Articles | Volume 16, issue 21
Atmos. Chem. Phys., 16, 13561–13577, 2016
https://doi.org/10.5194/acp-16-13561-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 16, 13561–13577, 2016
https://doi.org/10.5194/acp-16-13561-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 01 Nov 2016
Research article | 01 Nov 2016
Why do models overestimate surface ozone in the Southeast United States?
Katherine R. Travis et al.
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Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
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.
Katherine R. Travis and Daniel J. Jacob
Geosci. Model Dev., 12, 3641–3648, https://doi.org/10.5194/gmd-12-3641-2019, https://doi.org/10.5194/gmd-12-3641-2019, 2019
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Models of ozone air pollution are often evaluated with the policy metric set by the EPA of the maximum daily 8 h average ozone concentration. These models may be used in policy settings to evaluate air quality regulations. However, most models have difficulty simulating how ozone varies over the course of the day, and thus the use of this metric in model evaluation is problematic. Improved representation of mixed layer dynamics and ozone loss to the surface is needed to resolve this issue.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
Preprint retracted
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
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.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Glenn M. Wolfe, Margaret R. Marvin, Sandra J. Roberts, Katherine R. Travis, and Jin Liao
Geosci. Model Dev., 9, 3309–3319, https://doi.org/10.5194/gmd-9-3309-2016, https://doi.org/10.5194/gmd-9-3309-2016, 2016
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The Framework for 0-D Atmospheric Modeling (F0AM) is a new, user-friendly platform for simulation of atmospheric chemistry systems. It incorporates a suite of commonly used mechanisms and is adaptable to photochemical chambers, Lagrangian plumes, and steady-state or time-varying diurnal cycles. We provide a detailed model description, demonstrate several common applications, and highlight some of the advantages and challenges of the 0-D box modeling approach.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
H.-M. Lee, F. Paulot, D. K. Henze, K. Travis, D. J. Jacob, L. H. Pardo, and B. A. Schichtel
Atmos. Chem. Phys., 16, 525–540, https://doi.org/10.5194/acp-16-525-2016, https://doi.org/10.5194/acp-16-525-2016, 2016
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Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated, identifying unique features in contributions from different species, sectors and locations. Ndep in many parks is impacted by emissions several hundred km away; the role of oxidized vs reduced sources varies regionally. Emissions reductions in the western US most effectively reduce the extent of areas in critical load exceedance, while reductions in the east most effectively reduce exceedance magnitudes.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
P. Zoogman, D. J. Jacob, K. Chance, X. Liu, M. Lin, A. Fiore, and K. Travis
Atmos. Chem. Phys., 14, 6261–6271, https://doi.org/10.5194/acp-14-6261-2014, https://doi.org/10.5194/acp-14-6261-2014, 2014
J. Mao, S. Fan, D. J. Jacob, and K. R. Travis
Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, https://doi.org/10.5194/acp-13-509-2013, 2013
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, and Deborah Gordon
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-911, https://doi.org/10.5194/acp-2021-911, 2021
Preprint under review for ACP
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then compare our spatially explicit inventory with atmospheric methane observations with the goal of identifying potential under- and over-estimates in the national inventories.
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. Discuss., https://doi.org/10.5194/acp-2021-929, https://doi.org/10.5194/acp-2021-929, 2021
Preprint under review for ACP
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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.
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.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
Drew C. Pendergrass, Daniel J. Jacob, Shixian Zhai, Jhoon Kim, Ja-Ho Koo, Seoyoung Lee, Minah Bae, and Soontae Kim
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-273, https://doi.org/10.5194/amt-2021-273, 2021
Preprint under review for AMT
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This paper uses a machine learning algorithm to infer high resolution maps of particulate air quality in eastern China, Japan, and the Korean peninsula using data from a geostationary satellite, along with meteorology. We then perform extensive evaluation of this inferred air quality and use it to diagnose trends in the region. We hope this paper and the associated data will be valuable to other scientists interested in epidemiology, air quality, remote sensing, and machine learning.
Xiaomeng Jin, Qindan Zhu, and Ronald C. Cohen
Atmos. Chem. Phys., 21, 15569–15587, https://doi.org/10.5194/acp-21-15569-2021, https://doi.org/10.5194/acp-21-15569-2021, 2021
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We describe direct estimates of NOx emissions and lifetimes for biomass burning plumes using daily TROPOMI retrievals of NO2. Satellite-derived NOx emission factors are consistent with those from in situ measurements. We observe decreasing NOx lifetime with fire intensity, which is due to the increase in NOx abundance and radical production. Our findings suggest promise for applying space-based observations to track the emissions and chemical evolution of reactive nitrogen from wildfires.
Martin Breitenlechner, Gordon A. Novak, J. Andrew Neuman, Andrew W. Rollins, and Patrick R. Veres
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-330, https://doi.org/10.5194/amt-2021-330, 2021
Preprint under review for AMT
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We coupled a new ion source to a commercially available state-of-the-art trace gas analyzer. The instrument is particularly well suited for conducting high altitude observations, addressing the challenges of low ambient pressures and a complex sample matrix. The new instrument and ion source provides significant advantages to more traditional modes of operation, without sacrificing the sensitivity and flexibility of this technique.
Tianlang Zhao, Jingqiu Mao, William R. Simpson, Isabelle De Smedt, Lei Zhu, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Gonzalo González Abad, Caroline R. Nowlan, Barbara Barletta, Simone Meinardi, and Donald R. Blake
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-820, https://doi.org/10.5194/acp-2021-820, 2021
Preprint under review for ACP
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Monitoring formaldehyde (HCHO) can help understanding Arctic vegetation change. Here we compared satellite data and model and show that Alaska summertime HCHO is largely dominated by background from methane oxidation during mild wildfire year and is dominated by wildfire (largely from direct emission of fire) during strong fire year. Consequently, it is challenging to use satellite HCHO to study vegetation change in the Arctic region.
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.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Helen Fitzmaurice, Alexander J. Turner, Jinsol Kim, Katherine Chan, Erin R. Delaria, Catherine Newman, Paul Wooldridge, and Ronald C. Cohen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-808, https://doi.org/10.5194/acp-2021-808, 2021
Preprint under review for ACP
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On-road emissions are thought to vary widely from existing predictions because the effects of age of the vehicle fleet, performance of emission control systems and variations in speed are difficult to assess under ambient driving conditions. We present an observational approach to characterize on-road emissions and show that the method is consistent with other approaches to within ~3 %.
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.
Zhen Qu, Daniel J. Jacob, Lu Shen, Xiao Lu, Yuzhong Zhang, Tia R. Scarpelli, Hannah Nesser, Melissa P. Sulprizio, Joannes D. Maasakkers, A. Anthony Bloom, John R. Worden, Robert J. Parker, and Alba L. Delgado
Atmos. Chem. Phys., 21, 14159–14175, https://doi.org/10.5194/acp-21-14159-2021, https://doi.org/10.5194/acp-21-14159-2021, 2021
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The recent launch of TROPOMI offers an unprecedented opportunity to quantify the methane budget from a top-down perspective. We use TROPOMI and the more mature GOSAT methane observations to estimate methane emissions and get consistent global budgets. However, TROPOMI shows biases over regions where surface albedo is small and provides less information for the coarse-resolution inversion due to the larger error correlations and spatial variations in the number of observations.
Lee T. Murray, Eric M. Leibensperger, Clara Orbe, Loretta J. Mickley, and Melissa Sulprizio
Geosci. Model Dev., 14, 5789–5823, https://doi.org/10.5194/gmd-14-5789-2021, https://doi.org/10.5194/gmd-14-5789-2021, 2021
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Chemical-transport models are tools used to study air pollution and inform public policy. However, they are limited by the availability of archived meteorology. Here, we describe how the GEOS-Chem chemical-transport model may now be driven by meteorology archived from a state-of-the-art general circulation model for past and future climates, allowing it to be used to explore the impact of climate change on air pollution and atmospheric composition.
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. Discuss., https://doi.org/10.5194/acp-2021-761, https://doi.org/10.5194/acp-2021-761, 2021
Preprint under review for ACP
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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 asseses how much aerosol optical properties can tell us about aerosol composition.
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 W. Weickmann, and Li Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-690, https://doi.org/10.5194/acp-2021-690, 2021
Preprint under review for ACP
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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 on background ozone in the Southwestern U.S. during May and June. The study demonstrated that these processes contributed to background ozone levels that exceeded 70% of the U.S. National Ambient Air Quality Standard during the 6-week campaign.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
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.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Douglas A. Day, Pedro Campuzano-Jost, Benjamin A. Nault, Brett B. Palm, Weiwei Hu, Hongyu Guo, Paul J. Wooldridge, Ronald C. Cohen, Kenneth S. Docherty, J. Alex Huffman, Suzane S. de Sá, Scot T. Martin, and Jose L. Jimenez
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-263, https://doi.org/10.5194/amt-2021-263, 2021
Preprint under review for AMT
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Particle-phase nitrates are an important component of atmospheric aerosols and chemistry. In this manuscript, we systematically explore the application of aerosol mass spectrometry (AMS) to quantify the organic and inorganic nitrate fractions of aerosols in the atmosphere. While AMS has been used for a decade to quantify nitrates, methods are not standardized. We make recommendations for a more universal approach based on this analysis of a large range of field and laboratory observations.
Jiajue Chai, Jack E. Dibb, Bruce E. Anderson, Claire Bekker, Danielle E. Blum, Eric Heim, Carolyn E. Jordan, Emily E. Joyce, Jackson H. Kaspari, Hannah Munro, Wendell W. Walters, and Meredith G. Hastings
Atmos. Chem. Phys., 21, 13077–13098, https://doi.org/10.5194/acp-21-13077-2021, https://doi.org/10.5194/acp-21-13077-2021, 2021
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Nitrous acid (HONO) derived from wildfire emissions plays a key role in controlling atmospheric oxidation chemistry. However, the HONO budget remains poorly constrained. By combining the field-observed concentrations and novel isotopic composition (N and O) of HONO and nitrogen oxides (NOx), we quantitatively constrained the relative contribution of each pathway to secondary HONO production and the relative importance of major atmospheric oxidants (ozone versus peroxy) in aged wildfire smoke.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-672, https://doi.org/10.5194/acp-2021-672, 2021
Preprint under review for ACP
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. High CHOCHO concentrations were observed over highly populated cities and industrial areas. Aromatics were the most important precursors of CHOCHO production. Loss path to aerosol was the highest sink contributing to ~20 % of SOA formation. CHOCHO uptake rate can be affected by aerosol viscosity and irradiation. Finally, our work highlights the lacking knowledge to explain the CHOCHO solubility.
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.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, and Claudia A. Octaviano Villasana
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-671, https://doi.org/10.5194/acp-2021-671, 2021
Revised manuscript under review for ACP
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peaks in 2014, in contrast to the report of steady decreasing trend over 2010–2017 from US EPA.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-583, https://doi.org/10.5194/acp-2021-583, 2021
Preprint under review for ACP
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite based NOx emissions for several UK cities. In the case of London and Manchester, the NAEI NOx emissions are potentially too low by > 25 %.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Tia R. Scarpelli, Melissa P. Sulprizio, Yuzhong Zhang, and Chris H. Rycroft
Atmos. Meas. Tech., 14, 5521–5534, https://doi.org/10.5194/amt-14-5521-2021, https://doi.org/10.5194/amt-14-5521-2021, 2021
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Analytical inversions of satellite observations of atmospheric composition can improve emissions estimates and quantify errors but are computationally expensive at high resolutions. We propose two methods to decrease this cost. The methods reproduce a high-resolution inversion at a quarter of the cost. The reduced-dimension method creates a multiscale grid. The reduced-rank method solves the inversion where information content is highest.
Erin R. Delaria, Jinsol Kim, Helen L. Fitzmaurice, Catherine Newman, Paul J. Wooldridge, Kevin Worthington, and Ronald C. Cohen
Atmos. Meas. Tech., 14, 5487–5500, https://doi.org/10.5194/amt-14-5487-2021, https://doi.org/10.5194/amt-14-5487-2021, 2021
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The use of a dense network of low-cost CO2 sensors is an attractive option for measuring CO2 emissions in cities. However, these low-cost sensors are also subject to uncertainties. Here, we describe a novel method of field calibration for correcting temperature-related errors in the CO2 sensors deployed in the BEACO2N network. We show that with this temperature correction, we can achieve a sufficiently low network error to allow for the evaluation of CO2 emissions at a neighborhood scale.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea 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. Discuss., https://doi.org/10.5194/amt-2021-223, https://doi.org/10.5194/amt-2021-223, 2021
Revised manuscript accepted for AMT
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Satellite-derived NOx emissions from biomass burning are derived 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.
Thomas E. Taylor, Christopher W. O'Dell, David Crisp, Akhiko Kuze, Hannakaisa Lindqvist, Paul O. Wennberg, Abhishek Chatterjee, Michael Gunson, Annmarie Eldering, Brendan Fisher, Matthäus Kiel, Robert R. Nelson, Aronne Merrelli, Greg Osterman, Frédéric Chevallier, Paul I. Palmer, Liang Feng, Nicholas M. Deutscher, Manvendra K. Dubey, Dietrich G. Feist, Omaira E. Garcia, David Griffith, Frank Hase, Laura T. Iraci, Rigel Kivi, Cheng Liu, Martine De Mazière, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Coleen M. Roehl, Matthias Schneider, Mahesh Kumar Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, and Debra Wunch
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2021-247, https://doi.org/10.5194/essd-2021-247, 2021
Revised manuscript accepted for ESSD
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We provide an analysis of an eleven year record of atmospheric carbon dioxide (CO2) concentrations derived using an optimal estimation retrieval algorithm on measurements made by the GOSAT satellite . The new product (version 9) shows improvement over the previous version (v7.3) as evaluated against independent estimates of CO2 from ground-based sensors and atmospheric inversion systems. We also compare the new GOSAT CO2 values to collocated estimates from NASA's Orbiting Carbon Observatory-2.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript under review for ACP
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
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.
Kelvin Bates, Daniel Jacob, Ke Li, Peter Ivatt, Mat Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-605, https://doi.org/10.5194/acp-2021-605, 2021
Revised manuscript accepted for ACP
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Beata Bukosa, Jenny Fisher, Nicholas Deutscher, and Dylan Jones
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-173, https://doi.org/10.5194/gmd-2021-173, 2021
Revised manuscript under review for GMD
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Human activities led to rising levels of greenhouse gases (carbon dioxide (CO2), methane (CH4), carbon monoxide (CO)) in the atmosphere, threatening our future. We use models and measurements to predict and understand the climatological impact of these gases. Here, we describe a new simulation in the GEOS-Chem model that uses a more accurate method to simulate CO2, CH4 and CO, through their chemical dependence. Relative to the original simulations our results agree better with measurements.
Andrew Zammit-Mangion, Michael Bertolacci, Jenny Fisher, Ann Stavert, Matthew L. Rigby, Yi Cao, and Noel Cressie
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-181, https://doi.org/10.5194/gmd-2021-181, 2021
Revised manuscript accepted for GMD
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We present a statistical framework for estimating the sources and sinks (flux) of carbon dioxide from satellite data. The framework is statistical, and yields measures of uncertainty alongside all estimates of flux and other parameters in the underlying model. It also allows us to generate other insights, such as the size of errors and biases in the data. The primary aim of this research was to develop a fully statistical flux inversion framework for use by atmospheric scientists.
Jun Meng, Randall V. Martin, Paul Ginoux, Melanie Hammer, Melissa P. Sulprizio, David A. Ridley, and Aaron van Donkelaar
Geosci. Model Dev., 14, 4249–4260, https://doi.org/10.5194/gmd-14-4249-2021, https://doi.org/10.5194/gmd-14-4249-2021, 2021
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Dust emissions in models, for example, GEOS-Chem, have a strong nonlinear dependence on meteorology, which means dust emission strengths calculated from different resolution meteorological fields are different. Offline high-resolution dust emissions with an optimized global dust strength, presented in this work, can be implemented into GEOS-Chem as offline emission inventory so that it could promote model development by harmonizing dust emissions across simulations of different resolutions.
Xueling Liu, Arthur P. Mizzi, Jeffrey L. Anderson, Inez Fung, and Ronald C. Cohen
Atmos. Chem. Phys., 21, 9573–9583, https://doi.org/10.5194/acp-21-9573-2021, https://doi.org/10.5194/acp-21-9573-2021, 2021
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Observations of winds in the planetary boundary layer remain sparse, making it challenging to simulate and predict the atmospheric conditions that are most important for describing and predicting urban air quality. Here we investigate the application of data assimilation of NO2 columns as will be observed from geostationary orbit to improve predictions and retrospective analysis of wind fields in the boundary layer.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
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.
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. Discuss., https://doi.org/10.5194/acp-2021-389, https://doi.org/10.5194/acp-2021-389, 2021
Revised manuscript accepted for ACP
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Formaldehyde 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 a variety of wildfire plumes sampled by NASA DC-8 during FIREX-AQ field campaign. 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 VOC molecule oxidized in wildfire plumes.
Astrid Müller, Hiroshi Tanimoto, Takafumi Sugita, Toshinobu Machida, Shin-ichiro Nakaoka, Prabir K. Patra, Joshua Laughner, and David Crisp
Atmos. Chem. Phys., 21, 8255–8271, https://doi.org/10.5194/acp-21-8255-2021, https://doi.org/10.5194/acp-21-8255-2021, 2021
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Over oceans, high uncertainties in satellite CO2 retrievals exist due to limited reference data. We combine commercial ship and aircraft observations and, with the aid of model calculations, obtain column-averaged mixing ratios of CO2 (XCO2) data over the Pacific Ocean. This new dataset has great potential as a robust reference for XCO2 measured from space and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Dongwook Kim, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 3631–3655, https://doi.org/10.5194/amt-14-3631-2021, https://doi.org/10.5194/amt-14-3631-2021, 2021
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We utilize a set of high-quality datasets collected during the NASA Atmospheric Tomography Mission to investigate the impact of differences in observable particle sizes across aerosol instruments in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of an Aerodyne aerosol mass spectrometer (AMS) when sampling remote aerosols across the globe.
David R. Lyon, Benjamin Hmiel, Ritesh Gautam, Mark Omara, Katherine A. Roberts, Zachary R. Barkley, Kenneth J. Davis, Natasha L. Miles, Vanessa C. Monteiro, Scott J. Richardson, Stephen Conley, Mackenzie L. Smith, Daniel J. Jacob, Lu Shen, Daniel J. Varon, Aijun Deng, Xander Rudelis, Nikhil Sharma, Kyle T. Story, Adam R. Brandt, Mary Kang, Eric A. Kort, Anthony J. Marchese, and Steven P. Hamburg
Atmos. Chem. Phys., 21, 6605–6626, https://doi.org/10.5194/acp-21-6605-2021, https://doi.org/10.5194/acp-21-6605-2021, 2021
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The Permian Basin (USA) is the world’s largest oil field. We use tower- and aircraft-based approaches to measure how methane emissions in the Permian Basin changed throughout 2020. In early 2020, 3.3 % of the region’s gas was emitted; then in spring 2020, the loss rate temporarily dropped to 1.9 % as oil price crashed. We find this short-term reduction to be a result of reduced well development, less gas flaring, and fewer abnormal events despite minimal reductions in oil and gas production.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Karn Vohra, Eloise A. Marais, Shannen Suckra, Louisa Kramer, William J. Bloss, Ravi Sahu, Abhishek Gaur, Sachchida N. Tripathi, Martin Van Damme, Lieven Clarisse, and Pierre-F. Coheur
Atmos. Chem. Phys., 21, 6275–6296, https://doi.org/10.5194/acp-21-6275-2021, https://doi.org/10.5194/acp-21-6275-2021, 2021
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We find satellite observations of atmospheric composition generally reproduce variability in surface air pollution, so we use their long record to estimate air quality trends in major UK and Indian cities. Our trend analysis shows that pollutants targeted with air quality policies have not declined in Delhi and Kanpur but have in London and Birmingham, with the exception of a recent and dramatic increase in reactive volatile organics in London. Unregulated ammonia has increased only in Delhi.
Sébastien Roche, Kimberly Strong, Debra Wunch, Joseph Mendonca, Colm Sweeney, Bianca Baier, Sébastien C. Biraud, Joshua L. Laughner, Geoffrey C. Toon, and Brian J. Connor
Atmos. Meas. Tech., 14, 3087–3118, https://doi.org/10.5194/amt-14-3087-2021, https://doi.org/10.5194/amt-14-3087-2021, 2021
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We evaluate CO2 profile retrievals from ground-based near-infrared solar absorption spectra after implementing several improvements to the GFIT2 retrieval algorithm. Realistic errors in the a priori temperature profile (~ 2 °C in the lower troposphere) are found to be the leading source of differences between the retrieved and true CO2 profiles, differences that are larger than typical CO2 variability. A temperature retrieval or correction is critical to improve CO2 profile retrieval results.
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.
Daniel J. Varon, Dylan Jervis, Jason McKeever, Ian Spence, David Gains, and Daniel J. Jacob
Atmos. Meas. Tech., 14, 2771–2785, https://doi.org/10.5194/amt-14-2771-2021, https://doi.org/10.5194/amt-14-2771-2021, 2021
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Satellites can detect methane emissions by measuring sunlight reflected from the Earth's surface and atmosphere. Here we show that the European Space Agency's Sentinel-2 twin satellites can be used to monitor anomalously large methane point sources around the world, with global coverage every 2–5 days and 20 m spatial resolution. We demonstrate this previously unreported capability through high-frequency Sentinel-2 monitoring of two strong methane point sources in Algeria and Turkmenistan.
Eloise A. Marais, John F. Roberts, Robert G. Ryan, Henk Eskes, K. Folkert Boersma, Sungyeon Choi, Joanna Joiner, Nader Abuhassan, Alberto Redondas, Michel Grutter, Alexander Cede, Laura Gomez, and Monica Navarro-Comas
Atmos. Meas. Tech., 14, 2389–2408, https://doi.org/10.5194/amt-14-2389-2021, https://doi.org/10.5194/amt-14-2389-2021, 2021
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Nitrogen oxides in the upper troposphere have a profound influence on the global troposphere, but routine reliable observations there are exceedingly rare. We apply cloud-slicing to TROPOMI total columns of nitrogen dioxide (NO2) at high spatial resolution to derive near-global observations of NO2 in the upper troposphere and show consistency with existing datasets. These data offer tremendous potential to address knowledge gaps in this oft underappreciated portion of the atmosphere.
Pamela S. Rickly, Lu Xu, John D. Crounse, Paul O. Wennberg, and Andrew W. Rollins
Atmos. Meas. Tech., 14, 2429–2439, https://doi.org/10.5194/amt-14-2429-2021, https://doi.org/10.5194/amt-14-2429-2021, 2021
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Key improvements have been made to an in situ laser-induced fluorescence instrument for measuring SO2 in polluted and pristine environments. Laser linewidth is reduced, rapid laser tuning is implemented, and fluorescence bandpass filters are optimized. These improvements have led to a 50 % reduction in instrument detection limit. The influence of aromatic compounds was also investigated and determined to not bias SO2 measurements.
Xiao Lu, Daniel J. Jacob, Yuzhong Zhang, Joannes D. Maasakkers, Melissa P. Sulprizio, Lu Shen, Zhen Qu, Tia R. Scarpelli, Hannah Nesser, Robert M. Yantosca, Jianxiong Sheng, Arlyn Andrews, Robert J. Parker, Hartmut Boesch, A. Anthony Bloom, and Shuang Ma
Atmos. Chem. Phys., 21, 4637–4657, https://doi.org/10.5194/acp-21-4637-2021, https://doi.org/10.5194/acp-21-4637-2021, 2021
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We use an analytical solution to the Bayesian inverse problem to quantitatively compare and combine the information from satellite and in situ observations, and to estimate global methane budget and their trends over the 2010–2017 period. We find that satellite and in situ observations are to a large extent complementary in the inversion for estimating global methane budget, and reveal consistent corrections of regional anthropogenic and wetland methane emissions relative to the prior inventory.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jianxiong Sheng, Yuzhong Zhang, Xiao Lu, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, and Robert J. Parker
Atmos. Chem. Phys., 21, 4339–4356, https://doi.org/10.5194/acp-21-4339-2021, https://doi.org/10.5194/acp-21-4339-2021, 2021
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We use 2010–2015 GOSAT satellite observations of atmospheric methane over North America in a high-resolution inversion to estimate methane emissions. We find general consistency with the gridded EPA inventory but higher oil and gas production emissions, with oil production emissions twice as large as in the latest EPA Greenhouse Gas Inventory. We find lower wetland emissions than predicted by WetCHARTs and a small increasing trend in the eastern US, apparently related to unconventional oil/gas.
Yuzhong Zhang, Daniel J. Jacob, Xiao Lu, Joannes D. Maasakkers, Tia R. Scarpelli, Jian-Xiong Sheng, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Jinfeng Chang, A. Anthony Bloom, Shuang Ma, John Worden, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 21, 3643–3666, https://doi.org/10.5194/acp-21-3643-2021, https://doi.org/10.5194/acp-21-3643-2021, 2021
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We use 2010–2018 satellite observations of atmospheric methane to interpret the factors controlling atmospheric methane and its accelerating increase during the period. The 2010–2018 increase in global methane emissions is driven by tropical and boreal wetlands and tropical livestock (South Asia, Africa, Brazil), with an insignificant positive trend in emissions from the fossil fuel sector. The peak methane growth rates in 2014–2015 are also contributed by low OH and high fire emissions.
Alexander J. Turner, Philipp Köhler, Troy S. Magney, Christian Frankenberg, Inez Fung, and Ronald C. Cohen
Biogeosciences Discuss., https://doi.org/10.5194/bg-2021-49, https://doi.org/10.5194/bg-2021-49, 2021
Revised manuscript accepted for BG
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This work builds a high-resolution estimate (500-m) of gross primary productivity (GPP) over the United States using satellite measurements of solar-induced chlorophyll fluorescence from TROPOMI between 2018 and 2020. We identify ecosystem-specific scaling factors for estimating GPP from TROPOMI SIF. We find that extreme precipitation events drive four regional GPP anomalies that account for 28 % of the year-to-year differences in GPP across the United States.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Kelvin Bates, Jiawei Zhuang, and Wei Chen
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-425, https://doi.org/10.5194/gmd-2020-425, 2021
Preprint under review for GMD
Bo Zhang, Hongyu Liu, James H. Crawford, Gao Chen, T. Duncan Fairlie, Scott Chambers, Chang-Hee Kang, Alastair G. Williams, Kai Zhang, David B. Considine, Melissa P. Sulprizio, and Robert M. Yantosca
Atmos. Chem. Phys., 21, 1861–1887, https://doi.org/10.5194/acp-21-1861-2021, https://doi.org/10.5194/acp-21-1861-2021, 2021
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We simulate atmospheric 222Rn using the GEOS-Chem model to improve understanding of 222Rn emissions and characterize convective transport in the model. We demonstrate the potential of a customized global 222Rn emission scenario to improve simulated surface 222Rn concentrations and seasonality. We assess convective transport using observed 222Rn vertical profiles. Results have important implications for using chemical transport models to interpret the transport of trace gases and aerosols.
Alba Lorente, Tobias Borsdorff, Andre Butz, Otto Hasekamp, Joost aan de Brugh, Andreas Schneider, Lianghai Wu, Frank Hase, Rigel Kivi, Debra Wunch, David F. Pollard, Kei Shiomi, Nicholas M. Deutscher, Voltaire A. Velazco, Coleen M. Roehl, Paul O. Wennberg, Thorsten Warneke, and Jochen Landgraf
Atmos. Meas. Tech., 14, 665–684, https://doi.org/10.5194/amt-14-665-2021, https://doi.org/10.5194/amt-14-665-2021, 2021
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TROPOMI aboard Sentinel-5P satellite provides methane (CH4) measurements with exceptional temporal and spatial resolution. The study describes a series of improvements developed to retrieve CH4 from TROPOMI. The updated CH4 product features (among others) a more accurate a posteriori correction derived independently of any reference data. The validation of the improved data product shows good agreement with ground-based and satellite measurements, which highlights the quality of the TROPOMI CH4.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
Sabour Baray, Daniel J. Jacob, Joannes D. Massakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1195, https://doi.org/10.5194/acp-2020-1195, 2021
Revised manuscript accepted for ACP
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We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada, and lower natural emissions from Boreal wetlands.
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.
Robert J. Parker, Alex Webb, Hartmut Boesch, Peter Somkuti, Rocio Barrio Guillo, Antonio Di Noia, Nikoleta Kalaitzi, Jasdeep S. Anand, Peter Bergamaschi, Frederic Chevallier, Paul I. Palmer, Liang Feng, Nicholas M. Deutscher, Dietrich G. Feist, David W. T. Griffith, Frank Hase, Rigel Kivi, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, Christof Petri, David F. Pollard, Coleen Roehl, Mahesh K. Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Thorsten Warneke, Paul O. Wennberg, and Debra Wunch
Earth Syst. Sci. Data, 12, 3383–3412, https://doi.org/10.5194/essd-12-3383-2020, https://doi.org/10.5194/essd-12-3383-2020, 2020
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This work presents the latest release of the University of Leicester GOSAT methane data and acts as the definitive description of this dataset. We detail the processing, validation and evaluation involved in producing these data and highlight its many applications. With now over a decade of global atmospheric methane observations, this dataset has helped, and will continue to help, us better understand the global methane budget and investigate how it may respond to a future changing climate.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Erin R. Delaria, Bryan K. Place, Amy X. Liu, and Ronald C. Cohen
Atmos. Chem. Phys., 20, 14023–14041, https://doi.org/10.5194/acp-20-14023-2020, https://doi.org/10.5194/acp-20-14023-2020, 2020
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Observations of NO2 deposition to vegetation have been widely reported, but the magnitude and mechanism remain uncertain. We use laboratory measurements to study NO2 deposition to leaves of 10 native California tree species. We report important differences in the uptake rates between species and find that this process is primarily diffusion-regulated. We suggest that processes within leaves at a cellular level represent a negligible limitation to NO2 deposition at the canopy level.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
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.
Erik Lutsch, Kimberly Strong, Dylan B. A. Jones, Thomas Blumenstock, Stephanie Conway, Jenny A. Fisher, James W. Hannigan, Frank Hase, Yasuko Kasai, Emmanuel Mahieu, Maria Makarova, Isamu Morino, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Anatoly V. Poberovskii, Ralf Sussmann, and Thorsten Warneke
Atmos. Chem. Phys., 20, 12813–12851, https://doi.org/10.5194/acp-20-12813-2020, https://doi.org/10.5194/acp-20-12813-2020, 2020
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This paper describes the use of a network of 10 Arctic and midlatitude ground-based FTIR measurement sites to detect enhancements of the wildfire tracers carbon monoxide, hydrogen cyanide, and ethane from 2003 to 2018. A tagged CO GEOS-Chem simulation is used for source attribution and to evaluate the relative contribution of CO sources to the FTIR measurements. The use of FTIR measurements allowed for the emission ratios of hydrogen cyanide and ethane to be quantified.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
Viral Shah, Daniel J. Jacob, Jonathan M. Moch, Xuan Wang, and Shixian Zhai
Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, https://doi.org/10.5194/acp-20-12223-2020, 2020
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Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
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 %.
Ke Li, Daniel J. Jacob, Lu Shen, Xiao Lu, Isabelle De Smedt, and Hong Liao
Atmos. Chem. Phys., 20, 11423–11433, https://doi.org/10.5194/acp-20-11423-2020, https://doi.org/10.5194/acp-20-11423-2020, 2020
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Surface summer ozone increased in China from 2013 to 2019 despite new governmental efforts targeting ozone pollution. We find that the ozone increase is mostly due to anthropogenic drivers, although meteorology also plays a role. Further analysis for the North China Plain shows that PM2.5 continued to decrease through 2019, while emissions of volatile organic compounds (VOCs) stayed flat. This could explain the anthropogenic increase in ozone, as PM2.5 scavenges the radical precursors of ozone.
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.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
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This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Revised manuscript has not been submitted
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Yi Ji, L. Gregory Huey, David J. Tanner, Young Ro Lee, Patrick R. Veres, J. Andrew Neuman, Yuhang Wang, and Xinming Wang
Atmos. Meas. Tech., 13, 3683–3696, https://doi.org/10.5194/amt-13-3683-2020, https://doi.org/10.5194/amt-13-3683-2020, 2020
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A common way of measuring trace gases in the atmosphere is chemical ionization mass spectrometry. One large drawback of these instruments is that they require radioactive ion sources. In this work we demonstrate a simple ion source that uses a small krypton lamp that can be used to replace a radioactive source.
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.
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.
Xinning Wang, Xingnan Ye, Jianmin Chen, Xiaofei Wang, Xin Yang, Tzung-May Fu, Lei Zhu, and Chongxuan Liu
Atmos. Chem. Phys., 20, 6273–6290, https://doi.org/10.5194/acp-20-6273-2020, https://doi.org/10.5194/acp-20-6273-2020, 2020
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Hygroscopicity plays several key roles in determining aerosol optical properties and aging processes in the atmosphere. However, it is quite difficult to study aerosol hygroscopicity at the single-particle level. In this study, we built a comprehensive database linking hygroscopicities and mass spectra of individual particles. Based on the measured hygroscopicity–composition relations, we developed a statistical method to estimate ambient particle hygroscopicity just from their mass spectra.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Xuan Wang, and Wei Chen
Geosci. Model Dev., 13, 2475–2486, https://doi.org/10.5194/gmd-13-2475-2020, https://doi.org/10.5194/gmd-13-2475-2020, 2020
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Chemical mechanisms in air quality models tend to get more complicated with time, reflecting both increasing knowledge and the need for greater scope. This objectively improves the models but increases the computational burden. In this work, we present an approach that can reduce the computational cost of chemical integration by 30–40 % while maintaining an accuracy better than 1 %. It retains the complexity of the full mechanism where it is needed and preserves full diagnostic information.
Sungyeon Choi, Lok N. Lamsal, Melanie Follette-Cook, Joanna Joiner, Nickolay A. Krotkov, William H. Swartz, Kenneth E. Pickering, Christopher P. Loughner, Wyat Appel, Gabriele Pfister, Pablo E. Saide, Ronald C. Cohen, Andrew J. Weinheimer, and Jay R. Herman
Atmos. Meas. Tech., 13, 2523–2546, https://doi.org/10.5194/amt-13-2523-2020, https://doi.org/10.5194/amt-13-2523-2020, 2020
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.
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.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Tia R. Scarpelli, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Kelly Rose, Lucy Romeo, John R. Worden, and Greet Janssens-Maenhout
Earth Syst. Sci. Data, 12, 563–575, https://doi.org/10.5194/essd-12-563-2020, https://doi.org/10.5194/essd-12-563-2020, 2020
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Methane, a potent greenhouse gas, is emitted through the exploitation of oil, gas, and coal resources, and many efforts to reduce emissions have targeted these sources. We have created a global inventory of oil, gas, and coal methane emissions based on country reporting to the United Nations. The inventory can be used along with satellite observations of methane to better understand the contribution of these sources to global emissions and to identify potential biases in emissions reporting.
Erin R. Delaria and Ronald C. Cohen
Atmos. Chem. Phys., 20, 2123–2141, https://doi.org/10.5194/acp-20-2123-2020, https://doi.org/10.5194/acp-20-2123-2020, 2020
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Uptake of nitrogen dioxide (NO2) through pores in the surfaces of leaves has been identified as a significant, but inadequately understood, loss process of atmospheric nitrogen oxides. We have constructed a simple model for examining the impact of NO2 foliar uptake on the atmospheric chemistry of nitrogen oxides. We show that an accurate representation in atmospheric models of the effects of weather and soil conditions on leaf NO2 uptake may be important for accurately predicting NO2 deposition.
Viral Shah, Daniel J. Jacob, Ke Li, Rachel F. Silvern, Shixian Zhai, Mengyao Liu, Jintai Lin, and Qiang Zhang
Atmos. Chem. Phys., 20, 1483–1495, https://doi.org/10.5194/acp-20-1483-2020, https://doi.org/10.5194/acp-20-1483-2020, 2020
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We analyze 15 years of satellite observations of nitrogen dioxide (NO2) and use an atmospheric chemistry model to understand the seasonal changes and trends in nitrogen oxides (NOx) over China. We show that the seasonal changes in NO2 occur due to changes in the NOx oxidation lifetime. We find that Chinese NOx emissions peaked in 2011 and had decreased by about 25 % by 2018. But the decrease in NO2 in winter was larger, likely because of a simultaneous decrease in the NOx oxidation lifetime.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Alexander J. Turner, Philipp Köhler, Troy S. Magney, Christian Frankenberg, Inez Fung, and Ronald C. Cohen
Biogeosciences, 17, 405–422, https://doi.org/10.5194/bg-17-405-2020, https://doi.org/10.5194/bg-17-405-2020, 2020
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We present the highest resolution solar-induced chlorophyll fluorescence (SIF) dataset from satellite measurements, providing previously unobservable phenomena related to plant photosynthesis. We find a strong correspondence between TROPOMI SIF and AmeriFlux GPP. We then observe a double peak in the seasonality of California's photosynthesis, not seen by traditional vegetation indices (e.g., MODIS). This is further corroborated by EOF/PC analysis.
Paul S. Romer Present, Azimeh Zare, and Ronald C. Cohen
Atmos. Chem. Phys., 20, 267–279, https://doi.org/10.5194/acp-20-267-2020, https://doi.org/10.5194/acp-20-267-2020, 2020
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The chemistry of nitrogen oxides (NOx) affects both air quality and climate through its role in the production of ozone and secondary aerosols. We find that recent changes in emissions have caused a significant shift in the chemical loss of NOx away from direct production of HNO3 and towards production of organic nitrates. This shift is leading to a flatter distribution of NOx across the United States and helping transform air pollution from a local issue into a broader regional concern.
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.
Joshua D. Shutter, Norton T. Allen, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 6079–6089, https://doi.org/10.5194/amt-12-6079-2019, https://doi.org/10.5194/amt-12-6079-2019, 2019
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A new mid-infrared and ultra-portable formaldehyde (HCHO) sensor from Aeris Technologies is characterized and evaluated against well-established laser-induced fluorescence (LIF) instrumentation. The Aeris sensor displays linear behavior (R squared > 0.94) and shows good agreement with LIF instruments. While the compact sensor is not currently a replacement for the most sensitive research-grade instrumentation available, its sub-ppbv precision is sufficient for indoor and outdoor HCHO monitoring.
Susan S. Kulawik, Sean Crowell, David Baker, Junjie Liu, Kathryn McKain, Colm Sweeney, Sebastien C. Biraud, Steve Wofsy, Christopher W. O'Dell, Paul O. Wennberg, Debra Wunch, Coleen M. Roehl, Nicholas M. Deutscher, Matthäus Kiel, David W. T. Griffith, Voltaire A. Velazco, Justus Notholt, Thorsten Warneke, Christof Petri, Martine De Mazière, Mahesh K. Sha, Ralf Sussmann, Markus Rettinger, Dave F. Pollard, Isamu Morino, Osamu Uchino, Frank Hase, Dietrich G. Feist, Sébastien Roche, Kimberly Strong, Rigel Kivi, Laura Iraci, Kei Shiomi, Manvendra K. Dubey, Eliezer Sepulveda, Omaira Elena Garcia Rodriguez, Yao Té, Pascal Jeseck, Pauli Heikkinen, Edward J. Dlugokencky, Michael R. Gunson, Annmarie Eldering, David Crisp, Brendan Fisher, and Gregory B. Osterman
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2019-257, https://doi.org/10.5194/amt-2019-257, 2019
Publication in AMT not foreseen
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This paper provides a benchmark of OCO-2 v8 and ACOS-GOSAT v7.3 XCO2 and lowermost tropospheric (LMT) errors. The paper focuses on the systematic errors and subtracts out validation, co-location, and random errors, looks at the correlation scale-length (spatially and temporally) of systematic errors, finding that the scale lengths are similar to bias correction scale-lengths. The assimilates of the bias correction term is used to place an error on fluxes estimates.
Daniel H. Cusworth, Daniel J. Jacob, Daniel J. Varon, Christopher Chan Miller, Xiong Liu, Kelly Chance, Andrew K. Thorpe, Riley M. Duren, Charles E. Miller, David R. Thompson, Christian Frankenberg, Luis Guanter, and Cynthia A. Randles
Atmos. Meas. Tech., 12, 5655–5668, https://doi.org/10.5194/amt-12-5655-2019, https://doi.org/10.5194/amt-12-5655-2019, 2019
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We examine the potential for global detection of methane plumes from individual point sources with the new generation of spaceborne imaging spectrometers scheduled for launch in 2019–2025. We perform methane retrievals on simulated scenes with varying surfaces and atmospheric methane concentrations. Our results suggest that imaging spectrometers in space could play a transformative role in the future for quantifying methane emissions from point sources on a global scale.
Qindan Zhu, Joshua L. Laughner, and Ronald C. Cohen
Atmos. Chem. Phys., 19, 13067–13078, https://doi.org/10.5194/acp-19-13067-2019, https://doi.org/10.5194/acp-19-13067-2019, 2019
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Lightning NOx represents > 80 % of the NOx source in the upper troposphere. Despite its importance, lightning NOx is poorly understood. This work improves model performance in representing lighting NOx and reduces the uncertainty in satellite NO2 retrievals caused by poor representation of lightning NOx emissions in a priori assumptions.
Jacob K. Hedelius, Tai-Long He, Dylan B. A. Jones, Bianca C. Baier, Rebecca R. Buchholz, Martine De Mazière, Nicholas M. Deutscher, Manvendra K. Dubey, Dietrich G. Feist, David W. T. Griffith, Frank Hase, Laura T. Iraci, Pascal Jeseck, Matthäus Kiel, Rigel Kivi, Cheng Liu, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Sébastien Roche, Coleen M. Roehl, Matthias Schneider, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Colm Sweeney, Yao Té, Osamu Uchino, Voltaire A. Velazco, Wei Wang, Thorsten Warneke, Paul O. Wennberg, Helen M. Worden, and Debra Wunch
Atmos. Meas. Tech., 12, 5547–5572, https://doi.org/10.5194/amt-12-5547-2019, https://doi.org/10.5194/amt-12-5547-2019, 2019
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We seek ways to improve the accuracy of column measurements of carbon monoxide (CO) – an important tracer of pollution – made from the MOPITT satellite instrument. We devise a filtering scheme which reduces the scatter and also eliminates bias among the MOPITT detectors. Compared to ground-based observations, MOPITT measurements are about 6 %–8 % higher. When MOPITT data are implemented in a global assimilation model, they tend to reduce the model mismatch with aircraft measurements.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Jason M. St. Clair, Andrew K. Swanson, Steven A. Bailey, and Thomas F. Hanisco
Atmos. Meas. Tech., 12, 4581–4590, https://doi.org/10.5194/amt-12-4581-2019, https://doi.org/10.5194/amt-12-4581-2019, 2019
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NASA Compact Airborne Formadehyde Experiment (CAFE) is a nonresonant laser-induced fluorescence instrument for airborne in situ measurement of formaldehyde (HCHO). The instrument is described here with highlighted improvements from the predecessor instrument, COmpact Formaldehyde FluorescencE Experiment (COFFEE).
Shixian Zhai, Daniel J. Jacob, Xuan Wang, Lu Shen, Ke Li, Yuzhong Zhang, Ke Gui, Tianliang Zhao, and Hong Liao
Atmos. Chem. Phys., 19, 11031–11041, https://doi.org/10.5194/acp-19-11031-2019, https://doi.org/10.5194/acp-19-11031-2019, 2019
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Observed annual mean PM2.5 decreased by 30–50 % in China from 2013–2018. However, meteorologically PM2.5 variability complicates trend attribution. We used a stepwise multiple linear regression model to quantitatively separate contributions from anthropogenic emissions and meteorology. Results show that 88 % of the PM2.5 decrease across China is attributable to anthropogenic emission changes, and 12 % is attributable to meteorology.
Huisheng Bian, Karl Froyd, Daniel M. Murphy, Jack Dibb, Anton Darmenov, Mian Chin, Peter R. Colarco, Arlindo da Silva, Tom L. Kucsera, Gregory Schill, Hongbin Yu, Paul Bui, Maximilian Dollner, Bernadett Weinzierl, and Alexander Smirnov
Atmos. Chem. Phys., 19, 10773–10785, https://doi.org/10.5194/acp-19-10773-2019, https://doi.org/10.5194/acp-19-10773-2019, 2019
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We address the GEOS-GOCART sea salt simulations constrained by NASA EVS ATom measurements, as well as those by MODIS and the AERONET MAN. The study covers remote regions over the Pacific, Atlantic, and Southern oceans from near the surface to ~ 12 km altitude and covers both summer and winter seasons. Important sea salt fields, e.g., mass mixing ratio, vertical distribution, size distribution, and marine aerosol AOD, as well as their relationship to relative humidity and emissions, are examined.
Katherine R. Travis and Daniel J. Jacob
Geosci. Model Dev., 12, 3641–3648, https://doi.org/10.5194/gmd-12-3641-2019, https://doi.org/10.5194/gmd-12-3641-2019, 2019
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Models of ozone air pollution are often evaluated with the policy metric set by the EPA of the maximum daily 8 h average ozone concentration. These models may be used in policy settings to evaluate air quality regulations. However, most models have difficulty simulating how ozone varies over the course of the day, and thus the use of this metric in model evaluation is problematic. Improved representation of mixed layer dynamics and ozone loss to the surface is needed to resolve this issue.
Kelvin H. Bates and Daniel J. Jacob
Atmos. Chem. Phys., 19, 9613–9640, https://doi.org/10.5194/acp-19-9613-2019, https://doi.org/10.5194/acp-19-9613-2019, 2019
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Isoprene is a highly reactive chemical released to the atmosphere by plants. Its gas-phase reactions and interactions with chemicals released by human activity have far-reaching atmospheric consequences, contributing to ozone and particulate pollution and prolonging the lifetime of methane, a potent greenhouse gas. We use global simulations with a new isoprene reaction scheme to quantify those effects and to show how recently discovered aspects of isoprene chemistry play out on a global scale.
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.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
Rachel F. Silvern, Daniel J. Jacob, Loretta J. Mickley, Melissa P. Sulprizio, Katherine R. Travis, Eloise A. Marais, Ronald C. Cohen, Joshua L. Laughner, Sungyeon Choi, Joanna Joiner, and Lok N. Lamsal
Atmos. Chem. Phys., 19, 8863–8878, https://doi.org/10.5194/acp-19-8863-2019, https://doi.org/10.5194/acp-19-8863-2019, 2019
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The US EPA reports a steady decrease in nitrogen oxide (NOx) emissions from fuel combustion over the 2005–2017 period, while satellite observations show a leveling off after 2009, suggesting emission reductions and related air quality gains have halted. We show the sustained decrease in NOx emissions is in fact consistent with observed trends in surface NO2 and ozone concentrations and that the flattening of the satellite trend reflects a growing influence from the non-anthropogenic background.
Ilana B. Pollack, Jakob Lindaas, J. Robert Roscioli, Michael Agnese, Wade Permar, Lu Hu, and Emily V. Fischer
Atmos. Meas. Tech., 12, 3717–3742, https://doi.org/10.5194/amt-12-3717-2019, https://doi.org/10.5194/amt-12-3717-2019, 2019
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A closed-path infrared absorption spectrometer was outfitted with the option for active continuous passivation for measuring large, rapid gradients in atmospheric NH3 from a research aircraft. In-flight and ground observations show utility in passivant addition for recovering instrument time response when sampling surfaces are contaminated and cannot be cleaned in a timely manner and for maintaining rapid time response in an NH3-rich and humid environment over a several-week-long field campaign.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jian-Xiong Sheng, Yuzhong Zhang, Monica Hersher, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, Greet Janssens-Maenhout, and Robert J. Parker
Atmos. Chem. Phys., 19, 7859–7881, https://doi.org/10.5194/acp-19-7859-2019, https://doi.org/10.5194/acp-19-7859-2019, 2019
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We use 2010–2015 satellite observations of atmospheric methane to improve estimates of methane emissions and their trends, as well as the concentration and trend of tropospheric OH (hydroxyl radical, methane's main sink). We find overestimates of Chinese coal and Middle East oil/gas emissions in the prior estimate. The 2010–2015 growth in methane is attributed to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH is small in comparison.
Beata Bukosa, Nicholas M. Deutscher, Jenny A. Fisher, Dagmar Kubistin, Clare Paton-Walsh, and David W. T. Griffith
Atmos. Chem. Phys., 19, 7055–7072, https://doi.org/10.5194/acp-19-7055-2019, https://doi.org/10.5194/acp-19-7055-2019, 2019
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The carbon greenhouse gases (CO2, CH4 and CO) were proven to have a large impact on the global carbon cycle and our climate. To understand the variability of the carbon cycle and predict future climate change scenarios, we need to study the processes that drive the changes of these gases in the atmosphere. We study the sources and sinks of CO2, CH4 and CO with a combination of measurements and chemical transport modelling to identify missing, underestimated or overestimated sources in Australia.
Lu Shen, Daniel J. Jacob, Xiong Liu, Guanyu Huang, Ke Li, Hong Liao, and Tao Wang
Atmos. Chem. Phys., 19, 6551–6560, https://doi.org/10.5194/acp-19-6551-2019, https://doi.org/10.5194/acp-19-6551-2019, 2019
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
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.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Debra Wunch, Dylan B. A. Jones, Geoffrey C. Toon, Nicholas M. Deutscher, Frank Hase, Justus Notholt, Ralf Sussmann, Thorsten Warneke, Jeroen Kuenen, Hugo Denier van der Gon, Jenny A. Fisher, and Joannes D. Maasakkers
Atmos. Chem. Phys., 19, 3963–3980, https://doi.org/10.5194/acp-19-3963-2019, https://doi.org/10.5194/acp-19-3963-2019, 2019
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We used five atmospheric observatories in Europe measuring total column dry-air mole fractions of methane and carbon monoxide to infer methane emissions in the area between the observatories. We find that the methane emissions are overestimated by the state-of-the-art inventories, and that this is likely due, at least in part, to the inventory disaggregation. We find that there is significant uncertainty in the carbon monoxide inventories that requires further investigation.
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.
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.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Joshua L. Laughner, Qindan Zhu, and Ronald C. Cohen
Atmos. Meas. Tech., 12, 129–146, https://doi.org/10.5194/amt-12-129-2019, https://doi.org/10.5194/amt-12-129-2019, 2019
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We compared v3.0B of the BEHR satellite NO2 product against independent measurements to verify its accuracy. We found that the BEHR product generally performs better than standard NO2 products and the previous version of BEHR. Outside of the SE US, using daily NO2 profiles results in similar or better agreement with independent measurements than using monthly profiles, and direct evaluation of those profiles shows they better describe NO2 distribution in urban areas than monthly profiles.
Krystal T. Vasquez, Hannah M. Allen, John D. Crounse, Eric Praske, Lu Xu, Anke C. Noelscher, and Paul O. Wennberg
Atmos. Meas. Tech., 11, 6815–6832, https://doi.org/10.5194/amt-11-6815-2018, https://doi.org/10.5194/amt-11-6815-2018, 2018
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Oxygenated volatile organic compounds (OVOCs) are difficult to measure in the atmosphere due to their high reactivity and low concentrations. This hinders our understanding of their impact on air quality and climate. Therefore, we have developed a field-deployable instrument capable of providing isomer-resolved measurements of OVOCs in the ambient air. Its performance is assessed through data collected both in the laboratory and during two field studies.
Fabien Paulot, Sergey Malyshev, Tran Nguyen, John D. Crounse, Elena Shevliakova, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 17963–17978, https://doi.org/10.5194/acp-18-17963-2018, https://doi.org/10.5194/acp-18-17963-2018, 2018
Kang Sun, Lei Zhu, Karen Cady-Pereira, Christopher Chan Miller, Kelly Chance, Lieven Clarisse, Pierre-François Coheur, Gonzalo González Abad, Guanyu Huang, Xiong Liu, Martin Van Damme, Kai Yang, and Mark Zondlo
Atmos. Meas. Tech., 11, 6679–6701, https://doi.org/10.5194/amt-11-6679-2018, https://doi.org/10.5194/amt-11-6679-2018, 2018
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An agile, physics-based approach is developed to oversample irregular satellite observations to a high-resolution common grid. Instead of assuming each sounding as a point or a polygon as in previous methods, the proposed physical oversampling represents soundings as distributions of sensitivity on the ground. This sensitivity distribution can be determined by the spatial response function of each satellite sensor, parameterized as generalized 2-D super Gaussian functions.
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.
Christopher W. O'Dell, Annmarie Eldering, Paul O. Wennberg, David Crisp, Michael R. Gunson, Brendan Fisher, Christian Frankenberg, Matthäus Kiel, Hannakaisa Lindqvist, Lukas Mandrake, Aronne Merrelli, Vijay Natraj, Robert R. Nelson, Gregory B. Osterman, Vivienne H. Payne, Thomas E. Taylor, Debra Wunch, Brian J. Drouin, Fabiano Oyafuso, Albert Chang, James McDuffie, Michael Smyth, David F. Baker, Sourish Basu, Frédéric Chevallier, Sean M. R. Crowell, Liang Feng, Paul I. Palmer, Mavendra Dubey, Omaira E. García, David W. T. Griffith, Frank Hase, Laura T. Iraci, Rigel Kivi, Isamu Morino, Justus Notholt, Hirofumi Ohyama, Christof Petri, Coleen M. Roehl, Mahesh K. Sha, Kimberly Strong, Ralf Sussmann, Yao Te, Osamu Uchino, and Voltaire A. Velazco
Atmos. Meas. Tech., 11, 6539–6576, https://doi.org/10.5194/amt-11-6539-2018, https://doi.org/10.5194/amt-11-6539-2018, 2018
Lu Shen, Daniel J. Jacob, Loretta J. Mickley, Yuxuan Wang, and Qiang Zhang
Atmos. Chem. Phys., 18, 17489–17496, https://doi.org/10.5194/acp-18-17489-2018, https://doi.org/10.5194/acp-18-17489-2018, 2018
Eloise A. Marais, Daniel J. Jacob, Sungyeon Choi, Joanna Joiner, Maria Belmonte-Rivas, Ronald C. Cohen, Steffen Beirle, Lee T. Murray, Luke D. Schiferl, Viral Shah, and Lyatt Jaeglé
Atmos. Chem. Phys., 18, 17017–17027, https://doi.org/10.5194/acp-18-17017-2018, https://doi.org/10.5194/acp-18-17017-2018, 2018
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We intercompare two new products of global upper tropospheric nitrogen dioxide (NO2) retrieved from the Ozone Monitoring Instrument (OMI). We evaluate these products with aircraft observations from NASA DC8 aircraft campaigns and interpret the useful information these products can provide about nitrogen oxides (NOx) in the global upper troposphere using the GEOS-Chem chemical transport model.
Jian-Xiong Sheng, Daniel J. Jacob, Joannes D. Maasakkers, Yuzhong Zhang, and Melissa P. Sulprizio
Atmos. Meas. Tech., 11, 6379–6388, https://doi.org/10.5194/amt-11-6379-2018, https://doi.org/10.5194/amt-11-6379-2018, 2018
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We conduct Observing System Simulation Experiments to compare the ability of future satellite measurements of atmospheric methane columns for constraining methane emissions at the 25 km scale. We find that the geostationary instruments can do much better than TROPOMI and are less sensitive to cloud cover. GeoCARB observing twice a day would provide 70 % of the information from the nominal GEO-CAPE mission considered by NASA in response to the Decadal Survey of the US National Research Council.
Daniel H. Cusworth, Daniel J. Jacob, Jian-Xiong Sheng, Joshua Benmergui, Alexander J. Turner, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 16885–16896, https://doi.org/10.5194/acp-18-16885-2018, https://doi.org/10.5194/acp-18-16885-2018, 2018
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Methane emissions from oil/gas fields originate from a large number of small and densely clustered point sources. We examine the potential of recently launched or planned satellites to locate these high-mode emitters through measurements of atmospheric methane. We find that the recently launched TROPOMI and the planned GeoCARB instruments are successful at locating high-emitting sources for fields of 20-50 emitters within the 50 × 50 km2 geographic domain but are unsuccessful for denser fields.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Joshua L. Laughner, Qindan Zhu, and Ronald C. Cohen
Earth Syst. Sci. Data, 10, 2069–2095, https://doi.org/10.5194/essd-10-2069-2018, https://doi.org/10.5194/essd-10-2069-2018, 2018
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This paper describes the upgrade of the BErkeley High Resolution (BEHR) NO2 retrieval from versions 2.1C to 3.0B. This retrieval measures NO2 over the continental US using input data at higher spatial and temporal resolution than global retrievals. We analyze how each part of the upgrade affected the measured NO2. Most interestingly, we find that using NO2 profiles at daily (rather than monthly) time resolution does lead to differences in multi-month averages for regions affected by lightning.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Jacob K. Hedelius, Junjie Liu, Tomohiro Oda, Shamil Maksyutov, Coleen M. Roehl, Laura T. Iraci, James R. Podolske, Patrick W. Hillyard, Jianming Liang, Kevin R. Gurney, Debra Wunch, and Paul O. Wennberg
Atmos. Chem. Phys., 18, 16271–16291, https://doi.org/10.5194/acp-18-16271-2018, https://doi.org/10.5194/acp-18-16271-2018, 2018
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Human activities can cause concentrated emissions of greenhouse gases and other pollutants from cities. There is ongoing effort to convert new satellite observations of pollutants into fluxes for many cities. Here we present a method for determining the flux of three species (CO2, CH4, and CO) from the greater LA area using satellite (CO2 only) and ground-based (all three species) observations. We run tests to estimate uncertainty and find the direct net CO2 flux is 104 ± 26 Tg CO2 yr−1.
Yuzhong Zhang, Daniel J. Jacob, Joannes D. Maasakkers, Melissa P. Sulprizio, Jian-Xiong Sheng, Ritesh Gautam, and John Worden
Atmos. Chem. Phys., 18, 15959–15973, https://doi.org/10.5194/acp-18-15959-2018, https://doi.org/10.5194/acp-18-15959-2018, 2018
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We assess the potential of using satellite observations of atmospheric methane to monitor global mean tropospheric OH concentration, a key parameter for the oxidizing power of the atmosphere.
Azimeh Zare, Paul S. Romer, Tran Nguyen, Frank N. Keutsch, Kate Skog, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 15419–15436, https://doi.org/10.5194/acp-18-15419-2018, https://doi.org/10.5194/acp-18-15419-2018, 2018
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Organic nitrates play an important role in concentrations and distribution of NOx, ozone and aerosol as the most important air pollutants. We develop a state-of-the-science detailed chemical mechanism representing individual organic nitrates, which is appropriate to use in air quality models and results in a more accurate simulation of atmospheric chemistry. Using this mechanism we explore production and removal processes of organic nitrates in a rural environment that are poorly constrained.
Daniel J. Varon, Daniel J. Jacob, Jason McKeever, Dylan Jervis, Berke O. A. Durak, Yan Xia, and Yi Huang
Atmos. Meas. Tech., 11, 5673–5686, https://doi.org/10.5194/amt-11-5673-2018, https://doi.org/10.5194/amt-11-5673-2018, 2018
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Methane is a powerful greenhouse gas emitted from numerous human activities. Space-based observation of point sources would be a cost-effective monitoring solution, but the resolution of most current and planned methane-observing satellites is too coarse to resolve individual emitters. We simulate fine-resolution (50 m) satellite observations of methane plumes as would be measured by GHGSat (to be launched in 2019) and show that such data can usefully quantify large methane point sources.
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.
Erin R. Delaria, Megan Vieira, Julie Cremieux, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 14161–14173, https://doi.org/10.5194/acp-18-14161-2018, https://doi.org/10.5194/acp-18-14161-2018, 2018
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Observations of NOx exchange between the atmosphere and vegetation have been widely reported. However, the magnitude, direction, and mechanism of this atmosphere–biosphere exchange remain uncertain across different ecosystems. We use laboratory measurements to study the rates of NOx deposition to the leaves of a California oak tree species. We detect no evidence of NOx emission and find that NOx loss to oak leaves is substantial even at low NOx concentrations relevant to forested environments.
Alexis A. Shusterman, Jinsol Kim, Kaitlyn J. Lieschke, Catherine Newman, Paul J. Wooldridge, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 13773–13785, https://doi.org/10.5194/acp-18-13773-2018, https://doi.org/10.5194/acp-18-13773-2018, 2018
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We describe the diversity and heterogeneity of urban CO2 levels observed using the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of > 50 CO2 sensors stationed every ~ 2 km across the San Francisco Bay Area. We demonstrate that relatively simple mathematical techniques, applied to these observations, can be used to detect the small changes in highway CO2 emissions expected to result from upcoming fuel economy regulations, affirming the policy relevance of low-cost sensors.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Joshua Benmergui, A. Anthony Bloom, Claudia Arndt, Ritesh Gautam, Daniel Zavala-Araiza, Hartmut Boesch, and Robert J. Parker
Atmos. Chem. Phys., 18, 12257–12267, https://doi.org/10.5194/acp-18-12257-2018, https://doi.org/10.5194/acp-18-12257-2018, 2018
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Analysis of 7 years (2010–2016) of GOSAT methane trends over Canada, the contiguous US, and Mexico suggests that US methane emissions increased by 2.5 ± 1.4 % a−1 over the 7-year period, with contributions from both oil–gas systems and livestock in the Midwest. Mexican emissions show a decrease that can be attributed to a decreasing cattle population. Canadian emissions show year-to-year variability driven by wetland emissions and correlated with wetland areal extent.
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.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Sebastian D. Eastham, Michael S. Long, Christoph A. Keller, Elizabeth Lundgren, Robert M. Yantosca, Jiawei Zhuang, Chi Li, Colin J. Lee, Matthew Yannetti, Benjamin M. Auer, Thomas L. Clune, Jules Kouatchou, William M. Putman, Matthew A. Thompson, Atanas L. Trayanov, Andrea M. Molod, Randall V. Martin, and Daniel J. Jacob
Geosci. Model Dev., 11, 2941–2953, https://doi.org/10.5194/gmd-11-2941-2018, https://doi.org/10.5194/gmd-11-2941-2018, 2018
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Global atmospheric chemical transport models are crucial tools in atmospheric science, used to address problems ranging from climate change to acid rain. GEOS-Chem High Performance (GCHP) is a new implementation of the widely used GEOS-Chem model, designed for massively parallel architectures. GCHP v11-02c is shown to be highly scalable from 6 to over 500 cores, enabling the routine simulation of global atmospheric chemistry from the surface to the stratopause at resolutions of ~50 km or finer.
Chunxiang Ye, Xianliang Zhou, Dennis Pu, Jochen Stutz, James Festa, Max Spolaor, Catalina Tsai, Christopher Cantrell, Roy L. Mauldin III, Andrew Weinheimer, Rebecca S. Hornbrook, Eric C. Apel, Alex Guenther, Lisa Kaser, Bin Yuan, Thomas Karl, Julie Haggerty, Samuel Hall, Kirk Ullmann, James Smith, and John Ortega
Atmos. Chem. Phys., 18, 9107–9120, https://doi.org/10.5194/acp-18-9107-2018, https://doi.org/10.5194/acp-18-9107-2018, 2018
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Substantial levels of HONO existed during the day throughout the troposphere over the southeastern US during NOMADSS 2013. Particulate nitrate photolysis appeared to be the major volume HONO source, while NOx was an important HONO precursor only in industrial and urban plumes. HONO was not a significant OH radical precursor in the rural troposphere away from the ground surface; however, its production from particulate nitrate photolysis was an important renoxification pathway.
Alexander J. Turner, Daniel J. Jacob, Joshua Benmergui, Jeremy Brandman, Laurent White, and Cynthia A. Randles
Atmos. Chem. Phys., 18, 8265–8278, https://doi.org/10.5194/acp-18-8265-2018, https://doi.org/10.5194/acp-18-8265-2018, 2018
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We conduct a 1-week WRF-STILT simulation to generate methane column footprints at 1.3 km spatial resolution and hourly temporal resolution over the Barnett Shale. We find that a week of TROPOMI observations should provide regional (~30 km) information on temporally invariant sources and GeoCARB should provide information on temporally invariant sources at 2–7 km spatial resolution. An instrument precision better than 6 ppb is an important threshold for achieving fine resolution of emissions.
Jian-Xiong Sheng, Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Melissa P. Sulprizio, A. Anthony Bloom, Arlyn E. Andrews, and Debra Wunch
Atmos. Chem. Phys., 18, 6483–6491, https://doi.org/10.5194/acp-18-6483-2018, https://doi.org/10.5194/acp-18-6483-2018, 2018
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We use observations of boundary layer methane from the SEAC4RS aircraft campaign over the Southeast US to estimate methane emissions in that region. Our results suggest that the EPA inventory is regionally unbiased but there are large local biases, suggesting variable emission factors. Our results also suggest that the choice of landcover map is the dominant source of error for wetland emission estimates.
Jiawei Zhuang, Daniel J. Jacob, and Sebastian D. Eastham
Atmos. Chem. Phys., 18, 6039–6055, https://doi.org/10.5194/acp-18-6039-2018, https://doi.org/10.5194/acp-18-6039-2018, 2018
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Our work explains why current model simulations are unable to capture the intercontinental influences of pollution plumes that are often observed over some regions like California. Due to inadequate vertical grid resolution in these models, the plumes get diffused too rapidly during intercontinental transport. Increasing the vertical grid resolution greatly improves the simulation of plumes and considerably increases the estimate of local surface pollution influence.
Young-Suk Oh, S. Takele Kenea, Tae-Young Goo, Kyu-Sun Chung, Jae-Sang Rhee, Mi-Lim Ou, Young-Hwa Byun, Paul O. Wennberg, Matthäus Kiel, Joshua P. DiGangi, Glenn S. Diskin, Voltaire A. Velazco, and David W. T. Griffith
Atmos. Meas. Tech., 11, 2361–2374, https://doi.org/10.5194/amt-11-2361-2018, https://doi.org/10.5194/amt-11-2361-2018, 2018
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We focused on the measurements taken during the period of February 2014 to November 2017. The FTS instrument was stable during the whole measurement period. The g-b FTS retrieval of XCO2 and XCH4 were compared with aircraft measurements that were conducted over Anmyeondo station on 22 May 2016, 29 October, and 12 November 2017. The preliminary comparison results of XCO2 between FTS and OCO-2 were also presented over the Anmyeondo station.
Pieternel F. Levelt, Joanna Joiner, Johanna Tamminen, J. Pepijn Veefkind, Pawan K. Bhartia, Deborah C. Stein Zweers, Bryan N. Duncan, David G. Streets, Henk Eskes, Ronald van der A, Chris McLinden, Vitali Fioletov, Simon Carn, Jos de Laat, Matthew DeLand, Sergey Marchenko, Richard McPeters, Jerald Ziemke, Dejian Fu, Xiong Liu, Kenneth Pickering, Arnoud Apituley, Gonzalo González Abad, Antti Arola, Folkert Boersma, Christopher Chan Miller, Kelly Chance, Martin de Graaf, Janne Hakkarainen, Seppo Hassinen, Iolanda Ialongo, Quintus Kleipool, Nickolay Krotkov, Can Li, Lok Lamsal, Paul Newman, Caroline Nowlan, Raid Suleiman, Lieuwe Gijsbert Tilstra, Omar Torres, Huiqun Wang, and Krzysztof Wargan
Atmos. Chem. Phys., 18, 5699–5745, https://doi.org/10.5194/acp-18-5699-2018, https://doi.org/10.5194/acp-18-5699-2018, 2018
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The aim of this paper is to highlight the many successes of the Ozone Monitoring Instrument (OMI) spanning more than 13 years. Data from OMI have been used in a wide range of applications. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. OMI data continue to be used for new research and applications.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Jinsol Kim, Alexis A. Shusterman, Kaitlyn J. Lieschke, Catherine Newman, and Ronald C. Cohen
Atmos. Meas. Tech., 11, 1937–1946, https://doi.org/10.5194/amt-11-1937-2018, https://doi.org/10.5194/amt-11-1937-2018, 2018
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The newest generation of air quality sensors is small, low cost, and easy to deploy. These sensors are an attractive option for developing dense observation networks in support of regulatory activities and scientific research. However, these sensors are difficult to interpret. Here we describe a novel calibration strategy for a set of low cost sensors and demonstrate this calibration on a subset of the sensors comprising BEACO2N, a distributed network at the San Francisco Bay Area.
Glenn M. Wolfe, S. Randy Kawa, Thomas F. Hanisco, Reem A. Hannun, Paul A. Newman, Andrew Swanson, Steve Bailey, John Barrick, K. Lee Thornhill, Glenn Diskin, Josh DiGangi, John B. Nowak, Carl Sorenson, Geoffrey Bland, James K. Yungel, and Craig A. Swenson
Atmos. Meas. Tech., 11, 1757–1776, https://doi.org/10.5194/amt-11-1757-2018, https://doi.org/10.5194/amt-11-1757-2018, 2018
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We describe a new NASA airborne system for directly observing the surface–atmosphere exchange of greenhouse gases and energy over regional scales. Such measurements are needed benchmark model and satellite products and can improve process-level understanding of greenhouse gas sources and sinks over forest, croplands, wetlands, urban areas, and other ecosystems.
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.
Karen Yu, Christoph A. Keller, Daniel J. Jacob, Andrea M. Molod, Sebastian D. Eastham, and Michael S. Long
Geosci. Model Dev., 11, 305–319, https://doi.org/10.5194/gmd-11-305-2018, https://doi.org/10.5194/gmd-11-305-2018, 2018
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Global simulations of atmospheric chemistry are generally conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it is unable to reproduce the GCM transport exactly. We investigate the cascade of errors associated with the off-line approach using the GEOS-5 GCM and GEOS-Chem CTM and discuss improvements in the use of archived meteorology.
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.
Jason M. St. Clair, Andrew K. Swanson, Steven A. Bailey, Glenn M. Wolfe, Josette E. Marrero, Laura T. Iraci, John G. Hagopian, and Thomas F. Hanisco
Atmos. Meas. Tech., 10, 4833–4844, https://doi.org/10.5194/amt-10-4833-2017, https://doi.org/10.5194/amt-10-4833-2017, 2017
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Formaldehyde is an abundant, photochemically influential trace species in the Earth’s atmosphere. We present a new instrument for measuring atmospheric formaldehyde using a laser-based measurement technique that is more compact and lower cost than previous laser-based formaldehyde instruments. The instrument is part of the Alpha Jet Atmospheric eXperiment (AJAX) payload at the NASA Ames Research Center and has collected data on 27 flights between December 2015 and March 2017.
Joshua L. Laughner and Ronald C. Cohen
Atmos. Meas. Tech., 10, 4403–4419, https://doi.org/10.5194/amt-10-4403-2017, https://doi.org/10.5194/amt-10-4403-2017, 2017
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NO2 (a gas that plays an important role in air quality) can be measured by satellite-based instruments. These measurements require a best guess of the vertical distribution of NO2 and are very sensitive to the changes in that distribution near the top of the troposphere (~ 12 km). NO2 concentrations at this altitude are strongly influenced by lightning; therefore, we study how different representations of lightning in models that provide that best guess affect the NO2 measured by satellites.
Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144, https://doi.org/10.5194/gmd-10-4129-2017, https://doi.org/10.5194/gmd-10-4129-2017, 2017
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Carbon monoxide (CO) simulation in atmospheric chemistry models is used for source–receptor analysis, emission inversion, and interpretation of observations. We introduce a major update to CO simulation in the GEOS-Chem chemical transport model that removes fundamental inconsistencies relative to the standard model, resolving biases of more than 100 ppb and errors in vertical structure. We also add source tagging of secondary CO and demonstrate it provides added value in low-emission regions.
Dean Howard, Peter F. Nelson, Grant C. Edwards, Anthony L. Morrison, Jenny A. Fisher, Jason Ward, James Harnwell, Marcel van der Schoot, Brad Atkinson, Scott D. Chambers, Alan D. Griffiths, Sylvester Werczynski, and Alastair G. Williams
Atmos. Chem. Phys., 17, 11623–11636, https://doi.org/10.5194/acp-17-11623-2017, https://doi.org/10.5194/acp-17-11623-2017, 2017
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Mercury, a toxic metal, can be transported globally through the atmosphere, with deposition to ecosystems an important pathway to human exposure. 2 years of atmospheric mercury monitoring in tropical Australia supports recent evidence that Southern Hemisphere concentrations are lower than previously thought. Exchange between the atmosphere and ecosystems can take place on daily scales, with night deposition offset by morning re-emission. This could be an important transport pathway for mercury.
Jakob Lindaas, Delphine K. Farmer, Ilana B. Pollack, Andrew Abeleira, Frank Flocke, Rob Roscioli, Scott Herndon, and Emily V. Fischer
Atmos. Chem. Phys., 17, 10691–10707, https://doi.org/10.5194/acp-17-10691-2017, https://doi.org/10.5194/acp-17-10691-2017, 2017
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Wildfire smoke is becoming increasingly important for air quality in the US. We used measurements taken during the summer 2015 near Denver, CO, to provide a case study of how wildfire smoke can impact air quality, specifically ozone, which is harmful to humans. Wildfire smoke during this time period was associated with about 15 % more ozone than we would expect under normal conditions. This smoke came from fires in the Pacific Northwest and likely impacted much of the central and western US.
Jesse W. Greenslade, Simon P. Alexander, Robyn Schofield, Jenny A. Fisher, and Andrew K. Klekociuk
Atmos. Chem. Phys., 17, 10269–10290, https://doi.org/10.5194/acp-17-10269-2017, https://doi.org/10.5194/acp-17-10269-2017, 2017
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An analysis of data from ozonesondes released at three southern oceanic sites shows the impact of stratospheric ozone in this region. Using a novel method of transport classification, this work estimates the seasonality and quantity of stratospherically sourced ozone. We find that ozone is transported most frequently in summer due to regional-scale low-pressure weather systems. We also estimate a stratospheric ozone source of 2.0–3.3 Tg/year over three Southern Ocean regions.
Carlena J. Ebben, Tamara L. Sparks, Paul J. Wooldridge, Teresa L. Campos, Christopher A. Cantrell, Roy L. Mauldin, Andrew J. Weinheimer, and Ronald C. Cohen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-671, https://doi.org/10.5194/acp-2017-671, 2017
Revised manuscript has not been submitted
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We use observations from the FRAPPÉ campaign to examine the evolution of reactive nitrogen as it is transported from Denver. We provide estimates for dilution rates, chemical lifetimes, and deposition rates. While dilution is the primary loss process in the immediate outflow from Denver, chemically, a majority of NOx is converted to HNO3 and is subsequently deposited. Understanding the evolution of reactive nitrogen informs how urban emissions affect air quality in the surrounding regions.
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.
Karen E. Cady-Pereira, Vivienne H. Payne, Jessica L. Neu, Kevin W. Bowman, Kazuyuki Miyazaki, Eloise A. Marais, Susan Kulawik, Zitely A. Tzompa-Sosa, and Jennifer D. Hegarty
Atmos. Chem. Phys., 17, 9379–9398, https://doi.org/10.5194/acp-17-9379-2017, https://doi.org/10.5194/acp-17-9379-2017, 2017
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Air quality is a major issue for megacities. Our paper looks at satellite measurements over Mexico City and Lagos of several trace gases gases related to air quality to determine the temporal and spatial variability of these gases, and it relates this variability to local conditions, such as topography, winds and biomass burning events. We find that, while Mexico City is known for severe pollution events, the levels of of pollution in Lagos are much higher and more persistent.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
Preprint retracted
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
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.
Camille Viatte, Thomas Lauvaux, Jacob K. Hedelius, Harrison Parker, Jia Chen, Taylor Jones, Jonathan E. Franklin, Aijun J. Deng, Brian Gaudet, Kristal Verhulst, Riley Duren, Debra Wunch, Coleen Roehl, Manvendra K. Dubey, Steve Wofsy, and Paul O. Wennberg
Atmos. Chem. Phys., 17, 7509–7528, https://doi.org/10.5194/acp-17-7509-2017, https://doi.org/10.5194/acp-17-7509-2017, 2017
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This study estimates methane emissions at local scale in dairy farms using four new mobile ground-based remote sensing spectrometers (EM27/SUN) and isotopic in situ measurements. Our top-down estimates are in the low end of previous studies. Inverse modeling from a comprehensive high-resolution model simulations (WRF-LES) is used to assess the geographical distribution of the emissions. Both the model and the measurements indicate a mixture of anthropogenic and biogenic emissions.
Xueling Liu, Arthur P. Mizzi, Jeffrey L. Anderson, Inez Y. Fung, and Ronald C. Cohen
Atmos. Chem. Phys., 17, 7067–7081, https://doi.org/10.5194/acp-17-7067-2017, https://doi.org/10.5194/acp-17-7067-2017, 2017
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We describe a chemical ensemble data assimilation system with high spatial and temporal resolution that simultaneously adjusts meteorological and chemical variables and NOx emissions. We investigate the sensitivity of emission inversions to the accuracy and uncertainty of the wind analyses and the emission update scheme. The results provide insight into optimal uses of the observations from future geostationary satellite missions that will observe atmospheric composition.
Debra Wunch, Paul O. Wennberg, Gregory Osterman, Brendan Fisher, Bret Naylor, Coleen M. Roehl, Christopher O'Dell, Lukas Mandrake, Camille Viatte, Matthäus Kiel, David W. T. Griffith, Nicholas M. Deutscher, Voltaire A. Velazco, Justus Notholt, Thorsten Warneke, Christof Petri, Martine De Maziere, Mahesh K. Sha, Ralf Sussmann, Markus Rettinger, David Pollard, John Robinson, Isamu Morino, Osamu Uchino, Frank Hase, Thomas Blumenstock, Dietrich G. Feist, Sabrina G. Arnold, Kimberly Strong, Joseph Mendonca, Rigel Kivi, Pauli Heikkinen, Laura Iraci, James Podolske, Patrick W. Hillyard, Shuji Kawakami, Manvendra K. Dubey, Harrison A. Parker, Eliezer Sepulveda, Omaira E. García, Yao Te, Pascal Jeseck, Michael R. Gunson, David Crisp, and Annmarie Eldering
Atmos. Meas. Tech., 10, 2209–2238, https://doi.org/10.5194/amt-10-2209-2017, https://doi.org/10.5194/amt-10-2209-2017, 2017
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This paper describes the comparisons between NASA's Orbiting Carbon Observatory (OCO-2) column-averaged dry-air mole fractions of CO2 with its primary ground-based validation network, the Total Carbon Column Observing Network (TCCON). The paper shows that while the standard bias correction reduces much of the spurious variability in the satellite measurements, residual biases remain.
A. Anthony Bloom, Kevin W. Bowman, Meemong Lee, Alexander J. Turner, Ronny Schroeder, John R. Worden, Richard Weidner, Kyle C. McDonald, and Daniel J. Jacob
Geosci. Model Dev., 10, 2141–2156, https://doi.org/10.5194/gmd-10-2141-2017, https://doi.org/10.5194/gmd-10-2141-2017, 2017
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Wetland emissions are a principal source of uncertainty in the global atmospheric methane budget due to poor knowledge of wetland processes. We construct a wetland methane emission and uncertainty dataset for use in global atmospheric methane models. Our wetland model ensemble is based on static wetland maps, satellite-derived inundation and carbon cycle models. The ensemble performs favourably against regional flux estimates and atmospheric methane measurements relative to previous studies.
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.
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Jacob K. Hedelius, Harrison Parker, Debra Wunch, Coleen M. Roehl, Camille Viatte, Sally Newman, Geoffrey C. Toon, James R. Podolske, Patrick W. Hillyard, Laura T. Iraci, Manvendra K. Dubey, and Paul O. Wennberg
Atmos. Meas. Tech., 10, 1481–1493, https://doi.org/10.5194/amt-10-1481-2017, https://doi.org/10.5194/amt-10-1481-2017, 2017
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Two portable spectrometers, assumed to be internally precise, were taken to four different sites with (stationary) TCCON spectrometers. Biases of column averaged CO2 and CH4 measured among the TCCON sites were estimated experimentally. Results suggest that maximum (95 % confidence interval) bias among sites is less than what was estimated from a previous analytical error analysis.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
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.
Rebecca H. Schwantes, Katherine A. Schilling, Renee C. McVay, Hanna Lignell, Matthew M. Coggon, Xuan Zhang, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 17, 3453–3474, https://doi.org/10.5194/acp-17-3453-2017, https://doi.org/10.5194/acp-17-3453-2017, 2017
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Toluene, one of the principle aromatic compounds present in the atmosphere, is oxidized by OH to produce cresol and other products. Here later-generation low-volatility oxygenated products from cresol oxidation by OH are detected in the gas and particle phases. This work identifies a simple and significant mechanism for toluene secondary organic aerosol formation through the cresol pathway. Likely the phenolic pathway of other aromatic compounds is also important for secondary organic aerosol.
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.
Sebastian D. Eastham and Daniel J. Jacob
Atmos. Chem. Phys., 17, 2543–2553, https://doi.org/10.5194/acp-17-2543-2017, https://doi.org/10.5194/acp-17-2543-2017, 2017
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Intercontinental atmospheric transport can disrupt local chemistry and cause air quality issues thousands of kilometers from the source, complicating correct attribution of air quality exceedances. This transport occurs in long, thin plumes which current-generation models consistently fail to reproduce. Our study investigates the cause of this failure, finding that greater vertical resolution than is currently available is required to reliably resolve the plumes and their effects.
Zhao-Cheng Zeng, Qiong Zhang, Vijay Natraj, Jack S. Margolis, Run-Lie Shia, Sally Newman, Dejian Fu, Thomas J. Pongetti, Kam W. Wong, Stanley P. Sander, Paul O. Wennberg, and Yuk L. Yung
Atmos. Chem. Phys., 17, 2495–2508, https://doi.org/10.5194/acp-17-2495-2017, https://doi.org/10.5194/acp-17-2495-2017, 2017
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We propose a novel approach to describing the scattering effects of atmospheric aerosols using H2O retrievals in the near infrared. We found that the aerosol scattering effect is the primary contributor to the variations in the wavelength dependence of the H2O SCD retrievals and the scattering effects can be derived using H2O retrievals from multiple bands. This proposed method could potentially contribute towards reducing biases in greenhouse gas retrievals from space.
Annmarie Eldering, Chris W. O'Dell, Paul O. Wennberg, David Crisp, Michael R. Gunson, Camille Viatte, Charles Avis, Amy Braverman, Rebecca Castano, Albert Chang, Lars Chapsky, Cecilia Cheng, Brian Connor, Lan Dang, Gary Doran, Brendan Fisher, Christian Frankenberg, Dejian Fu, Robert Granat, Jonathan Hobbs, Richard A. M. Lee, Lukas Mandrake, James McDuffie, Charles E. Miller, Vicky Myers, Vijay Natraj, Denis O'Brien, Gregory B. Osterman, Fabiano Oyafuso, Vivienne H. Payne, Harold R. Pollock, Igor Polonsky, Coleen M. Roehl, Robert Rosenberg, Florian Schwandner, Mike Smyth, Vivian Tang, Thomas E. Taylor, Cathy To, Debra Wunch, and Jan Yoshimizu
Atmos. Meas. Tech., 10, 549–563, https://doi.org/10.5194/amt-10-549-2017, https://doi.org/10.5194/amt-10-549-2017, 2017
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This paper describes the measurements of atmospheric carbon dioxide collected in the first 18 months of the satellite mission known as the Orbiting Carbon Observatory-2 (OCO-2). The paper shows maps of the carbon dioxide data, data density, and other data fields that illustrate the data quality. This mission has collected a more precise, more dense dataset of carbon dioxide then we have ever had previously.
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.
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.
David Crisp, Harold R. Pollock, Robert Rosenberg, Lars Chapsky, Richard A. M. Lee, Fabiano A. Oyafuso, Christian Frankenberg, Christopher W. O'Dell, Carol J. Bruegge, Gary B. Doran, Annmarie Eldering, Brendan M. Fisher, Dejian Fu, Michael R. Gunson, Lukas Mandrake, Gregory B. Osterman, Florian M. Schwandner, Kang Sun, Tommy E. Taylor, Paul O. Wennberg, and Debra Wunch
Atmos. Meas. Tech., 10, 59–81, https://doi.org/10.5194/amt-10-59-2017, https://doi.org/10.5194/amt-10-59-2017, 2017
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The Orbiting Carbon Observatory-2 carries and points a three-channel imaging grating spectrometer designed to collect high-resolution spectra of reflected sunlight within the molecular oxygen A-band at 0.765 microns and the carbon dioxide bands at 1.61 and 2.06 microns. Here, we describe the OCO-2 instrument, its data products, and its performance during its first 18 months in orbit.
Joshua L. Laughner, Azimeh Zare, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 15247–15264, https://doi.org/10.5194/acp-16-15247-2016, https://doi.org/10.5194/acp-16-15247-2016, 2016
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Satellite measurements of the atmosphere provide global information on pollutants that play an important role in air quality. These measurements require assumed knowledge about the vertical profile of these pollutants, which are often simulated at coarse resolution in space and time. We find that simulating these inputs with better spatial and temporal resolution alters individual measurements by up to 40 % and the average measurement by up to 13 %, and increases derived emissions by up to 100 %.
Daniel J. Jacob, Alexander J. Turner, Joannes D. Maasakkers, Jianxiong Sheng, Kang Sun, Xiong Liu, Kelly Chance, Ilse Aben, Jason McKeever, and Christian Frankenberg
Atmos. Chem. Phys., 16, 14371–14396, https://doi.org/10.5194/acp-16-14371-2016, https://doi.org/10.5194/acp-16-14371-2016, 2016
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Methane is a greenhouse gas emitted by a range of natural and anthropogenic sources. Atmospheric methane has been measured continuously from space since 2003, and new instruments are planned to launch in the near future that will greatly expand the capabilities of space-based observations. We review the value of current, future, and proposed satellite observations to better quantify methane emissions from the global scale down to the scale of point sources.
Debra Wunch, Geoffrey C. Toon, Jacob K. Hedelius, Nicholas Vizenor, Coleen M. Roehl, Katherine M. Saad, Jean-François L. Blavier, Donald R. Blake, and Paul O. Wennberg
Atmos. Chem. Phys., 16, 14091–14105, https://doi.org/10.5194/acp-16-14091-2016, https://doi.org/10.5194/acp-16-14091-2016, 2016
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This paper investigates the cause of the known underestimate of bottom-up inventories of methane in California's South Coast Air Basin (SoCAB). We use total column measurements of methane, ethane, carbon monoxide, and other trace gases beginning in the late 1980s to calculate emissions and attribute sources of excess methane to the atmosphere. We conclude that more than half of the excess methane to the SoCAB atmosphere is attributable to processed natural gas.
Katherine M. Saad, Debra Wunch, Nicholas M. Deutscher, David W. T. Griffith, Frank Hase, Martine De Mazière, Justus Notholt, David F. Pollard, Coleen M. Roehl, Matthias Schneider, Ralf Sussmann, Thorsten Warneke, and Paul O. Wennberg
Atmos. Chem. Phys., 16, 14003–14024, https://doi.org/10.5194/acp-16-14003-2016, https://doi.org/10.5194/acp-16-14003-2016, 2016
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Current approaches to constrain the global methane budget assimilate total column measurements into models, but model biases can impact results. We use tropospheric methane columns to evaluate model transport errors and identify a seasonal time lag in the Northern Hemisphere troposphere masked by stratospheric compensating effects. We find systematic biases in the stratosphere will alias into model-derived emissions estimates, especially those in the high Northern latitudes that vary seasonally.
Lei Zhu, Daniel J. Jacob, Patrick S. Kim, Jenny A. Fisher, Karen Yu, Katherine R. Travis, Loretta J. Mickley, Robert M. Yantosca, Melissa P. Sulprizio, Isabelle De Smedt, Gonzalo González Abad, Kelly Chance, Can Li, Richard Ferrare, Alan Fried, Johnathan W. Hair, Thomas F. Hanisco, Dirk Richter, Amy Jo Scarino, James Walega, Petter Weibring, and Glenn M. Wolfe
Atmos. Chem. Phys., 16, 13477–13490, https://doi.org/10.5194/acp-16-13477-2016, https://doi.org/10.5194/acp-16-13477-2016, 2016
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HCHO column data are widely used as a proxy for VOCs emissions, but validation of the data has been extremely limited. We use accurate aircraft observations to validate and intercompare 6 HCHO retrievals with GEOS-Chem as the intercomparison platform. Retrievals are interconsistent in spatial variability over the SE US and in daily variability, but are biased low by 20–51 %. Our work supports the use of HCHO column as a quantitative proxy for isoprene emission after correction of the low bias.
Alexander J. Turner, Alexis A. Shusterman, Brian C. McDonald, Virginia Teige, Robert A. Harley, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 13465–13475, https://doi.org/10.5194/acp-16-13465-2016, https://doi.org/10.5194/acp-16-13465-2016, 2016
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Our paper investigates the ability of different types of observational networks to estimate urban CO2 emissions. We have quantified the trade-off between precision and network density for estimating urban greenhouse gas emissions. Our results show that different observing systems may fall into noise- or site-limited regimes where reducing the uncertainty in the estimated emissions is governed by a single factor.
Alexis A. Shusterman, Virginia E. Teige, Alexander J. Turner, Catherine Newman, Jinsol Kim, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 13449–13463, https://doi.org/10.5194/acp-16-13449-2016, https://doi.org/10.5194/acp-16-13449-2016, 2016
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We describe the design of and first results from the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of 28 CO2 sensors stationed across and around the city of Oakland, California at ~ 2 km intervals. We evaluate the network via 4 performance parameters (cost, reliability, precision, systematic uncertainty) and find this high density technique to be sufficiently cost-effective and rigorous to inform understanding of small-scale urban emissions relevant to climate regulation.
Gerard Ancellet, Nikos Daskalakis, Jean Christophe Raut, David Tarasick, Jonathan Hair, Boris Quennehen, François Ravetta, Hans Schlager, Andrew J. Weinheimer, Anne M. Thompson, Bryan Johnson, Jennie L. Thomas, and Katharine S. Law
Atmos. Chem. Phys., 16, 13341–13358, https://doi.org/10.5194/acp-16-13341-2016, https://doi.org/10.5194/acp-16-13341-2016, 2016
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An integrated analysis of all the ozone observations (lidar, sondes, and airborne in situ measurements) conducted during the 2008 IPY campaigns is performed and the processes that determine summer ozone concentrations over Greenland and Canada are discussed. Combined with a regional model simulation (WRFChem), the analysis of ozone, CO, and PV latitudinal and vertical variability allows the determination of the influence of stratospheric sources and biomass burning and anthropogenic emissions.
Luke D. Schiferl, Colette L. Heald, Martin Van Damme, Lieven Clarisse, Cathy Clerbaux, Pierre-François Coheur, John B. Nowak, J. Andrew Neuman, Scott C. Herndon, Joseph R. Roscioli, and Scott J. Eilerman
Atmos. Chem. Phys., 16, 12305–12328, https://doi.org/10.5194/acp-16-12305-2016, https://doi.org/10.5194/acp-16-12305-2016, 2016
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This study combines new observations and a simulation to assess the interannual variability of atmospheric ammonia concentrations over the United States. The model generally underrepresents the observed variability. Nearly two-thirds of the simulated variability is caused by meteorology, twice that caused by regulations on fossil fuel combustion emissions. Adding ammonia emissions variability does not substantially improve the simulation and has little impact on summer particle concentrations.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Glenn M. Wolfe, Margaret R. Marvin, Sandra J. Roberts, Katherine R. Travis, and Jin Liao
Geosci. Model Dev., 9, 3309–3319, https://doi.org/10.5194/gmd-9-3309-2016, https://doi.org/10.5194/gmd-9-3309-2016, 2016
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The Framework for 0-D Atmospheric Modeling (F0AM) is a new, user-friendly platform for simulation of atmospheric chemistry systems. It incorporates a suite of commonly used mechanisms and is adaptable to photochemical chambers, Lagrangian plumes, and steady-state or time-varying diurnal cycles. We provide a detailed model description, demonstrate several common applications, and highlight some of the advantages and challenges of the 0-D box modeling approach.
Jason M. St. Clair, Jean C. Rivera-Rios, John D. Crounse, Eric Praske, Michelle J. Kim, Glenn M. Wolfe, Frank N. Keutsch, Paul O. Wennberg, and Thomas F. Hanisco
Atmos. Meas. Tech., 9, 4561–4568, https://doi.org/10.5194/amt-9-4561-2016, https://doi.org/10.5194/amt-9-4561-2016, 2016
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Global isoprene emissions are the largest source of atmospheric non-methane hydrocarbons. Lab results show that ISOPOOH, a low-NOx isoprene oxidation product, can decompose on instrument surfaces to form high-NOx isoprene oxidation products, causing misinterpretation of oxidation conditions. This study investigated the potential formaldehyde artifact from ISOPOOH for the NASA ISAF instrument, and found that it does not significantly affect the accuracy of the ISAF field measurements.
Jacob K. Hedelius, Camille Viatte, Debra Wunch, Coleen M. Roehl, Geoffrey C. Toon, Jia Chen, Taylor Jones, Steven C. Wofsy, Jonathan E. Franklin, Harrison Parker, Manvendra K. Dubey, and Paul O. Wennberg
Atmos. Meas. Tech., 9, 3527–3546, https://doi.org/10.5194/amt-9-3527-2016, https://doi.org/10.5194/amt-9-3527-2016, 2016
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Portable FTS instruments with lower resolution are being used to measure gases (including CO2, CH4, CO, and N2O) in the atmosphere. We compared measurements from four of these instruments for a few weeks, and with one for nearly a year to a higher resolution TCCON standard. We also performed tests to assess performance under different atmospheric and instrumental conditions. We noted consistent offsets in the short-term (~1 month); more research is still needed to assess precision longer term.
Brian J. Connor, Vanessa Sherlock, Geoff Toon, Debra Wunch, and Paul O. Wennberg
Atmos. Meas. Tech., 9, 3513–3525, https://doi.org/10.5194/amt-9-3513-2016, https://doi.org/10.5194/amt-9-3513-2016, 2016
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An algorithm for retrieval of vertical profiles of CO2 from ground-based spectra is described. Retrieval of CO2 vertical profiles from would be very beneficial for carbon cycle studies and the validation of satellite measurements. There are approximately 3 degrees of freedom for the CO2 profile. The accuracy of retrievals of CO2 from the spectral band used is limited by small errors in the calculated spectrum. Ongoing research is needed and described.
Makoto Inoue, Isamu Morino, Osamu Uchino, Takahiro Nakatsuru, Yukio Yoshida, Tatsuya Yokota, Debra Wunch, Paul O. Wennberg, Coleen M. Roehl, David W. T. Griffith, Voltaire A. Velazco, Nicholas M. Deutscher, Thorsten Warneke, Justus Notholt, John Robinson, Vanessa Sherlock, Frank Hase, Thomas Blumenstock, Markus Rettinger, Ralf Sussmann, Esko Kyrö, Rigel Kivi, Kei Shiomi, Shuji Kawakami, Martine De Mazière, Sabrina G. Arnold, Dietrich G. Feist, Erica A. Barrow, James Barney, Manvendra Dubey, Matthias Schneider, Laura T. Iraci, James R. Podolske, Patrick W. Hillyard, Toshinobu Machida, Yousuke Sawa, Kazuhiro Tsuboi, Hidekazu Matsueda, Colm Sweeney, Pieter P. Tans, Arlyn E. Andrews, Sebastien C. Biraud, Yukio Fukuyama, Jasna V. Pittman, Eric A. Kort, and Tomoaki Tanaka
Atmos. Meas. Tech., 9, 3491–3512, https://doi.org/10.5194/amt-9-3491-2016, https://doi.org/10.5194/amt-9-3491-2016, 2016
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In this study, we correct the biases of GOSAT XCO2 and XCH4 using TCCON data. To evaluate the effectiveness of our correction method, uncorrected/corrected GOSAT data are compared to independent XCO2 and XCH4 data derived from aircraft measurements. Consequently, we suggest that this method is effective for reducing the biases of the GOSAT data. We consider that our work provides GOSAT data users with valuable information and contributes to the further development of studies on greenhouse gases.
Matthew J. Alvarado, Chantelle R. Lonsdale, Helen L. Macintyre, Huisheng Bian, Mian Chin, David A. Ridley, Colette L. Heald, Kenneth L. Thornhill, Bruce E. Anderson, Michael J. Cubison, Jose L. Jimenez, Yutaka Kondo, Lokesh K. Sahu, Jack E. Dibb, and Chien Wang
Atmos. Chem. Phys., 16, 9435–9455, https://doi.org/10.5194/acp-16-9435-2016, https://doi.org/10.5194/acp-16-9435-2016, 2016
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Understanding the scattering and absorption of light by aerosols is necessary for understanding air quality and climate change. We used data from the 2008 ARCTAS campaign to evaluate aerosol optical property models using a closure methodology that separates errors in these models from other errors in aerosol emissions, chemistry, or transport. We find that the models on average perform reasonably well, and make suggestions for how remaining biases could be reduced.
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.
Jia Chen, Camille Viatte, Jacob K. Hedelius, Taylor Jones, Jonathan E. Franklin, Harrison Parker, Elaine W. Gottlieb, Paul O. Wennberg, Manvendra K. Dubey, and Steven C. Wofsy
Atmos. Chem. Phys., 16, 8479–8498, https://doi.org/10.5194/acp-16-8479-2016, https://doi.org/10.5194/acp-16-8479-2016, 2016
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This paper helps establish a range of new applications for compact solar-tracking Fourier transform spectrometers, and shows the capability of differential column measurements for determining urban emissions. By accurately measuring the differences in the integrated column amounts of carbon dioxide and methane across local and regional sources in California, we directly observe the mass loading of the atmosphere due to the influence of emissions in the intervening locale.
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.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Hongyu Liu, David B. Considine, Larry W. Horowitz, James H. Crawford, Jose M. Rodriguez, Susan E. Strahan, Megan R. Damon, Stephen D. Steenrod, Xiaojing Xu, Jules Kouatchou, Claire Carouge, and Robert M. Yantosca
Atmos. Chem. Phys., 16, 4641–4659, https://doi.org/10.5194/acp-16-4641-2016, https://doi.org/10.5194/acp-16-4641-2016, 2016
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We assess the utility of cosmogenic beryllium-7, a natural aerosol tracer, for evaluating cross-tropopause transport in global models. We show that model excessive cross-tropopause transport of beryllium-7 corresponds to overestimated stratospheric contribution to tropospheric ozone. We conclude that the observational constraints for beryllium-7 and observed beryllium-7 total deposition fluxes can be used routinely as a first-order assessment of cross-tropopause transport in global models.
Christopher Chan Miller, Daniel J. Jacob, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 16, 4631–4639, https://doi.org/10.5194/acp-16-4631-2016, https://doi.org/10.5194/acp-16-4631-2016, 2016
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Volatile organic compounds (VOCs) are important precursors for photochemical smog.
Glyoxal is an organic compound produced in the atmosphere from reactions of larger VOCs. OMI satellite observations of glyoxal show a large hotspot over the Pearl River delta. The hotspot can be explained by industrial paint and solvent emissions of aromatic VOCs. Our work shows OMI observations are consistent with current VOC emissions estimates, whereas previous work has suggested large underestimates.
Karen Yu, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Christopher C. Miller, Katherine R. Travis, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Ron C. Cohen, Jack E. Dibb, Alan Fried, Tomas Mikoviny, Thomas B. Ryerson, Paul O. Wennberg, and Armin Wisthaler
Atmos. Chem. Phys., 16, 4369–4378, https://doi.org/10.5194/acp-16-4369-2016, https://doi.org/10.5194/acp-16-4369-2016, 2016
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Increasing the spatial resolution of a chemical transport model may improve simulations but can be computationally expensive. Using observations from the SEAC4RS aircraft campaign, we find that at higher spatial resolutions, models are better able to simulate the chemical pathways of ozone precursors, but the overall effect on regional mean concentrations is small. This implies that for continental boundary layer applications, coarse resolution models are adequate.
Bruno Franco, Eloise A. Marais, Benoît Bovy, Whitney Bader, Bernard Lejeune, Ginette Roland, Christian Servais, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 4171–4189, https://doi.org/10.5194/acp-16-4171-2016, https://doi.org/10.5194/acp-16-4171-2016, 2016
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The long-term evolution of HCHO in the remote troposphere is characterized using a 27-year time series of total columns from high-resolution FTIR solar spectra recorded at Jungfraujoch. A parametric model is used to remove the effect of the HCHO diurnal variations for improving the trend determination and the comparison with columns simulated by GEOS-Chem. Sensitivity tests are performed to identify the main drivers of the HCHO seasonal and inter-annual variations, as well as their contribution.
Renee C. McVay, Xuan Zhang, Bernard Aumont, Richard Valorso, Marie Camredon, Yuyi S. La, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 16, 2785–2802, https://doi.org/10.5194/acp-16-2785-2016, https://doi.org/10.5194/acp-16-2785-2016, 2016
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Short summary
Secondary organic aerosol (SOA) affects climate change, human health, and cloud formation. We examine SOA formation from the biogenic hydrocarbon α-pinene and observe unexpected experimental results that run contrary to model predictions. Various processes are explored via modeling to rationalize the observations. The paper identifies the importance of further constraining via experiments various steps in the chemical mechanism in order to accurately predict SOA worldwide.
S. E. Pusede, K. C. Duffey, A. A. Shusterman, A. Saleh, J. L. Laughner, P. J. Wooldridge, Q. Zhang, C. L. Parworth, H. Kim, S. L. Capps, L. C. Valin, C. D. Cappa, A. Fried, J. Walega, J. B. Nowak, A. J. Weinheimer, R. M. Hoff, T. A. Berkoff, A. J. Beyersdorf, J. Olson, J. H. Crawford, and R. C. Cohen
Atmos. Chem. Phys., 16, 2575–2596, https://doi.org/10.5194/acp-16-2575-2016, https://doi.org/10.5194/acp-16-2575-2016, 2016
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
Susan Kulawik, Debra Wunch, Christopher O'Dell, Christian Frankenberg, Maximilian Reuter, Tomohiro Oda, Frederic Chevallier, Vanessa Sherlock, Michael Buchwitz, Greg Osterman, Charles E. Miller, Paul O. Wennberg, David Griffith, Isamu Morino, Manvendra K. Dubey, Nicholas M. Deutscher, Justus Notholt, Frank Hase, Thorsten Warneke, Ralf Sussmann, John Robinson, Kimberly Strong, Matthias Schneider, Martine De Mazière, Kei Shiomi, Dietrich G. Feist, Laura T. Iraci, and Joyce Wolf
Atmos. Meas. Tech., 9, 683–709, https://doi.org/10.5194/amt-9-683-2016, https://doi.org/10.5194/amt-9-683-2016, 2016
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To accurately estimate source and sink locations of carbon dioxide, systematic errors in satellite measurements and models must be characterized. This paper examines two satellite data sets (GOSAT, launched 2009, and SCIAMACHY, launched 2002), and two models (CarbonTracker and MACC) vs. the TCCON CO2 validation data set. We assess biases and errors by season and latitude, satellite performance under averaging, and diurnal variability. Our findings are useful for assimilation of satellite data.
M. Kiel, D. Wunch, P. O. Wennberg, G. C. Toon, F. Hase, and T. Blumenstock
Atmos. Meas. Tech., 9, 669–682, https://doi.org/10.5194/amt-9-669-2016, https://doi.org/10.5194/amt-9-669-2016, 2016
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fis