Articles | Volume 17, issue 17
Research article 01 Sep 2017
Research article | 01 Sep 2017
Stratospheric ozone intrusion events and their impacts on tropospheric ozone in the Southern Hemisphere
Jesse W. Greenslade et al.
No articles found.
Camilla K. Crockart, Tessa R. Vance, Alexander D. Fraser, Nerilie J. Abram, Alison S. Criscitiello, Mark A. J. Curran, Vincent Favier, Ailie J. E. Gallant, Christoph Kittel, Helle A. Kjær, Andrew R. Klekociuk, Lenneke M. Jong, Andrew D. Moy, Christopher T. Plummer, Paul T. Vallelonga, Jonathan Wille, and Lingwei Zhang
Clim. Past, 17, 1795–1818,Short summary
We present preliminary analyses of the annual sea salt concentrations and snowfall accumulation in a new East Antarctic ice core, Mount Brown South. We compare this record with an updated Law Dome (Dome Summit South site) ice core record over the period 1975–2016. The Mount Brown South record preserves a stronger and inverse signal for the El Niño–Southern Oscillation (in austral winter and spring) compared to the Law Dome record (in summer).
Sonya Fiddes, Matthew Woodhouse, Steve Utembe, Robyn Schofield, Joel Alroe, Scott Chambers, Luke Cravigan, Erin Dunne, Ruhi Humphries, Graham Johnson, Melita Keywood, Todd Lane, Branka Miljevic, Yuko Omori, Zoran Ristovski, Paul Sellek, Hilton Swan, Hiroshi Tanimoto, Jason Ward, and Alister Williams
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
Coral reefs have been found to produce the climatically relevant chemical compound dimethyl sulfide (DMS). It has been suggested that corals can modify their environment via the production of DMS. We use an atmospheric-chemistry model to test this theory at a regional scale for the first time. We find that it is unlikely that coral reef derived DMS has an influence over local climate, in part due to their proximity to terrestrial and anthropogenic aerosol sources.
Beata Bukosa, Jenny Fisher, Nicholas Deutscher, and Dylan Jones
Geosci. Model Dev. Discuss.,
Preprint under review for GMDShort summary
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.,
Revised manuscript under review for GMDShort summary
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.
Sonya L. Fiddes, Matthew T. Woodhouse, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 21, 5883–5903,Short summary
Coral reefs are known to produce the aerosol precursor dimethyl sulfide (DMS). Currently, this source of coral DMS is unaccounted for in climate modelling, and the impact of coral reef extinction on aerosol and climate is unknown. In this study, we address this problem using a coupled chemistry–climate model for the first time. We find that coral reefs make a minimal contribution to the aerosol population and are unlikely to play a role in climate modulation.
Alexander D. Fraser, Robert A. Massom, Mark S. Handcock, Phillip Reid, Kay I. Ohshima, Marilyn N. Raphael, Jessica Cartwright, Andrew R. Klekociuk, Zhaohui Wang, and Richard Porter-Smith
The Cryosphere Discuss.,
Revised manuscript accepted for TCShort summary
Landfast ice is sea ice that remains stationary by attaching to Antarctica’s coastline and grounded icebergs. Although a variable feature, landfast ice exerts influence on key coastal processes involving pack ice, the ice sheet, ocean and atmosphere, and is of ecological importance. We present a first analysis of change in landfast-ice over an 18 y period, and quantify trends (−0.19 ± 0.18 %/year). This analysis forms a reference of landfast ice extent and variability for use in other studies.
Robert G. Ryan, Jeremy D. Silver, Richard Querel, Dan Smale, Steve Rhodes, Matt Tully, Nicholas Jones, and Robyn Schofield
Atmos. Meas. Tech., 13, 6501–6519,Short summary
Models have identified Australasia as a formaldehyde (HCHO) hotspot from vegetation sources, but few measurement studies exist to verify this. We compare, and find good agreement between, HCHO measurements using three – two ground-based and one satellite-based – different spectroscopic techniques in Australia and New Zealand. This gives confidence in using satellite observations to study HCHO and associated air chemistry and pollution problems in this under-studied part of the world.
William R. Hobbs, Andrew R. Klekociuk, and Yuhang Pan
Atmos. Chem. Phys., 20, 14757–14768,Short summary
Reanalysis products are an invaluable tool for representing variability and long-term trends in regions with limited in situ data. However, validation of these products is difficult because of that lack of station data. Here we present a novel assessment of eight reanalyses over the polar Southern Ocean, leveraging the close relationship between trends in sea ice cover and surface air temperature, that provides clear guidance on the most reliable product for Antarctic research.
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,Short summary
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.
W. John R. French, Andrew R. Klekociuk, and Frank J. Mulligan
Atmos. Chem. Phys., 20, 8691–8708,Short summary
We explore a quasi-quadrennial oscillation (QQO; 3–4 K amplitude, ~ 4-year period) in mesopause region temperatures observed in 24 years of hydroxyl airglow measurements over Davis, Antarctica (68° S, 78° E). Correlation and composite analysis using meteorological reanalysis and satellite data reveals complex patterns on the QQO timescale in both hemispheres. Modulation of the meridional circulation, linked to the propagation of gravity waves, plays a significant role in producing the QQO response.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss.,
Preprint withdrawnShort summary
In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
Peter Kuma, Adrian J. McDonald, Olaf Morgenstern, Simon P. Alexander, John J. Cassano, Sally Garrett, Jamie Halla, Sean Hartery, Mike J. Harvey, Simon Parsons, Graeme Plank, Vidya Varma, and Jonny Williams
Atmos. Chem. Phys., 20, 6607–6630,Short summary
We evaluate clouds over the Southern Ocean in the climate model HadGEM3 and reanalysis MERRA-2 using ship-based ceilometer and radiosonde observations. We find the models underestimate cloud cover by 18–25 %, with clouds below 2 km dominant in reality but lacking in the models. We find a strong link between clouds, atmospheric stability and sea surface temperature in observations but not in the models, implying that sub-grid processes do not generate enough cloud in response to these conditions.
W. John R. French, Frank J. Mulligan, and Andrew R. Klekociuk
Atmos. Chem. Phys., 20, 6379–6394,Short summary
In this study, we analyse 24 years of atmospheric temperatures from the mesopause region (~87 km altitude) derived from ground-based spectrometer observations of hydroxyl airglow at Davis station, Antarctica (68° S, 78° E). These data are used to quantify the effect of the solar cycle and the long-term trend due to increasing greenhouse gas emissions on the atmosphere at this level. A record-low winter-average temperature is reported for 2018 and comparisons are made with satellite observations.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877,Short summary
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.
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,Short summary
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.
Yuke Wang, Valerii Shulga, Gennadi Milinevsky, Aleksey Patoka, Oleksandr Evtushevsky, Andrew Klekociuk, Wei Han, Asen Grytsai, Dmitry Shulga, Valery Myshenko, and Oleksandr Antyufeyev
Atmos. Chem. Phys., 19, 10303–10317,Short summary
The major sudden stratospheric warming (SSW) dramatically changed atmospheric conditions. This event is accompanied by a sharp increase in the polar stratosphere temperature, zonal wind reverse, and strong changes in the polar mesosphere. These changes affect even the midlatitude mesosphere, which is not widely covered by observations. Our newly installed microwave radiometer allowed for studying mesospheric zonal wind and CO variations to understand the SSW 2018 effects at midlatitudes.
Beata Bukosa, Nicholas M. Deutscher, Jenny A. Fisher, Dagmar Kubistin, Clare Paton-Walsh, and David W. T. Griffith
Atmos. Chem. Phys., 19, 7055–7072,Short summary
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.
Huang Yang, Darryn W. Waugh, Clara Orbe, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, Patrick Jöckel, Susan E. Strahan, Kane A. Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 5511–5528,Short summary
We evaluate the performance of a suite of models in simulating the large-scale transport from the northern midlatitudes to the Arctic using a CO-like idealized tracer. We find a large multi-model spread of the Arctic concentration of this CO-like tracer that is well correlated with the differences in the location of the midlatitude jet as well as the northern Hadley Cell edge. Our results suggest the Hadley Cell is key and zonal-mean transport by surface meridional flow needs better constraint.
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,Short summary
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.
Roland Eichinger, Simone Dietmüller, Hella Garny, Petr Šácha, Thomas Birner, Harald Bönisch, Giovanni Pitari, Daniele Visioni, Andrea Stenke, Eugene Rozanov, Laura Revell, David A. Plummer, Patrick Jöckel, Luke Oman, Makoto Deushi, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 921–940,Short summary
To shed more light upon the changes in stratospheric circulation in the 21st century, climate projection simulations of 10 state-of-the-art global climate models, spanning from 1960 to 2100, are analyzed. The study shows that in addition to changes in transport, mixing also plays an important role in stratospheric circulation and that the properties of mixing vary over time. Furthermore, the influence of mixing is quantified and a dynamical framework is provided to understand the changes.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172,Short summary
Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Robert G. Ryan, Steve Rhodes, Matthew Tully, Stephen Wilson, Nicholas Jones, Udo Frieß, and Robyn Schofield
Atmos. Chem. Phys., 18, 13969–13985,Short summary
Nitrous acid (HONO) plays a crucial role in the self-cleansing capacity of the atmosphere but its formation mechanisms and spatial distributions are not well understood. This paper presents spectroscopic measurements of HONO, NO2 and aerosol measurements from Melbourne, Australia. HONO levels are at a maximum in the middle of the day, which is unprecedented for an urban area, and these measurements provide evidence for the existence of a strong ground-based, daytime nitrogen oxide source.
Blanca Ayarzagüena, Lorenzo M. Polvani, Ulrike Langematz, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Dameris, Makoto Deushi, Steven C. Hardiman, Patrick Jöckel, Andrew Klekociuk, Marion Marchand, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, David A. Plummer, Laura Revell, Eugene Rozanov, David Saint-Martin, John Scinocca, Andrea Stenke, Kane Stone, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Atmos. Chem. Phys., 18, 11277–11287,Short summary
Stratospheric sudden warmings (SSWs) are natural major disruptions of the polar stratospheric circulation that also affect surface weather. In the literature there are conflicting claims as to whether SSWs will change in the future. The confusion comes from studies using different models and methods. Here we settle the question by analysing 12 models with a consistent methodology, to show that no robust changes in frequency and other features are expected over the 21st century.
Sonya L. Fiddes, Matthew T. Woodhouse, Zebedee Nicholls, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 18, 10177–10198,Short summary
The role of natural aerosol in the climate system is uncertain. A key contributor to marine aerosol is dimethyl sulfide (DMS), released by phytoplankton in the oceans. We study the effect of DMS on clouds and rain using a climate model with a detailed aerosol scheme. We show that DMS acts to reduce rainfall in cloud deck regions, leading to longer lived clouds and a large impact on solar energy reaching the surface. Further study of these areas will improve future climate projections.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438,Short summary
We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Clara Orbe, Huang Yang, Darryn W. Waugh, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, John F. Scinocca, Beatrice Josse, Virginie Marecal, Patrick Jöckel, Luke D. Oman, Susan E. Strahan, Makoto Deushi, Taichu Y. Tanaka, Kohei Yoshida, Hideharu Akiyoshi, Yousuke Yamashita, Andreas Stenke, Laura Revell, Timofei Sukhodolov, Eugene Rozanov, Giovanni Pitari, Daniele Visioni, Kane A. Stone, Robyn Schofield, and Antara Banerjee
Atmos. Chem. Phys., 18, 7217–7235,Short summary
In this study we compare a few atmospheric transport properties among several numerical models that are used to study the influence of atmospheric chemistry on climate. We show that there are large differences among models in terms of the timescales that connect the Northern Hemisphere midlatitudes, where greenhouse gases and ozone-depleting substances are emitted, to the Southern Hemisphere. Our results may have important implications for how models represent atmospheric composition.
Simone Dietmüller, Roland Eichinger, Hella Garny, Thomas Birner, Harald Boenisch, Giovanni Pitari, Eva Mancini, Daniele Visioni, Andrea Stenke, Laura Revell, Eugene Rozanov, David A. Plummer, John Scinocca, Patrick Jöckel, Luke Oman, Makoto Deushi, Shibata Kiyotaka, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 18, 6699–6720,
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,Short summary
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.
Olaf Morgenstern, Kane A. Stone, Robyn Schofield, Hideharu Akiyoshi, Yousuke Yamashita, Douglas E. Kinnison, Rolando R. Garcia, Kengo Sudo, David A. Plummer, John Scinocca, Luke D. Oman, Michael E. Manyin, Guang Zeng, Eugene Rozanov, Andrea Stenke, Laura E. Revell, Giovanni Pitari, Eva Mancini, Glauco Di Genova, Daniele Visioni, Sandip S. Dhomse, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 1091–1114,Short summary
We assess how ozone as simulated by a group of chemistry–climate models responds to variations in man-made climate gases and ozone-depleting substances. We find some agreement, particularly in the middle and upper stratosphere, but also considerable disagreement elsewhere. Such disagreement affects the reliability of future ozone projections based on these models, and also constitutes a source of uncertainty in climate projections using prescribed ozone derived from these simulations.
Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144,Short summary
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,Short summary
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.
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,Short summary
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.
Chris S.~M. Turney, Andrew Klekociuk, Christopher J. Fogwill, Violette Zunz, Hugues Goosse, Claire L. Parkinson, Gilbert Compo, Matthew Lazzara, Linda Keller, Rob Allan, Jonathan G. Palmer, Graeme Clark, and Ezequiel Marzinelli
The Cryosphere Discuss.,
Revised manuscript not acceptedShort summary
We demonstrate that a mid-twentieth century decrease in geopotential height in the southwest Pacific marks a Rossby wave response to equatorial Pacific warming, leading to enhanced easterly airflow off George V Land. Our results suggest that in contrast to ozone hole-driven changes in the Amundsen Sea, the 1979–2015 increase in sea ice extent off George V Land may be in response to reduced northward Ekman drift and enhanced (near-coast) production as a consequence of low latitude forcing.
Iain M. Reid, Andrew J. Spargo, Jonathan M. Woithe, Andrew R. Klekociuk, Joel P. Younger, and Gulamabas G. Sivjee
Ann. Geophys., 35, 567–582,Short summary
We measured temperatures in the atmosphere at heights near 90 km using nightglow emissions and compared them with satellite measurements and with measurements made with a meteor radar. We found good agreement between the techniques, which improved when we used the meteor radar and satellite data to measure densities at two heights separated by about 10 km to estimate the nightglow emission height.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671,Short summary
We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Asen Grytsai, Andrew Klekociuk, Gennadi Milinevsky, Oleksandr Evtushevsky, and Kane Stone
Atmos. Chem. Phys., 17, 1741–1758,Short summary
Twenty years ago we discovered that the ozone hole shape is asymmetric. This asymmetry is minimum over the Weddell Sea region and maximum over the Ross Sea area. Later we detected that the position of the ozone minimum is shifting east. We have continued to follow this event, and a couple years ago we revealed that the shift is slowing down and starting to move back. We connect all this movement with ozone hole increase; since 2000 the ozone layer has been stabilizing and recently recovering.
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,Short summary
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.
Katherine R. Travis, Daniel J. Jacob, Jenny A. Fisher, Patrick S. Kim, Eloise A. Marais, Lei Zhu, Karen Yu, Christopher C. Miller, Robert M. Yantosca, Melissa P. Sulprizio, Anne M. Thompson, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Ronald C. Cohen, Joshua L. Laughner, Jack E. Dibb, Samuel R. Hall, Kirk Ullmann, Glenn M. Wolfe, Illana B. Pollack, Jeff Peischl, Jonathan A. Neuman, and Xianliang Zhou
Atmos. Chem. Phys., 16, 13561–13577,Short summary
Ground-level ozone pollution in the Southeast US involves complex chemistry driven by anthropogenic emissions of nitrogen oxides (NOx) and biogenic emissions of isoprene. We find that US NOx emissions are overestimated nationally by as much as 50 % and that reducing model emissions by this amount results in good agreement with SEAC4RS aircraft measurements in August and September 2013. Observations of nitrate wet deposition fluxes and satellite NO2 columns further support this result.
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,Short summary
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,Short summary
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.
Kane A. Stone, Olaf Morgenstern, David J. Karoly, Andrew R. Klekociuk, W. John French, N. Luke Abraham, and Robyn Schofield
Atmos. Chem. Phys., 16, 2401–2415,Short summary
This paper describes the set-up and evaluation of the Australian Community Climate and Earth System Simulator – chemistry-climate model.
Emphasis is placed on the Antarctic ozone hole, which is very important considering its role modulating Southern Hemisphere surface climate. While the model simulates the global distribution of ozone well, there is a disparity in the vertical location of springtime ozone depletion over Antarctica, highlighting important areas for future development.
Emphasis is placed on the Antarctic ozone hole, which is very important considering its role modulating Southern Hemisphere surface climate. While the model simulates the global distribution of ozone well, there is a disparity in the vertical location of springtime ozone depletion over Antarctica, highlighting important areas for future development.
R. S. Humphries, A. R. Klekociuk, R. Schofield, M. Keywood, J. Ward, and S. R. Wilson
Atmos. Chem. Phys., 16, 2185–2206,Short summary
This work represents the first observational study of atmospheric sub-micron aerosols in the East Antarctic pack ice region and found springtime aerosol concentrations were higher than any observed elsewhere in the Antarctic and Southern Ocean region. Further analysis suggested these aerosols formed in the Antarctic free troposphere. Their subsequent transport to the Southern Ocean, as suggest by trajectory analyses, could help to reduce the discrepancy in the radiative budget in the region.
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,Short summary
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.
C. S. M. Turney, C. J. Fogwill, A. R. Klekociuk, T. D. van Ommen, M. A. J. Curran, A. D. Moy, and J. G. Palmer
The Cryosphere, 9, 2405–2415,Short summary
Recent trends in ocean circulation, sea ice and climate over the Southern Ocean and Antarctica are highly complex. Here we report a new snow core from the South Pole alongside reanalysis of 20th century global atmospheric circulation. We demonstrate for the first time that atmospheric pressure anomalies in the mid-latitudes act as "gatekeepers" to meridional exchange over continental Antarctica, modulated by the tropical Pacific, with potentially significant impacts on surface mass balance.
R. S. Humphries, R. Schofield, M. D. Keywood, J. Ward, J. R. Pierce, C. M. Gionfriddo, M. T. Tate, D. P. Krabbenhoft, I. E. Galbally, S. B. Molloy, A. R. Klekociuk, P. V. Johnston, K. Kreher, A. J. Thomas, A. D. Robinson, N. R. P. Harris, R. Johnson, and S. R. Wilson
Atmos. Chem. Phys., 15, 13339–13364,Short summary
An atmospheric new particle formation event that was observed in the pristine East Antarctic pack ice during a springtime voyage in 2012 is characterised in terms of formation and growth rates. Known nucleation mechanisms (e.g. those involving sulfate, iodine and organics) were unable to explain observations; however, correlations with total gaseous mercury were found, leading to the suggestion of a possible mercury-driven nucleation mechanism not previously described.
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,
G. Zeng, J. E. Williams, J. A. Fisher, L. K. Emmons, N. B. Jones, O. Morgenstern, J. Robinson, D. Smale, C. Paton-Walsh, and D. W. T. Griffith
Atmos. Chem. Phys., 15, 7217–7245,Short summary
We assess the impact of biogenic emissions on CO and HCHO in the Southern Hemisphere (SH), with simulations using different emission inventories. Differences in biogenic emissions result in large differences on modelled CO in the source and the remote regions. Substantial inter-model differences exist. Models significantly underestimate observed HCHO columns in the SH, suggesting missing sources in the models. Differences in the CO/OH/CH4 chemistry lead to differences in HCHO in remote regions.
W. Frey, R. Schofield, P. Hoor, D. Kunkel, F. Ravegnani, A. Ulanovsky, S. Viciani, F. D'Amato, and T. P. Lane
Atmos. Chem. Phys., 15, 6467–6486,Short summary
This study examines the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 campaign in connection with a deep convective system, using the WRF model. Passive tracers are initialised to study the impact of the deep convection on the tracers and water vapour. We use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
J. A. Fisher, S. R. Wilson, G. Zeng, J. E. Williams, L. K. Emmons, R. L. Langenfelds, P. B. Krummel, and L. P. Steele
Atmos. Chem. Phys., 15, 3217–3239,Short summary
The Southern Hemisphere (SH) serves as an important test bed for evaluating our understanding of the processes that drive the composition of the clean background atmosphere. Using data from two aircraft campaigns, combined with four atmospheric chemistry models, we find a large sensitivity in the remote SH to biogenic emissions and their subsequent chemistry and transport. Future model evaluation and measurement campaigns should prioritize reducing uncertainties in these processes.
R. Schofield, L. M. Avallone, L. E. Kalnajs, A. Hertzog, I. Wohltmann, and M. Rex
Atmos. Chem. Phys., 15, 2463–2472,Short summary
Ozone measurements onboard three Concordiasi balloons flown in the stratosphere in the Antarctic spring of 2010 are presented. These measurements are the first long-duration in situ measurements of Antarctic springtime stratospheric ozone. By matching air parcels, ozone loss rates where derived. Downwind of the Antarctic Peninsula, very large ozone losses of up to 230 ppb per day or 16 ppbv per sunlit hour were observed. These high rates are consistent with almost complete chlorine activation.
K. Stone, M. B. Tully, S. K. Rhodes, and R. Schofield
Atmos. Meas. Tech., 8, 1043–1053,
J. M. Siddaway, S. V. Petelina, D. J. Karoly, A. R. Klekociuk, and R. J. Dargaville
Atmos. Chem. Phys., 13, 4413–4427,
S. P. Alexander, D. J. Murphy, and A. R. Klekociuk
Atmos. Chem. Phys., 13, 3121–3132,
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Spatially and temporally resolved measurements of NOx fluxes by airborne eddy covariance over Greater LondonTemporary pause in the growth of atmospheric ethane and propane in 2015–2018Formation of condensable organic vapors from anthropogenic and biogenic volatile organic compounds (VOCs) is strongly perturbed by NOx in eastern ChinaSeasonal and diurnal variations in biogenic volatile organic compounds in highland and lowland ecosystems in southern KenyaOrigins and characterization of CO and O3 in the African upper troposphereIn situ ozone production is highly sensitive to volatile organic compounds in Delhi, IndiaRole of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissionsDynamics of gaseous oxidized mercury at Villum Research Station during the High Arctic summerIsotopic evidence for dominant secondary production of HONO in near-ground wildfire plumesOpinion: Papers that shaped tropospheric chemistryMeasurement report: Source apportionment of volatile organic compounds at the remote high-altitude Maïdo observatoryShipborne measurements of methane and carbon dioxide in the Middle East and Mediterranean areas and the contribution from oil and gas emissionsObservations of iodine monoxide over three summers at the Indian Antarctic bases of Bharati and MaitriUnexplored volatile organic compound emitted from petrochemical facilities: implications for ozone production and atmospheric chemistryAtmospheric gaseous hydrochloric and hydrobromic acid in urban Beijing, China: detection, source identification and potential atmospheric impactsImpact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATomSpectrometric measurements of atmospheric propane (C3H8)Air–sea exchange of acetone, acetaldehyde, DMS and isoprene at a UK coastal siteMeasurement report: Emissions of intermediate-volatility organic compounds from vehicles under real-world driving conditions in an urban tunnelLong-Term Atmospheric Emissions for the Coal Oil Point Natural Marine Hydrocarbon Seep Field, Offshore CaliforniaInvestigations on the anthropogenic reversal of the natural ozone gradient between northern and southern midlatitudesThe Effects of the COVID-19 Lockdowns on the Composition of the Troposphere as Seen by IAGOSSpeciated atmospheric mercury at Waliguan Global Atmospheric Watch station in the northeastern Tibetan Plateau: implication of dust related sources for particulate bound mercuryMeasurement report: Molecular composition and volatility of gaseous organic compounds in a boreal forest – from volatile organic compounds to highly oxygenated organic moleculesBoreal forest fire CO and CH4 emission factors derived from tower observations in Alaska during the extreme fire season of 2015Chemical characterization of oxygenated organic compounds in the gas phase and particle phase using iodide CIMS with FIGAERO in urban airNew approach to evaluate satellite-derived XCO2 over oceans by integrating ship and aircraft observationsCentral role of nitric oxide in ozone production in the upper tropical troposphere over the Atlantic Ocean and western AfricaSesquiterpenes and oxygenated sesquiterpenes dominate the VOC (C5–C20) emissions of downy birchesMeasurement report: Online measurement of gas-phase nitrated phenols utilizing a CI-LToF-MS: primary sources and secondary formationMeasurement report: In situ observations of deep convection without lightning during the tropical cyclone Florence 2018Measurement report: Regional characteristics of seasonal and long-term variations in greenhouse gases at Nainital, India and Comilla, BangladeshMeasurement Report: Variability in the composition of biogenic volatile organic compounds in a southeastern US forest and their role in atmospheric reactivityReactive nitrogen around the Arabian Peninsula and in the Mediterranean Sea during the 2017 AQABA ship campaignStratospheric carbon isotope fractionation and tropospheric histories of CFC-11, CFC-12, and CFC-113 isotopologuesIsotopic compositions of atmospheric total gaseous mercury in 10 Chinese cities and implications for land surface emissionsMeasurement report: Observation-based formaldehyde production rates and their relation to OH reactivity around the Arabian PeninsulaObservations of speciated isoprene nitrates in Beijing: implications for isoprene chemistryContributions to OH reactivity from unexplored volatile organic compounds measured by PTR-ToF-MS – a case study in a suburban forest of the Seoul metropolitan area during the Korea–United States Air Quality Study (KORUS-AQ) 2016Total OH reactivity over the Amazon rainforest: variability with temperature, wind, rain, altitude, time of day, season, and an overall budget closureWhere there is smoke there is mercury: Assessing boreal forest fire mercury emissions using aircraft and highlighting uncertainties associated with upscaling emissions estimatesNighttime and Daytime Dark Oxidation Chemistry in Wildfire Plumes: An Observation and Model Analysis of FIREX-AQ Aircraft DataFormation of nighttime sulfuric acid from the ozonolysis of alkenes in BeijingSpatiotemporal variation, sources, and secondary transformation potential of volatile organic compounds in Xi'an, ChinaIdentifying and quantifying source contributions of air quality contaminants during unconventional shale gas extractionObserved decreases in on-road CO2 concentrations in Beijing during COVID-19 restrictionsInvestigation of several proxies to estimate sulfuric acid concentration under volcanic plume conditionsMeasurement report: Exploring NH3 behavior in urban and suburban Beijing: comparison and implicationsAtmospheric organic vapors in two European pine forests measured by a Vocus PTR-TOF: insights into monoterpene and sesquiterpene oxidation processesSpeciation of VOC emissions related to offshore North Sea oil and gas production
Adam R. Vaughan, James D. Lee, Stefan Metzger, David Durden, Alastair C. Lewis, Marvin D. Shaw, Will S. Drysdale, Ruth M. Purvis, Brian Davison, and C. Nicholas Hewitt
Atmos. Chem. Phys., 21, 15283–15298,Short summary
Validating emissions estimates of atmospheric pollutants is a vital pathway towards reducing urban concentrations of air pollution and ensuring effective legislative controls are implemented. The work presented here highlights a strategy capable of quantifying and spatially disaggregating NOx emissions over challenging urban terrain. This work shows great scope as a tool for emission inventory validation and independent generation of high-resolution surface emissions on a city-wide scale.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170,Short summary
After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814,Short summary
Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Yang Liu, Simon Schallhart, Ditte Taipale, Toni Tykkä, Matti Räsänen, Lutz Merbold, Heidi Hellén, and Petri Pellikka
Atmos. Chem. Phys., 21, 14761–14787,Short summary
We studied the mixing ratio of biogenic volatile organic compounds (BVOCs) in a humid highland and dry lowland African ecosystem in Kenya. The mixing ratio of monoterpenoids was similar to that measured in the relevant ecosystems in western and southern Africa, while that of isoprene was lower. Modeling the emission factors (EFs) for BVOCs from the lowlands, the EFs for isoprene and β-pinene agreed well with what is assumed in the MEGAN, while those of α-pinene and limonene were higher.
Victor Lannuque, Bastien Sauvage, Brice Barret, Hannah Clark, Gilles Athier, Damien Boulanger, Jean-Pierre Cammas, Jean-Marc Cousin, Alain Fontaine, Eric Le Flochmoën, Philippe Nédélec, Hervé Petetin, Isabelle Pfaffenzeller, Susanne Rohs, Herman G. J. Smit, Pawel Wolff, and Valérie Thouret
Atmos. Chem. Phys., 21, 14535–14555,Short summary
The African intertropical troposphere is one of the world areas where the increase in ozone mixing ratio has been most pronounced since 1980 and where high carbon monoxide mixing ratios are found in altitude. In this article, IAGOS aircraft measurements, IASI satellite instrument observations, and SOFT-IO model products are used to explore the seasonal distribution variations and the origin of ozone and carbon monoxide over the African upper troposphere.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630,Short summary
Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
Alexandre Kukui, Michel Chartier, Jinhe Wang, Hui Chen, Sébastien Dusanter, Stéphane Sauvage, Vincent Michoud, Nadine Locoge, Valérie Gros, Thierry Bourrianne, Karine Sellegri, and Jean-Marc Pichon
Atmos. Chem. Phys., 21, 13333–13351,Short summary
Sulfuric acid, H2SO4, plays a key role in formation of secondary atmospheric aerosol particles. It is generally accepted that the major atmospheric source of H2SO4 is the reaction of OH radicals with SO2. In this study, importance of an additional H2SO4 source via oxidation of SO2 by stabilized Criegee intermediates was estimated based on measurements at a remote site on Cape Corsica. It was found that the oxidation of SO2 by SCI may be an important source of H2SO4, especially during nighttime.
Jakob Boyd Pernov, Bjarne Jensen, Andreas Massling, Daniel Charles Thomas, and Henrik Skov
Atmos. Chem. Phys., 21, 13287–13309,Short summary
Atmospheric mercury species (GEM, GOM, PHg) are important constituents in the High Arctic due to their detrimental effects on human and ecosystem health. However, understanding their behavior in the High Arctic summer remains lacking. This research investigates the dynamics of mercury oxidation in the High Arctic summer. The cold, dry, sunlit free troposphere was associated with events of high GOM in the High Arctic summer, while individual events yielded unique origins.
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,Short summary
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.
Paul S. Monks, A. R. Ravishankara, Erika von Schneidemesser, and Roberto Sommariva
Atmos. Chem. Phys., 21, 12909–12948,Short summary
Which published papers have transformed our understanding of the chemical processes in the troposphere and shaped the field of atmospheric chemistry? We explore how these papers have shaped the development of the field of atmospheric chemistry and identify the major landmarks in the field of atmospheric chemistry through the lens of those papers' impact on science, legislation and environmental events.
Bert Verreyken, Crist Amelynck, Niels Schoon, Jean-François Müller, Jérôme Brioude, Nicolas Kumps, Christian Hermans, Jean-Marc Metzger, Aurélie Colomb, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 12965–12988,Short summary
We present a 2-year dataset of trace gas concentrations, specifically an array of volatile organic compounds (VOCs), recorded at the Maïdo observatory, a remote tropical high-altitude site located on a small island in the southwest Indian Ocean. We found that island-scale transport is an important driver for the daily cycle of VOC concentrations. During the day, surface emissions from the island affect the atmospheric composition at Maïdo greatly, while at night this impact is strongly reduced.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462,Short summary
We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Anoop S. Mahajan, Mriganka S. Biswas, Steffen Beirle, Thomas Wagner, Anja Schönhardt, Nuria Benavent, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 11829–11842,Short summary
Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone. We present IO observations over three summers (2015–2017) at the Indian Antarctic bases of Bharati and Maitri. IO was observed during all campaigns with mixing ratios below 2 pptv, which is lower than the peak levels observed in West Antarctica, showing the differences in regional chemistry and emissions.
Chinmoy Sarkar, Gracie Wong, Anne Mielnik, Sanjeevi Nagalingam, Nicole Jenna Gross, Alex B. Guenther, Taehyoung Lee, Taehyun Park, Jihee Ban, Seokwon Kang, Jin-Soo Park, Joonyoung Ahn, Danbi Kim, Hyunjae Kim, Jinsoo Choi, Beom-Keun Seo, Jong-Ho Kim, Jeong-Ho Kim, Soo Bog Park, and Saewung Kim
Atmos. Chem. Phys., 21, 11505–11518,Short summary
We present experimental proofs illustrating the emission of an unexplored volatile organic compound, tentatively assigned as ketene, in an industrial facility in South Korea. The emission of such a compound has rarely been reported, but our experimental data show that the emission rate is substantial. It potentially has tremendous implications for regional air quality and public health, as it is highly reactive and toxic at the same time.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452,Short summary
We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
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,Short summary
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.
Geoffrey C. Toon, Jean-Francois L. Blavier, Keeyoon Sung, and Katelyn Yu
Atmos. Chem. Phys., 21, 10727–10743,Short summary
We report measurements of atmospheric propane (C3H8) from analysis of ground-based infra-red solar absorption spectra measured from various sites by the Jet Propulsion Laboratory (JPL) MkIV interferometer. These measurements suggest that exploitation of natural gas fields is a major and growing source of propane in the USA. Also, there seem to be propane sources in large cities such as Los Angeles, possibly related to use of liquefied petroleum gas (LPG).
Daniel P. Phillips, Frances E. Hopkins, Thomas G. Bell, Peter S. Liss, Philip D. Nightingale, Claire E. Reeves, Charel Wohl, and Mingxi Yang
Atmos. Chem. Phys., 21, 10111–10132,Short summary
We present the first measurements of the rate of transfer (flux) of three gases between the atmosphere and the ocean, using a direct flux measurement technique, at a coastal site. We show greater atmospheric loss of acetone and acetaldehyde into the ocean than estimated by global models for the open water; importantly, the acetaldehyde transfer direction is opposite to the model estimates. Measured dimethylsulfide fluxes agreed with a recent model. Isoprene fluxes were too weak to be measured.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 21, 10005–10013,Short summary
A tunnel test was initiated to measure the vehicular IVOC emissions under real-world driving conditions. Higher SOA formation estimated from vehicular IVOCs compared to those from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
Ira Leifer, Christopher Melton, and Donald R. Blake
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We demonstrate a novel approach using air quality station data to derive three decade averaged emissions from the Coal Oil Point seep field, a highly variable geological migration system spatially and temporally. Emissions were 19 Gigagrams per year, suggesting that the COP seep field contributes 0.25 % of the marine seep budget based on a recent global estimate. Unlike surveys, which provide snapshots of seepage – a highly variable geo-migration process.
David D. Parrish, Richard G. Derwent, Steven T. Turnock, Fiona M. O'Connor, Johannes Staehelin, Susanne E. Bauer, Makoto Deushi, Naga Oshima, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 21, 9669–9679,Short summary
The few ozone measurements made before the 1980s indicate that industrial development increased ozone concentrations by a factor of ~ 2 at northern midlatitudes, which are now larger than at southern midlatitudes. This difference was much smaller, and likely reversed, in the pre-industrial atmosphere. Earth system models find similar increases, but not higher pre-industrial ozone in the south. This disagreement may indicate that modeled natural ozone sources and/or deposition loss are inadequate.
Hannah Clark, Yasmine Bennouna, Maria Tsivlidou, Pawel Wolff, Bastien Sauvage, Brice Barret, Eric Le Flochmoën, Romain Blot, Damien Boulanger, Jean-Marc Cousin, Philippe Nédélec, Andreas Petzold, and Valérie Thouret
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We examined 27 years of IAGOS (In-service Aircraft for a Global Observing System) measurements at Frankfurt to see if there were unusual or extreme features during the spring of 2020 when there were lockdowns across Europe and when pollution was reported to have fallen. Ozone increased at the surface which might be linked to the reduction of pollution from lockdown. The amount of CO decreased but the impact of the lockdowns in Europe was off-set by pollution from elsewhere.
Hui Zhang, Xuewu Fu, Ben Yu, Baoxin Li, Peng Liu, Guoqing Zhang, Leiming Zhang, and Xinbin Feng
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Our observations of speciated atmospheric Hg at Waliguan GAW Observatory found the concentrations gaseous elemental mercury (GEM) and particulate bound mercury (PBM) were elevated as compared to the Northern Hemisphere background. We propose that the major sources of GEM and PBM were mainly related to anthropogenic emissions and desert dust related sources, respectively. This study highlights that dust related sources played an important role in the variations of PBM in the Tibetan Plateau.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977,Short summary
We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
Elizabeth B. Wiggins, Arlyn Andrews, Colm Sweeney, John B. Miller, Charles E. Miller, Sander Veraverbeke, Roisin Commane, Steven Wofsy, John M. Henderson, and James T. Randerson
Atmos. Chem. Phys., 21, 8557–8574,Short summary
We analyzed high-resolution trace gas measurements collected from a tower in Alaska during a very active fire season to improve our understanding of trace gas emissions from boreal forest fires. Our results suggest previous studies may have underestimated emissions from smoldering combustion in boreal forest fires.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478,Short summary
We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
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,Short summary
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.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211,Short summary
Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Heidi Hellén, Arnaud P. Praplan, Toni Tykkä, Aku Helin, Simon Schallhart, Piia P. Schiestl-Aalto, Jaana Bäck, and Hannele Hakola
Atmos. Chem. Phys., 21, 8045–8066,Short summary
Even though terpene emissions of boreal needle trees have been studied quite intensively, there is less knowledge of the emissions of broadleaved deciduous trees and emissions of larger terpenes and oxygenated volatile organic compounds. Here we studied downy birch (Betula pubescens) emissions, and especially sesquiterpene and oxygenated sesquiterpene emissions were found to be high. These emissions may have significant effects on secondary organic aerosol formation in boreal areas.
Kai Song, Song Guo, Haichao Wang, Ying Yu, Hui Wang, Rongzhi Tang, Shiyong Xia, Yuanzheng Gong, Zichao Wan, Daqi Lv, Rui Tan, Wenfei Zhu, Ruizhe Shen, Xin Li, Xuena Yu, Shiyi Chen, Liming Zeng, and Xiaofeng Huang
Atmos. Chem. Phys., 21, 7917–7932,Short summary
Nitrated phenols (NPs) are crucial components of brown carbon. To comprehend the constitutes and sources of NPs in winter of Beijing, their concentrations were measured by a CI-LToF-MS. The secondary formation process was simulated by a box model. NPs were mainly influenced by primary emissions and regional transport. Primary emitted phenol rather than benzene oxidation was crucial in the heavy pollution episode in Beijing. This provides more insight into pollution control strategies of NPs.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945,Short summary
Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Shohei Nomura, Manish Naja, Md. Kawser Ahmed, Hitoshi Mukai, Yukio Terao, Toshinobu Machida, Motoki Sasakawa, and Prabir K. Patra
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Long-term measurements of greenhouse gases at India and Bangladesh unveiled specific characteristics in their variations in these regions. Plants including rice cultivated in winter and summer strongly affected seasonal variations and levels in CO2 and CH4. Long-term variability of GHGs showed quite different feature in their growth rates from those in Mauna Loa. GHGs trends in this region seemed to be hardly affected by ENSO.
Deborah F. McGlynn, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We present one year of hourly measurements of chemically resolved BVOCs between September 15, 2019, and September 15, 2020, collected at a research tower in Central Virginia. Concentrations of a range of BVOCs are described and examined for their impact on atmospheric reactivity. A majority of reactivity comes from α-pinene and limonene, highlighting the importance of both concentration and structure in assessing atmospheric impacts of emissions.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498,Short summary
This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873,Short summary
CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Xuewu Fu, Chen Liu, Hui Zhang, Yue Xu, Hui Zhang, Jun Li, Xiaopu Lyu, Gan Zhang, Hai Guo, Xun Wang, Leiming Zhang, and Xinbin Feng
Atmos. Chem. Phys., 21, 6721–6734,Short summary
TGM concentrations and isotopic compositions in 10 Chinese cities showed strong seasonality with higher TGM concentrations and Δ199Hg and lower δ202Hg in summer. We found the seasonal variations in TGM concentrations and isotopic compositions were highly related to regional surface Hg(0) emissions, suggesting land surface Hg(0) emissions are an important source of atmospheric TGM that contribute dominantly to the seasonal variations in TGM concentrations and isotopic compositions.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radical (OH) and the OH reactivity around the Arabian Peninsula, which were used to perform a comparison between local HCHO production and the related OH chemistry. This regression analysis revealed the regional HCHO yield alpha, which was elevated in the Arabian Gulf (also known as the Persion Gulf) and highlights the area as a hotspot of photochemical air pollution.
Claire E. Reeves, Graham P. Mills, Lisa K. Whalley, W. Joe F. Acton, William J. Bloss, Leigh R. Crilley, Sue Grimmond, Dwayne E. Heard, C. Nicholas Hewitt, James R. Hopkins, Simone Kotthaus, Louisa J. Kramer, Roderic L. Jones, James D. Lee, Yanhui Liu, Bin Ouyang, Eloise Slater, Freya Squires, Xinming Wang, Robert Woodward-Massey, and Chunxiang Ye
Atmos. Chem. Phys., 21, 6315–6330,Short summary
The impact of isoprene on atmospheric chemistry is dependent on how its oxidation products interact with other pollutants, specifically nitrogen oxides. Such interactions can lead to isoprene nitrates. We made measurements of the concentrations of individual isoprene nitrate isomers in Beijing and used a model to test current understanding of their chemistry. We highlight areas of uncertainty in understanding, in particular the chemistry following oxidation of isoprene by the nitrate radical.
Dianne Sanchez, Roger Seco, Dasa Gu, Alex Guenther, John Mak, Youngjae Lee, Danbi Kim, Joonyoung Ahn, Don Blake, Scott Herndon, Daun Jeong, John T. Sullivan, Thomas Mcgee, Rokjin Park, and Saewung Kim
Atmos. Chem. Phys., 21, 6331–6345,Short summary
We present observations of total reactive gases in a suburban forest observatory in the Seoul metropolitan area. The quantitative comparison with speciated trace gas observations illustrated significant underestimation in atmospheric reactivity from the speciated trace gas observational dataset. We present scientific discussion about potential causes.
Eva Y. Pfannerstill, Nina G. Reijrink, Achim Edtbauer, Akima Ringsdorf, Nora Zannoni, Alessandro Araújo, Florian Ditas, Bruna A. Holanda, Marta O. Sá, Anywhere Tsokankunku, David Walter, Stefan Wolff, Jošt V. Lavrič, Christopher Pöhlker, Matthias Sörgel, and Jonathan Williams
Atmos. Chem. Phys., 21, 6231–6256,Short summary
Tropical forests are globally significant for atmospheric chemistry. However, the mixture of reactive organic gases emitted by these ecosystems is poorly understood. By comprehensive observations at an Amazon forest site, we show that oxygenated species were previously underestimated in their contribution to the tropical-forest reactant mix. Our results show rain and temperature effects and have implications for models and the understanding of ozone and particle formation above tropical forests.
David S. McLagan, Geoff W. Stupple, Andrea Darlington, Katherine Hayden, and Alexandra Steffen
Atmos. Chem. Phys., 21, 5635–5653,Short summary
An assessment of mercury emissions from a burning boreal forest was made by flying an aircraft through its plume to collect in situ gas and particulate measurements. Direct data show that in-plume gaseous elemental mercury concentrations reach up to 2.4× background for this fire and up to 5.6× when using a correlation with CO data. These unique data are applied to a series of known empirical emissions estimates and used to highlight current uncertainties in the literature.
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, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard H. Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Lee Thornhill, Joel A. Thornton, Geoff S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
To understand air quality impacts from wildfire smoke 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 “nighttime” chemistry thrives and controls the fate of key smoke plume chemical processes.
Yishuo Guo, Chao Yan, Chang Li, Wei Ma, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 5499–5511,Short summary
Fog, cloud and haze are very common natural phenomena. Sulfuric acid (SA) is one of the key compounds forming those suspended particles, technically called aerosols, through gas-to-particle conversion. Therefore, the concentration level, source and sink of SA is very important. Our results show that ozonolysis of alkenes plays a major role in nighttime SA formation under unpolluted conditions in urban Beijing, and nighttime cluster mode particles are probably driven by SA in urban environments.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958,Short summary
Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
Nur H. Orak, Matthew Reeder, and Natalie J. Pekney
Atmos. Chem. Phys., 21, 4729–4739,Short summary
In this paper, we investigate the effect of unconventional natural gas development activities on local air quality. This is the first study, to our knowledge, to collect high-time-resolution ambient concentrations of compounds emitted from well pad activity on Marcellus Shale during various phases of operation such that the relative air quality effect of each phase of development can be investigated.
Di Liu, Wanqi Sun, Ning Zeng, Pengfei Han, Bo Yao, Zhiqiang Liu, Pucai Wang, Ke Zheng, Han Mei, and Qixiang Cai
Atmos. Chem. Phys., 21, 4599–4614,Short summary
It is difficult to directly observe the COVID-19 signals in CO2 due to the strong weather induced variations. Here, we determined the on-road CO2 concentration declines in Beijing using mobile observatory data before (BC), during (DC) and after COVID-19 (AC). We chose trips with the most similar weather and calculated the enhancement, the difference between on-road and the city “background”. We showed a clear on-road CO2 decrease in DC, which is consistent with the emissions reductions in DC.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560,Short summary
Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Ziru Lan, Weili Lin, Weiwei Pu, and Zhiqiang Ma
Atmos. Chem. Phys., 21, 4561–4573,Short summary
Haze related to particulate matter has become a big problem in eastern China, and ammonia (NH3) plays an important role in secondary particulate matter formation. In this work, variations in the NH3 mixing ratio showed that the contributions of NH3 sources and sinks in urban and suburban areas were quite different, although the areas were under the influence of similar weather systems. This study furthers the understanding of the behavior of NH3 in a megacity environment.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147,Short summary
For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Shona E. Wilde, Pamela A. Dominutti, Grant Allen, Stephen J. Andrews, Prudence Bateson, Stephane J.-B. Bauguitte, Ralph R. Burton, Ioana Colfescu, James France, James R. Hopkins, Langwen Huang, Anna E. Jones, Tom Lachlan-Cope, James D. Lee, Alastair C. Lewis, Stephen D. Mobbs, Alexandra Weiss, Stuart Young, and Ruth M. Purvis
Atmos. Chem. Phys., 21, 3741–3762,Short summary
We use airborne measurements to evaluate the speciation of volatile organic compound (VOC) emissions from offshore oil and gas (O&G) installations in the North Sea. The composition of emissions varied across regions associated with either gas, condensate or oil extraction, demonstrating that VOC emissions are not uniform across the whole O&G sector. We compare our results to VOC source profiles in the UK emissions inventory, showing these emissions are not currently fully characterized.
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Alexander, S. P., Murphy, D. J., and Klekociuk, A. R.: High resolution VHF radar measurements of tropopause structure and variability at Davis, Antarctica (69S, 78E), Atmos. Chem. Phys., 13, 3121–3132, https://doi.org/10.5194/acp-13-3121-2013, 2013.
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Das, S. S., Ratnam, M. V., Uma, K. N., Subrahmanyam, K. V., Girach, I. A., Patra, A. K., Aneesh, S., Suneeth, K. V., Kishore Kumar, K., Kesarkar, A. P., Sijikumar, S., and Ramkumar, G.: Influence of tropical cyclones on tropospheric ozone: possible implications, Atmos. Chem. Phys., 16, 4837–4847, https://doi.org/10.5194/acp-16-4837-2016, 2016.
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Frey, W., Schofield, R., Hoor, P., Kunkel, D., Ravegnani, F., Ulanovsky, a., Viciani, S., D'Amato, F., and Lane, T. P.: The impact of overshooting deep convection on local transport and mixing in the tropical upper troposphere/lower stratosphere (UTLS), Atmos. Chem. Phys., 15, 6467–6486, https://doi.org/10.5194/acp-15-6467-2015, 2015.
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Giglio, L., Randerson, J. T., and Van Der Werf, G. R.: Analysis of daily, monthly, and annual burned area using the fourth-generation global fire emissions database (GFED4), J. Geophys. Res., 118, 317–328, https://doi.org/10.1002/jgrg.20042, 2013.
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Lin, M., Fiore, A. M., Cooper, O. R., Horowitz, L. W., Langford, A. O., Levy, H., Johnson, B. J., Naik, V., Oltmans, S. J., and Senff, C. J.: Springtime high surface ozone events over the western United States: Quantifying the role of stratospheric intrusions, J. Geophys. Res., 117, 1–20, https://doi.org/10.1029/2012JD018151, 2012.
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Liu, J., Rodriguez, J. M., Thompson, A. M., Logan, J. A., Douglass, A. R., Olsen, M. A., Steenrod, S. D., and Posny, F.: Origins of tropospheric ozone interannual variation over Réunion: A model investigation, J. Geophys. Res., 1–19, https://doi.org/10.1002/2015JD023981, 2015.
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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.
An analysis of data from ozonesondes released at three southern oceanic sites shows the impact...