, Eric C. Apel, Elliot Atlas, Valeria Donets, James R. Hopkins, Rebecca S. Hornbrook, Alastair C. Lewis, Richard T. Lidster, Richard Lueb, Jamie Minaeian, Maria Navarro, Shalini Punjabi, Daniel Riemer, and Sue Schauffler
Atmos. Meas. Tech., 9, 5213–5225, https://doi.org/10.5194/amt-9-5213-2016, https://doi.org/10.5194/amt-9-5213-2016, 2016
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We present a comparison of aircraft measurements of important trace gases from a co-ordinated campaign in Jan–Feb 2014 in the tropical west Pacific involving the NASA Global Hawk, NCAR GV and FAAM BAe-146 aircraft.
The paper studies the comparability of separate measurements across platforms and demonstrates that aircraft measurements are relevant for characterising the vertical uplift of important gases, such as those with ozone-depleting potential, to the upper troposphere–lower stratosphere.
Steffen Fuhlbrügge, Birgit Quack, Elliot Atlas, Alina Fiehn, Helmke Hepach, and Kirstin Krüger
Atmos. Chem. Phys., 16, 12205–12217, https://doi.org/10.5194/acp-16-12205-2016, https://doi.org/10.5194/acp-16-12205-2016, 2016
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This study presents novel observations of the very short lived substances (VSLSs) bromoform, dibromomethane and methyl iodide with high-resolution meteorological measurements and Lagrangian transport in the Peruvian upwelling. With a simple source–loss estimate we identified VSLS abundances below the trade inversion to be significantly influenced by advection of regional sources, underscoring the importance of oceanic upwelling and trade winds on the atmospheric distribution of VSLS emission.
Helmke Hepach, Birgit Quack, Susann Tegtmeier, Anja Engel, Astrid Bracher, Steffen Fuhlbrügge, Luisa Galgani, Elliot L. Atlas, Johannes Lampel, Udo Frieß, and Kirstin Krüger
Atmos. Chem. Phys., 16, 12219–12237, https://doi.org/10.5194/acp-16-12219-2016, https://doi.org/10.5194/acp-16-12219-2016, 2016
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We present surface seawater measurements of bromo- and iodocarbons, which are involved in numerous atmospheric processes such as tropospheric and stratospheric ozone chemistry, from the highly productive Peruvian upwelling. By combining trace gas measurements, characterization of organic matter and phytoplankton species, and tropospheric modelling, we show that large amounts of iodocarbons produced from the pool of organic matter may contribute strongly to local tropospheric iodine loading.
Kennedy T. Vu, Justin H. Dingle, Roya Bahreini, Patrick J. Reddy, Eric C. Apel, Teresa L. Campos, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Scott C. Herndon, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Denise D. Montzka, John B. Nowak, Sally E. Pusede, Dirk Richter, Joseph R. Roscioli, Glen W. Sachse, Stephen Shertz, Meghan Stell, David Tanner, Geoffrey S. Tyndall, James Walega, Peter Weibring, Andrew J. Weinheimer, Gabriele Pfister, and Frank Flocke
Atmos. Chem. Phys., 16, 12039–12058, https://doi.org/10.5194/acp-16-12039-2016, https://doi.org/10.5194/acp-16-12039-2016, 2016
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In this manuscript, we report on airborne measurements of non-refractory composition and optical extinction along with relevant trace gases during a unique surface mesoscale circulation event, namely the Denver Cyclone, in Colorado, USA, during in July–August 2014. The focus of this paper is to investigate how meteorological conditions associated with the Denver Cyclone impacted air quality of the Colorado Front Range.
Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Paul I. Palmer, Michael Schlundt, Elliot L. Atlas, Astrid Bracher, Eric S. Saltzman, and Douglas W. R. Wallace
Atmos. Chem. Phys., 16, 11807–11821, https://doi.org/10.5194/acp-16-11807-2016, https://doi.org/10.5194/acp-16-11807-2016, 2016
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Isoprene, a biogenic trace gas, is an important precursor of secondary organic aerosol/cloud condensation nuclei. Here, we use isoprene and related field measurements from three different ocean data sets together with remotely sensed satellite data to model global marine isoprene emissions. Our findings suggest that there is at least one missing oceanic source of isoprene and possibly other unknown factors in the ocean or atmosphere influencing the atmospheric values.
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.
Justin H. Dingle, Kennedy Vu, Roya Bahreini, Eric C. Apel, Teresa L. Campos, Frank Flocke, Alan Fried, Scott Herndon, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Denise D. Montzka, John B. Nowak, Mike Reeves, Dirk Richter, Joseph R. Roscioli, Stephen Shertz, Meghan Stell, David Tanner, Geoff Tyndall, James Walega, Petter Weibring, and Andrew Weinheimer
Atmos. Chem. Phys., 16, 11207–11217, https://doi.org/10.5194/acp-16-11207-2016, https://doi.org/10.5194/acp-16-11207-2016, 2016
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The focus of this paper was to use gas-phase tracers and aerosol composition to characterize t