Articles | Volume 20, issue 20
Atmos. Chem. Phys., 20, 12033–12045, 2020
https://doi.org/10.5194/acp-20-12033-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 12033–12045, 2020
https://doi.org/10.5194/acp-20-12033-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 26 Oct 2020
Research article | 26 Oct 2020
Observations of atmospheric 14CO2 at Anmyeondo GAW station, South Korea: implications for fossil fuel CO2 and emission ratios
Haeyoung Lee et al.
Related authors
Lev D. Labzovskii, Samuel Takele Kenea, Jinwon Kim, Haeyoung Lee, Shanlan Li, Young-Hwa Byun, Tae-Young Goo, and Young-Suk Oh
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-114, https://doi.org/10.5194/acp-2020-114, 2020
Revised manuscript not accepted
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Global CO2 growth rate is a key indicator of the balance between carbon sources and sinks but there are few observational methods to quantify this rate. We proved that the estimates of global CO2 growth rate are consistent across wide range of data sources. This finding is essential given recently shown disagreement between CO2 models in simulating global CO2 growth rate, lack of consensus about the method for quantifying this rate and dearth of observational methods to infer global CO2 growth.
Christoph Zellweger, Rainer Steinbrecher, Olivier Laurent, Haeyoung Lee, Sumin Kim, Lukas Emmenegger, Martin Steinbacher, and Brigitte Buchmann
Atmos. Meas. Tech., 12, 5863–5878, https://doi.org/10.5194/amt-12-5863-2019, https://doi.org/10.5194/amt-12-5863-2019, 2019
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We analysed results obtained through CO and N2O performance audits conducted within the framework of the Global Atmosphere Watch (GAW) quality management system of the World Meteorology Organization (WMO). The results reveal that current spectroscopic measurement techniques have clear advantages with respect to data quality objectives compared to more traditional methods. Further, they allow for a smooth continuation of historic CO and N2O time series.
Haeyoung Lee, Sang-Ok Han, Sang-Boom Ryoo, Jeong-Soon Lee, and Gang-Woong Lee
Atmos. Chem. Phys., 19, 2149–2163, https://doi.org/10.5194/acp-19-2149-2019, https://doi.org/10.5194/acp-19-2149-2019, 2019
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We introduced our identical systems, which were installed at three S. Korea stations, using CRDS and a drying system. The measurement uncertainty was ~ 0.11 ppm across the stations. CO2 observed in the west of S. Korea was very sensitive to East Asia (e.g., China), indicating that data include CO2 flux information from East Asia. Through long-term comparison to other East Asian stations, it was suggested that they could be affected not only by local vegetation but also by measurement quality.
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.
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.
Regina Gonzalez Moguel, Felix Vogel, Sébastien Ars, Hinrich Schaefer, Jocelyn Turnbull, and Peter Douglas
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-622, https://doi.org/10.5194/acp-2021-622, 2021
Preprint under review for ACP
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Evaluating methane (CH4) sources in the Athabasca Oil Sands Region (AOSR) is crucial to effectively mitigate CH4 emissions. We tested the use of carbon isotopes to estimate source contributions from key CH4 sources in the AOSR and found that 53 ± 18 % of CH4 emissions originated from surface mining and processing facilities, 36 ± 18 % from tailings ponds, and 10 < 1 % from wetlands, confirming previous findings and showing that this method can be successfully used to partition CH4 sources.
Linda M. J. Kooijmans, Ara Cho, Jin Ma, Aleya Kaushik, Katherine D. Haynes, Ian Baker, Ingrid T. Luijkx, Mathijs Groenink, Wouter Peters, John B. Miller, Joseph A. Berry, Jérôme Ogée, Laura K. Meredith, Wu Sun, Kukka-Maaria Kohonen, Timo Vesala, Ivan Mammarella, Huilin Chen, Felix M. Spielmann, Georg Wohlfahrt, Max Berkelhammer, Mary E. Whelan, Kadmiel Maseyk, Ulli Seibt, Roisin Commane, Richard Wehr, and Maarten Krol
Biogeosciences Discuss., https://doi.org/10.5194/bg-2021-192, https://doi.org/10.5194/bg-2021-192, 2021
Preprint under review for BG
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The gas carbonyl sulfide (COS) can be used to estimate photosynthesis. To adopt this approach on regional and global scales, we need biosphere models that can simulate COS exchange. So far, such models haven’t been evaluated against observations. We evaluate the COS biosphere exchange of the SiB4 model against COS flux observations. We find that the model is capable of simulating key processes in COS biosphere exchange. Still, we give recommendations for further improvement of the model.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
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, https://doi.org/10.5194/acp-21-8557-2021, https://doi.org/10.5194/acp-21-8557-2021, 2021
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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.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-299, https://doi.org/10.5194/acp-2021-299, 2021
Revised manuscript accepted for ACP
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Predicting Earth's climate is difficult partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement in these data is necessary.
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. Discuss., https://doi.org/10.5194/acp-2021-285, https://doi.org/10.5194/acp-2021-285, 2021
Revised manuscript accepted for ACP
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After a multi-decade global decline in atmospheric concentrations of ethane and propane (precursors to 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.
Junjie Liu, Latha Baskaran, Kevin Bowman, David Schimel, A. Anthony Bloom, Nicholas C. Parazoo, Tomohiro Oda, Dustin Carroll, Dimitris Menemenlis, Joanna Joiner, Roisin Commane, Bruce Daube, Lucianna V. Gatti, Kathryn McKain, John Miller, Britton B. Stephens, Colm Sweeney, and Steven Wofsy
Earth Syst. Sci. Data, 13, 299–330, https://doi.org/10.5194/essd-13-299-2021, https://doi.org/10.5194/essd-13-299-2021, 2021
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On average, the terrestrial biosphere carbon sink is equivalent to ~ 20 % of fossil fuel emissions. Understanding where and why the terrestrial biosphere absorbs carbon from the atmosphere is pivotal to any mitigation policy. Here we present a regionally resolved satellite-constrained net biosphere exchange (NBE) dataset with corresponding uncertainties between 2010–2018: CMS-Flux NBE 2020. The dataset provides a unique perspective on monitoring regional contributions to the CO2 growth rate.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266, https://doi.org/10.5194/acp-21-1245-2021, https://doi.org/10.5194/acp-21-1245-2021, 2021
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In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
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.
Tea Thum, Julia E. M. S. Nabel, Aki Tsuruta, Tuula Aalto, Edward J. Dlugokencky, Jari Liski, Ingrid T. Luijkx, Tiina Markkanen, Julia Pongratz, Yukio Yoshida, and Sönke Zaehle
Biogeosciences, 17, 5721–5743, https://doi.org/10.5194/bg-17-5721-2020, https://doi.org/10.5194/bg-17-5721-2020, 2020
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Global vegetation models are important tools in estimating the impacts of global climate change. The fate of soil carbon is of the upmost importance as its emissions will enhance the atmospheric carbon dioxide concentration. To evaluate the skill of global vegetation models to model the soil carbon and its responses to environmental factors, it is important to use different data sources. We evaluated two different soil carbon models by using atmospheric carbon dioxide concentrations.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546, https://doi.org/10.5194/acp-20-9525-2020, https://doi.org/10.5194/acp-20-9525-2020, 2020
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The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Dipayan Paul, Hubertus A. Scheeren, Henk G. Jansen, Bert A. M. Kers, John B. Miller, Andrew M. Crotwell, Sylvia E. Michel, Luciana V. Gatti, Lucas G. Domingues, Caio S. C. Correia, Raiane A. L. Neves, Harro A. J. Meijer, and Wouter Peters
Atmos. Meas. Tech., 13, 4051–4064, https://doi.org/10.5194/amt-13-4051-2020, https://doi.org/10.5194/amt-13-4051-2020, 2020
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For reliable measurements of CO2 mole fractions and its stable isotope composition in air samples, one needs to carefully dry them during collection. Here we describe evaluation of a portable, consumable-free and power-free Nafion-based drying system that is currently being used for sample collection over the Amazon. Laboratory tests indicate that this Nafion-based system does not influence the mole fraction measurements of CH4, CO, N2O, SF6, and CO2 and the stable isotope composition of CO2.
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623, https://doi.org/10.5194/essd-12-1561-2020, https://doi.org/10.5194/essd-12-1561-2020, 2020
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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
Lev D. Labzovskii, Samuel Takele Kenea, Jinwon Kim, Haeyoung Lee, Shanlan Li, Young-Hwa Byun, Tae-Young Goo, and Young-Suk Oh
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-114, https://doi.org/10.5194/acp-2020-114, 2020
Revised manuscript not accepted
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Global CO2 growth rate is a key indicator of the balance between carbon sources and sinks but there are few observational methods to quantify this rate. We proved that the estimates of global CO2 growth rate are consistent across wide range of data sources. This finding is essential given recently shown disagreement between CO2 models in simulating global CO2 growth rate, lack of consensus about the method for quantifying this rate and dearth of observational methods to infer global CO2 growth.
Jian He, Vaishali Naik, Larry W. Horowitz, Ed Dlugokencky, and Kirk Thoning
Atmos. Chem. Phys., 20, 805–827, https://doi.org/10.5194/acp-20-805-2020, https://doi.org/10.5194/acp-20-805-2020, 2020
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In this work, methane representation in AM4.1 is improved by optimizing CH4 emissions to match surface observations. We find increases in CH4 sources balanced by increases in sinks lead to CH4 stabilization during 1999–2006, and anthropogenic sources (e.g., agriculture, energy, and waste) are more likely major contributors to the renewed growth after 2006. Increases in CH4 emissions and decreases in OH levels during 2008–2015 prolong CH4 lifetime and amplify methane response to emission changes.
Junsu Gil, Jeonghwan Kim, Meehye Lee, Gangwoong Lee, Dongsoo Lee, Jinsang Jung, Joonyeong An, Jinkyu Hong, Seogju Cho, Jeonghoon Lee, and Russell Long
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1012, https://doi.org/10.5194/acp-2019-1012, 2019
Preprint withdrawn
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During the KORUS-AQ campaign, nitrous acid (HONO) concentrations in Seoul were higher in high-O3 episodes than non-episodes. The photochemical model simulation demonstrates the role of HONO in promoting O3 formation through OH production and subsequent VOCs oxidation. The ambient HONO concentrations were reasonably represented by an Artificial Neural Network model, highlighting NOx, surface area, and relative humidity as crucial parameters for HONO formation in Seoul under high NOx conditions.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Christoph Zellweger, Rainer Steinbrecher, Olivier Laurent, Haeyoung Lee, Sumin Kim, Lukas Emmenegger, Martin Steinbacher, and Brigitte Buchmann
Atmos. Meas. Tech., 12, 5863–5878, https://doi.org/10.5194/amt-12-5863-2019, https://doi.org/10.5194/amt-12-5863-2019, 2019
Short summary
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We analysed results obtained through CO and N2O performance audits conducted within the framework of the Global Atmosphere Watch (GAW) quality management system of the World Meteorology Organization (WMO). The results reveal that current spectroscopic measurement techniques have clear advantages with respect to data quality objectives compared to more traditional methods. Further, they allow for a smooth continuation of historic CO and N2O time series.
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.
Sean Crowell, David Baker, Andrew Schuh, Sourish Basu, Andrew R. Jacobson, Frederic Chevallier, Junjie Liu, Feng Deng, Liang Feng, Kathryn McKain, Abhishek Chatterjee, John B. Miller, Britton B. Stephens, Annmarie Eldering, David Crisp, David Schimel, Ray Nassar, Christopher W. O'Dell, Tomohiro Oda, Colm Sweeney, Paul I. Palmer, and Dylan B. A. Jones
Atmos. Chem. Phys., 19, 9797–9831, https://doi.org/10.5194/acp-19-9797-2019, https://doi.org/10.5194/acp-19-9797-2019, 2019
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Space-based retrievals of carbon dioxide offer the potential to provide dense data in regions that are sparsely observed by the surface network. We find that flux estimates that are informed by the Orbiting Carbon Observatory-2 (OCO-2) show different character from that inferred using surface measurements in tropical land regions, particularly in Africa, with a much larger total emission and larger amplitude seasonal cycle.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
Haeyoung Lee, Sang-Ok Han, Sang-Boom Ryoo, Jeong-Soon Lee, and Gang-Woong Lee
Atmos. Chem. Phys., 19, 2149–2163, https://doi.org/10.5194/acp-19-2149-2019, https://doi.org/10.5194/acp-19-2149-2019, 2019
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We introduced our identical systems, which were installed at three S. Korea stations, using CRDS and a drying system. The measurement uncertainty was ~ 0.11 ppm across the stations. CO2 observed in the west of S. Korea was very sensitive to East Asia (e.g., China), indicating that data include CO2 flux information from East Asia. Through long-term comparison to other East Asian stations, it was suggested that they could be affected not only by local vegetation but also by measurement quality.
Stijn Naus, Stephen A. Montzka, Sudhanshu Pandey, Sourish Basu, Ed J. Dlugokencky, and Maarten Krol
Atmos. Chem. Phys., 19, 407–424, https://doi.org/10.5194/acp-19-407-2019, https://doi.org/10.5194/acp-19-407-2019, 2019
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We investigate how the use of a two-box model to describe the troposphere can impact derived results, relative to more complex models. For this, we use a 3-D transport model to tune a two-box model of OH, CH4, and MCF. By comparing the tuned two-box model with a standard model run, we can diagnose and quantify biases inherent to a two-box model. We find strong biases, but these have only a small impact on our final conclusions. However, it is not obvious that this should hold for future studies.
Christine D. Groot Zwaaftink, Stephan Henne, Rona L. Thompson, Edward J. Dlugokencky, Toshinobu Machida, Jean-Daniel Paris, Motoki Sasakawa, Arjo Segers, Colm Sweeney, and Andreas Stohl
Geosci. Model Dev., 11, 4469–4487, https://doi.org/10.5194/gmd-11-4469-2018, https://doi.org/10.5194/gmd-11-4469-2018, 2018
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A Lagrangian particle dispersion model is used to simulate global fields of methane, constrained by observations through nudging. We show that this rather simple and computationally inexpensive method can give results similar to or as good as a computationally expensive Eulerian chemistry transport model with a data assimilation scheme. The three-dimensional methane fields are of interest to applications such as inverse modelling and satellite retrievals.
Xiaona Shang, Meehye Lee, Saehee Lim, Örjan Gustafsson, Gangwoong Lee, and Limseok Chang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-721, https://doi.org/10.5194/acp-2018-721, 2018
Preprint withdrawn
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At Gosan Climate Observatory, the three main sources including anthropogenic pollution, soil dust, and agricultural fertilizer were distinguished for PM10, PM2.5, and PM1, which accounted for 71 % of the total variances for their mass and composition. The mass of mean + σ were comparable to the 90th percentile and the top 10 % implies the substantial impact of soil dust and haze pollution. In PM2.5, the contribution from non-combustion source such as soil dust should not be ignored.
Wei He, Ivar R. van der Velde, Arlyn E. Andrews, Colm Sweeney, John Miller, Pieter Tans, Ingrid T. van der Laan-Luijkx, Thomas Nehrkorn, Marikate Mountain, Weimin Ju, Wouter Peters, and Huilin Chen
Geosci. Model Dev., 11, 3515–3536, https://doi.org/10.5194/gmd-11-3515-2018, https://doi.org/10.5194/gmd-11-3515-2018, 2018
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We have implemented a regional, high-resolution, and computationally attractive carbon dioxide data assimilation system. This system, named CTDAS-Lagrange, is capable of simultaneously optimizing terrestrial biosphere fluxes and the lateral boundary conditions. The CTDAS-Lagrange system can be easily extended to assimilate an additional tracer, e.g., carbonyl sulfide (COS or OCS), for regional estimates of both net and gross carbon fluxes.
Sourish Basu, David F. Baker, Frédéric Chevallier, Prabir K. Patra, Junjie Liu, and John B. Miller
Atmos. Chem. Phys., 18, 7189–7215, https://doi.org/10.5194/acp-18-7189-2018, https://doi.org/10.5194/acp-18-7189-2018, 2018
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CO2 measurements from the global surface network and CO2 estimates from satellites such as the Orbiting Carbon Observatory 2 (OCO-2) are currently used to quantify the surface sources and sinks of CO2, using what we know about atmospheric transport of gases. In this work, we quantify the uncertainties in those surface source/sink estimates that stem from errors in our atmospheric transport models, using an observing system simulation experiment (OSSE).
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.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Peter Bergamaschi, Ute Karstens, Alistair J. Manning, Marielle Saunois, Aki Tsuruta, Antoine Berchet, Alexander T. Vermeulen, Tim Arnold, Greet Janssens-Maenhout, Samuel Hammer, Ingeborg Levin, Martina Schmidt, Michel Ramonet, Morgan Lopez, Jost Lavric, Tuula Aalto, Huilin Chen, Dietrich G. Feist, Christoph Gerbig, László Haszpra, Ove Hermansen, Giovanni Manca, John Moncrieff, Frank Meinhardt, Jaroslaw Necki, Michal Galkowski, Simon O'Doherty, Nina Paramonova, Hubertus A. Scheeren, Martin Steinbacher, and Ed Dlugokencky
Atmos. Chem. Phys., 18, 901–920, https://doi.org/10.5194/acp-18-901-2018, https://doi.org/10.5194/acp-18-901-2018, 2018
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European methane (CH4) emissions are estimated for 2006–2012 using atmospheric in situ measurements from 18 European monitoring stations and 7 different inverse models. Our analysis highlights the potential significant contribution of natural emissions from wetlands (including peatlands and wet soils) to the total European emissions. The top-down estimates of total EU-28 CH4 emissions are broadly consistent with the sum of reported anthropogenic CH4 emissions and the estimated natural emissions.
Ivar R. van der Velde, John B. Miller, Michiel K. van der Molen, Pieter P. Tans, Bruce H. Vaughn, James W. C. White, Kevin Schaefer, and Wouter Peters
Geosci. Model Dev., 11, 283–304, https://doi.org/10.5194/gmd-11-283-2018, https://doi.org/10.5194/gmd-11-283-2018, 2018
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We explored an inverse modeling technique to interpret global atmospheric measurements of CO2 and the ratio of its stable carbon isotopes (δ13C). We detected the possible underestimation of drought stress in biosphere models after applying combined atmospheric CO2 and δ13C constraints. This study highlights the importance of improving the representation of the biosphere in carbon–climate models, in particular in a world where droughts become more extreme and more frequent.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Xin Lan, Pieter Tans, Colm Sweeney, Arlyn Andrews, Andrew Jacobson, Molly Crotwell, Edward Dlugokencky, Jonathan Kofler, Patricia Lang, Kirk Thoning, and Sonja Wolter
Atmos. Chem. Phys., 17, 15151–15165, https://doi.org/10.5194/acp-17-15151-2017, https://doi.org/10.5194/acp-17-15151-2017, 2017
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We analyze spatial patterns of column CO2 over North America using well-calibrated aircraft and tall tower measurements. We find that the long-term averaged spatial gradients of column CO2 across North America show a smooth pattern that mainly reflects the large-scale circulation. Our results can serve as a good reference for evaluating current and future column CO2 retrievals from both ground and satellite platforms.
Jocelyn C. Turnbull, Sara E. Mikaloff Fletcher, India Ansell, Gordon W. Brailsford, Rowena C. Moss, Margaret W. Norris, and Kay Steinkamp
Atmos. Chem. Phys., 17, 14771–14784, https://doi.org/10.5194/acp-17-14771-2017, https://doi.org/10.5194/acp-17-14771-2017, 2017
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We present a 60-year record of radiocarbon in carbon dioxide (14CO2) from Wellington New Zealand. It records the atmospheric 14C “bomb spike” and decline as bomb 14C moved through the carbon cycle and fossil fuel emissions increased. The bomb peak is lower and 1.4 years later than in the Northern Hemisphere. Since the early 2000s, Wellington 14CO2 has been elevated above the Northern Hemisphere, possibly due to a reinvigorated Southern Ocean carbon sink.
Demerval S. Moreira, Karla M. Longo, Saulo R. Freitas, Marcia A. Yamasoe, Lina M. Mercado, Nilton E. Rosário, Emauel Gloor, Rosane S. M. Viana, John B. Miller, Luciana V. Gatti, Kenia T. Wiedemann, Lucas K. G. Domingues, and Caio C. S. Correia
Atmos. Chem. Phys., 17, 14785–14810, https://doi.org/10.5194/acp-17-14785-2017, https://doi.org/10.5194/acp-17-14785-2017, 2017
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Fire in the Amazon forest produces a large amount of smoke that is released into the atmosphere and covers a large portion of South America for about 3 months each year. The smoke affects the energy and CO2 budgets. Using a numerical atmospheric model, we demonstrated that the smoke changes the forest from a source to a sink of CO2 to the atmosphere. The smoke ultimately acts to at least partially compensate for the forest carbon lost due to fire emissions.
Jeong Sik Lim, Miyeon Park, Jinbok Lee, and Jeongsoon Lee
Atmos. Meas. Tech., 10, 4613–4621, https://doi.org/10.5194/amt-10-4613-2017, https://doi.org/10.5194/amt-10-4613-2017, 2017
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Effect of background gas composition on the spectroscopic measurement of CO2 concentration at ambient levels has been investigated. The wavelength-scanned cavity ring-down spectroscopy was employed to explore the spectral line shape of CO2 at 1603 nm. It is revealed that the instrument response should be corrected with respect to a total pressure broadening coefficient given by a matrix composition. The correction method is validated by high accurate gravimetric standard gas mixture.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Ray Weiss, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Atmos. Chem. Phys., 17, 11135–11161, https://doi.org/10.5194/acp-17-11135-2017, https://doi.org/10.5194/acp-17-11135-2017, 2017
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Following the Global Methane Budget 2000–2012 published in Saunois et al. (2016), we use the same dataset of bottom-up and top-down approaches to discuss the variations in methane emissions over the period 2000–2012. The changes in emissions are discussed both in terms of trends and quasi-decadal changes. The ensemble gathered here allows us to synthesise the robust changes in terms of regional and sectorial contributions to the increasing methane emissions.
Jihyun Han, Meehye Lee, Xiaona Shang, Gangwoong Lee, and Louisa K. Emmons
Atmos. Chem. Phys., 17, 10619–10631, https://doi.org/10.5194/acp-17-10619-2017, https://doi.org/10.5194/acp-17-10619-2017, 2017
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Peroxyacetyl nitrate (PAN) was first measured at Gosan Climate Observatory during the fall of 2010, when PAN was better correlated with PM10 than with O3. In particular, PAN and O3 concentrations were greatly elevated in haze and the Beijing plume and much higher than those from model simulation. This study highlights the decoupling of PAN from O3 in Chinese outflows and suggests PAN as a potential indicator of overall aerosol formation in aged air masses impacted by biomass burning.
Thibaud Thonat, Marielle Saunois, Philippe Bousquet, Isabelle Pison, Zeli Tan, Qianlai Zhuang, Patrick M. Crill, Brett F. Thornton, David Bastviken, Ed J. Dlugokencky, Nikita Zimov, Tuomas Laurila, Juha Hatakka, Ove Hermansen, and Doug E. J. Worthy
Atmos. Chem. Phys., 17, 8371–8394, https://doi.org/10.5194/acp-17-8371-2017, https://doi.org/10.5194/acp-17-8371-2017, 2017
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Atmospheric methane simulations in the Arctic have been made for 2012 and compared to continuous observations at six measurement sites. All methane sources significantly affect the measurements at all stations, at least at the synoptic scale, except for biomass burning. An appropriate modelling framework combined with continuous observations of atmospheric methane enables us to gain knowledge on regional methane sources, including those which are usually poorly represented, such as freshwater.
Kristal R. Verhulst, Anna Karion, Jooil Kim, Peter K. Salameh, Ralph F. Keeling, Sally Newman, John Miller, Christopher Sloop, Thomas Pongetti, Preeti Rao, Clare Wong, Francesca M. Hopkins, Vineet Yadav, Ray F. Weiss, Riley M. Duren, and Charles E. Miller
Atmos. Chem. Phys., 17, 8313–8341, https://doi.org/10.5194/acp-17-8313-2017, https://doi.org/10.5194/acp-17-8313-2017, 2017
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We present the first carbon dioxide (CO2) and methane (CH4) measurements from an extensive surface network as part of the Los Angeles Megacity Carbon Project. We describe methods that are essential for understanding carbon fluxes from complex urban environments. CO2 and CH4 levels are spatially and temporally variable, with urban sites showing significant enhancements relative to background. In 2015, the median afternoon enhancement near downtown Los Angeles was ~15 ppm CO2 and ~80 ppb CH4.
Liang Feng, Paul I. Palmer, Hartmut Bösch, Robert J. Parker, Alex J. Webb, Caio S. C. Correia, Nicholas M. Deutscher, Lucas G. Domingues, Dietrich G. Feist, Luciana V. Gatti, Emanuel Gloor, Frank Hase, Rigel Kivi, Yi Liu, John B. Miller, Isamu Morino, Ralf Sussmann, Kimberly Strong, Osamu Uchino, Jing Wang, and Andreas Zahn
Atmos. Chem. Phys., 17, 4781–4797, https://doi.org/10.5194/acp-17-4781-2017, https://doi.org/10.5194/acp-17-4781-2017, 2017
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We use the GEOS-Chem global 3-D model of atmospheric chemistry and transport and an ensemble Kalman filter to simultaneously infer regional fluxes of methane (CH4) and carbon dioxide (CO2) directly from GOSAT retrievals of XCH4:XCO2, using sparse ground-based CH4 and CO2 mole fraction data to anchor the ratio. Our results show that assimilation of GOSAT data significantly reduced the posterior uncertainty and changed the a priori spatial distribution of CH4 emissions.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Ed Dlugokencky, Angel J. Gomez-Pelaez, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, Jgor Arduini, Francesco Apadula, Christoph Gerbig, Dietrich G. Feist, Rigel Kivi, Yukio Yoshida, and Wouter Peters
Geosci. Model Dev., 10, 1261–1289, https://doi.org/10.5194/gmd-10-1261-2017, https://doi.org/10.5194/gmd-10-1261-2017, 2017
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In this study, we found that the average global methane emission for 2000–2012, estimated by the CTE-CH4 model, was 516±51 Tg CH4 yr-1, and the estimates for 2007–2012 were 4 % larger than for 2000–2006. The model estimates are sensitive to inputs and setups, but according to sensitivity tests the study suggests that the increase in atmospheric methane concentrations during 21st century was due to an increase in emissions from the 35S-EQ latitudinal bands.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751, https://doi.org/10.5194/essd-8-697-2016, https://doi.org/10.5194/essd-8-697-2016, 2016
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An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
Zeli Tan, Qianlai Zhuang, Daven K. Henze, Christian Frankenberg, Ed Dlugokencky, Colm Sweeney, Alexander J. Turner, Motoki Sasakawa, and Toshinobu Machida
Atmos. Chem. Phys., 16, 12649–12666, https://doi.org/10.5194/acp-16-12649-2016, https://doi.org/10.5194/acp-16-12649-2016, 2016
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Methane emissions from the pan-Arctic could be important in understanding the global carbon cycle but are still poorly constrained to date. This study demonstrated that satellite retrievals can be used to reduce the uncertainty of the estimates of these emissions. We also provided additional evidence for the existence of large methane emissions from pan-Arctic lakes in the Siberian yedoma permafrost region. We found that biogeochemical models should be improved for better estimates.
Congsheng Fu, Xuhui Lee, Timothy J. Griffis, Edward J. Dlugokencky, and Arlyn E. Andrews
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-761, https://doi.org/10.5194/acp-2016-761, 2016
Revised manuscript not accepted
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To the best of our knowledge, no modeling studies have been published on the relationship between the spatial characteristics of agricultural N2O emissions and the atmospheric N2O mixing ratio at the regional scale. To fill this gap, we proposed a simple inverse analysis method based on tower measurements and an Eulerian model. According to our study, the N2O emissions from the U. S. Corn Belt is clearly estimated by IPCC, and such underestimate is not dependent on tower measurement location.
M. N. Deeter, S. Martínez-Alonso, L. V. Gatti, M. Gloor, J. B. Miller, L. G. Domingues, and C. S. C. Correia
Atmos. Meas. Tech., 9, 3999–4012, https://doi.org/10.5194/amt-9-3999-2016, https://doi.org/10.5194/amt-9-3999-2016, 2016
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Satellite methods allow biomass burning emissions to be accurately quantified with high spatial and temporal resolution. With that ultimate goal, we analyze satellite retrievals of carbon monoxide from the MOPITT instrument over the Amazon Basin. Validation results for four Amazonian sites indicate a significant negative bias in retrieved lower-tropospheric CO concentrations. The interannual variability of biomass burning emissions from 2000 to 2015 is also studied using the MOPITT record.
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
Sourish Basu, John Bharat Miller, and Scott Lehman
Atmos. Chem. Phys., 16, 5665–5683, https://doi.org/10.5194/acp-16-5665-2016, https://doi.org/10.5194/acp-16-5665-2016, 2016
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We present a dual tracer atmospheric inversion technique to separately estimate biospheric and fossil fuel CO2 fluxes from atmospheric measurements of CO2 and 14CO2. In addition to estimating monthly regional fossil fuel fluxes of CO2, this system can also reduce biases in biospheric fluxes that arise in a traditional CO2 inversion from prescribing a fixed but inaccurate fossil fuel flux.
Elizabeth D. Keller, Jocelyn C. Turnbull, and Margaret W. Norris
Atmos. Chem. Phys., 16, 5481–5495, https://doi.org/10.5194/acp-16-5481-2016, https://doi.org/10.5194/acp-16-5481-2016, 2016
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We examine the utility of tree ring 14C archives for detecting long-term changes in fossil CO2 emissions from a point source using six years of observations from two trees near the Kapuni Gas Treatment Plant in New Zealand. Pairing these observations with an atmospheric transport model, we quantify the minimum amount of change in annual emissions that it would be possible to detect in new samples representing averages over one, two, and four years.
Anna Karion, Colm Sweeney, John B. Miller, Arlyn E. Andrews, Roisin Commane, Steven Dinardo, John M. Henderson, Jacob Lindaas, John C. Lin, Kristina A. Luus, Tim Newberger, Pieter Tans, Steven C. Wofsy, Sonja Wolter, and Charles E. Miller
Atmos. Chem. Phys., 16, 5383–5398, https://doi.org/10.5194/acp-16-5383-2016, https://doi.org/10.5194/acp-16-5383-2016, 2016
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Northern high-latitude carbon sources and sinks, including those resulting from degrading permafrost, are thought to be sensitive to the rapidly warming climate. Here we use carbon dioxide and methane measurements from a tower near Fairbanks AK to investigate regional Alaskan fluxes of CO2 and CH4 for 2012–2014.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
Antoine Berchet, Philippe Bousquet, Isabelle Pison, Robin Locatelli, Frédéric Chevallier, Jean-Daniel Paris, Ed J. Dlugokencky, Tuomas Laurila, Juha Hatakka, Yrjo Viisanen, Doug E. J. Worthy, Euan Nisbet, Rebecca Fisher, James France, David Lowry, Viktor Ivakhov, and Ove Hermansen
Atmos. Chem. Phys., 16, 4147–4157, https://doi.org/10.5194/acp-16-4147-2016, https://doi.org/10.5194/acp-16-4147-2016, 2016
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We propose insights based on atmospheric observations around the Arctic circle to evaluate estimates of methane emissions to the atmosphere from the East Siberian Arctic Shelf. Based on a comprehensive statistical analysis of the observations and of high-resolution transport simulations, annual methane emissions from ESAS are estimated to range from 0.0 to 4.5 TgCH4 yr−1, with a maximum in summer and very low emissions in winter.
Scot M. Miller, Roisin Commane, Joe R. Melton, Arlyn E. Andrews, Joshua Benmergui, Edward J. Dlugokencky, Greet Janssens-Maenhout, Anna M. Michalak, Colm Sweeney, and Doug E. J. Worthy
Biogeosciences, 13, 1329–1339, https://doi.org/10.5194/bg-13-1329-2016, https://doi.org/10.5194/bg-13-1329-2016, 2016
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We use atmospheric data from the US and Canada to examine seven wetland methane flux estimates. Relative to existing estimates, we find a methane source that is smaller in magnitude with a broader seasonal cycle. Furthermore, we estimate the largest fluxes over the Hudson Bay Lowlands, a spatial distribution that differs from commonly used remote sensing estimates of wetland location.
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
A. Berchet, I. Pison, F. Chevallier, J.-D. Paris, P. Bousquet, J.-L. Bonne, M. Y. Arshinov, B. D. Belan, C. Cressot, D. K. Davydov, E. J. Dlugokencky, A. V. Fofonov, A. Galanin, J. Lavrič, T. Machida, R. Parker, M. Sasakawa, R. Spahni, B. D. Stocker, and J. Winderlich
Biogeosciences, 12, 5393–5414, https://doi.org/10.5194/bg-12-5393-2015, https://doi.org/10.5194/bg-12-5393-2015, 2015
L. Molina, G. Broquet, P. Imbach, F. Chevallier, B. Poulter, D. Bonal, B. Burban, M. Ramonet, L. V. Gatti, S. C. Wofsy, J. W. Munger, E. Dlugokencky, and P. Ciais
Atmos. Chem. Phys., 15, 8423–8438, https://doi.org/10.5194/acp-15-8423-2015, https://doi.org/10.5194/acp-15-8423-2015, 2015
A. P. Ballantyne, R. Andres, R. Houghton, B. D. Stocker, R. Wanninkhof, W. Anderegg, L. A. Cooper, M. DeGrandpre, P. P. Tans, J. B. Miller, C. Alden, and J. W. C. White
Biogeosciences, 12, 2565–2584, https://doi.org/10.5194/bg-12-2565-2015, https://doi.org/10.5194/bg-12-2565-2015, 2015
J. M. Henderson, J. Eluszkiewicz, M. E. Mountain, T. Nehrkorn, R. Y.-W. Chang, A. Karion, J. B. Miller, C. Sweeney, N. Steiner, S. C. Wofsy, and C. E. Miller
Atmos. Chem. Phys., 15, 4093–4116, https://doi.org/10.5194/acp-15-4093-2015, https://doi.org/10.5194/acp-15-4093-2015, 2015
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This paper describes the atmospheric modeling that underlies the science analysis for the NASA Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). Summary statistics of the WRF meteorological model performance on a 3.3 km grid indicate good overall agreement with surface and radiosonde observations. The high quality of the WRF meteorological fields inspires confidence in their use to drive the STILT transport model for the purpose of computing surface influence fields (“footprints”).
A. Ghosh, P. K. Patra, K. Ishijima, T. Umezawa, A. Ito, D. M. Etheridge, S. Sugawara, K. Kawamura, J. B. Miller, E. J. Dlugokencky, P. B. Krummel, P. J. Fraser, L. P. Steele, R. L. Langenfelds, C. M. Trudinger, J. W. C. White, B. Vaughn, T. Saeki, S. Aoki, and T. Nakazawa
Atmos. Chem. Phys., 15, 2595–2612, https://doi.org/10.5194/acp-15-2595-2015, https://doi.org/10.5194/acp-15-2595-2015, 2015
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Atmospheric CH4 increased from 900ppb to 1800ppb during the period 1900–2010 at a rate unprecedented in any observational records. We use bottom-up emissions and a chemistry-transport model to simulate CH4. The optimized global total CH4 emission, estimated from the model–observation differences, increased at fastest rate during 1940–1990. Using δ13C of CH4 measurements we attribute this emission increase to biomass burning. Total CH4 lifetime is shortened by 4% over the simulation period.
P. Bergamaschi, M. Corazza, U. Karstens, M. Athanassiadou, R. L. Thompson, I. Pison, A. J. Manning, P. Bousquet, A. Segers, A. T. Vermeulen, G. Janssens-Maenhout, M. Schmidt, M. Ramonet, F. Meinhardt, T. Aalto, L. Haszpra, J. Moncrieff, M. E. Popa, D. Lowry, M. Steinbacher, A. Jordan, S. O'Doherty, S. Piacentino, and E. Dlugokencky
Atmos. Chem. Phys., 15, 715–736, https://doi.org/10.5194/acp-15-715-2015, https://doi.org/10.5194/acp-15-715-2015, 2015
M. Alexe, P. Bergamaschi, A. Segers, R. Detmers, A. Butz, O. Hasekamp, S. Guerlet, R. Parker, H. Boesch, C. Frankenberg, R. A. Scheepmaker, E. Dlugokencky, C. Sweeney, S. C. Wofsy, and E. A. Kort
Atmos. Chem. Phys., 15, 113–133, https://doi.org/10.5194/acp-15-113-2015, https://doi.org/10.5194/acp-15-113-2015, 2015
A. Fraser, P. I. Palmer, L. Feng, H. Bösch, R. Parker, E. J. Dlugokencky, P. B. Krummel, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 12883–12895, https://doi.org/10.5194/acp-14-12883-2014, https://doi.org/10.5194/acp-14-12883-2014, 2014
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Satellite measurements of CO2 and CH4 can be subject to regional systematic errors that can consequently compromise their ability to infer robust flux estimates of these two gases. We develop a method to use retrieved ratios of CH4 and CO2 that are less affected by systematic error. We show that additional in situ data are needed to anchor these observed ratios so they can simultaneously infer fluxes of CO2 and CH4. We argue the ratio data will provide a more faithful description of true fluxes.
I. R. van der Velde, J. B. Miller, K. Schaefer, G. R. van der Werf, M. C. Krol, and W. Peters
Biogeosciences, 11, 6553–6571, https://doi.org/10.5194/bg-11-6553-2014, https://doi.org/10.5194/bg-11-6553-2014, 2014
L. Bruhwiler, E. Dlugokencky, K. Masarie, M. Ishizawa, A. Andrews, J. Miller, C. Sweeney, P. Tans, and D. Worthy
Atmos. Chem. Phys., 14, 8269–8293, https://doi.org/10.5194/acp-14-8269-2014, https://doi.org/10.5194/acp-14-8269-2014, 2014
P. Ciais, A. J. Dolman, A. Bombelli, R. Duren, A. Peregon, P. J. Rayner, C. Miller, N. Gobron, G. Kinderman, G. Marland, N. Gruber, F. Chevallier, R. J. Andres, G. Balsamo, L. Bopp, F.-M. Bréon, G. Broquet, R. Dargaville, T. J. Battin, A. Borges, H. Bovensmann, M. Buchwitz, J. Butler, J. G. Canadell, R. B. Cook, R. DeFries, R. Engelen, K. R. Gurney, C. Heinze, M. Heimann, A. Held, M. Henry, B. Law, S. Luyssaert, J. Miller, T. Moriyama, C. Moulin, R. B. Myneni, C. Nussli, M. Obersteiner, D. Ojima, Y. Pan, J.-D. Paris, S. L. Piao, B. Poulter, S. Plummer, S. Quegan, P. Raymond, M. Reichstein, L. Rivier, C. Sabine, D. Schimel, O. Tarasova, R. Valentini, R. Wang, G. van der Werf, D. Wickland, M. Williams, and C. Zehner
Biogeosciences, 11, 3547–3602, https://doi.org/10.5194/bg-11-3547-2014, https://doi.org/10.5194/bg-11-3547-2014, 2014
R. L. Thompson, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, P. K. Patra, P. Bergamaschi, F. Chevallier, E. Dlugokencky, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, A. Vermeulen, Y. Tohjima, A. Jordan, L. Haszpra, M. Steinbacher, S. Van der Laan, T. Aalto, F. Meinhardt, M. E. Popa, J. Moncrieff, and P. Bousquet
Atmos. Chem. Phys., 14, 6177–6194, https://doi.org/10.5194/acp-14-6177-2014, https://doi.org/10.5194/acp-14-6177-2014, 2014
E. Saikawa, R. G. Prinn, E. Dlugokencky, K. Ishijima, G. S. Dutton, B. D. Hall, R. Langenfelds, Y. Tohjima, T. Machida, M. Manizza, M. Rigby, S. O'Doherty, P. K. Patra, C. M. Harth, R. F. Weiss, P. B. Krummel, M. van der Schoot, P. J. Fraser, L. P. Steele, S. Aoki, T. Nakazawa, and J. W. Elkins
Atmos. Chem. Phys., 14, 4617–4641, https://doi.org/10.5194/acp-14-4617-2014, https://doi.org/10.5194/acp-14-4617-2014, 2014
R. L. Thompson, P. K. Patra, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, C. Wilson, P. Bergamaschi, E. Dlugokencky, C. Sweeney, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, M. Saunois, M. Chipperfield, and P. Bousquet
Atmos. Chem. Phys., 14, 4349–4368, https://doi.org/10.5194/acp-14-4349-2014, https://doi.org/10.5194/acp-14-4349-2014, 2014
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
A. E. Andrews, J. D. Kofler, M. E. Trudeau, J. C. Williams, D. H. Neff, K. A. Masarie, D. Y. Chao, D. R. Kitzis, P. C. Novelli, C. L. Zhao, E. J. Dlugokencky, P. M. Lang, M. J. Crotwell, M. L. Fischer, M. J. Parker, J. T. Lee, D. D. Baumann, A. R. Desai, C. O. Stanier, S. F. J. De Wekker, D. E. Wolfe, J. W. Munger, and P. P. Tans
Atmos. Meas. Tech., 7, 647–687, https://doi.org/10.5194/amt-7-647-2014, https://doi.org/10.5194/amt-7-647-2014, 2014
M. E. Park, C. H. Song, R. S. Park, J. Lee, J. Kim, S. Lee, J.-H. Woo, G. R. Carmichael, T. F. Eck, B. N. Holben, S.-S. Lee, C. K. Song, and Y. D. Hong
Atmos. Chem. Phys., 14, 659–674, https://doi.org/10.5194/acp-14-659-2014, https://doi.org/10.5194/acp-14-659-2014, 2014
C. Cressot, F. Chevallier, P. Bousquet, C. Crevoisier, E. J. Dlugokencky, A. Fortems-Cheiney, C. Frankenberg, R. Parker, I. Pison, R. A. Scheepmaker, S. A. Montzka, P. B. Krummel, L. P. Steele, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 577–592, https://doi.org/10.5194/acp-14-577-2014, https://doi.org/10.5194/acp-14-577-2014, 2014
B. W. LaFranchi, G. Pétron, J. B. Miller, S. J. Lehman, A. E. Andrews, E. J. Dlugokencky, B. Hall, B. R. Miller, S. A. Montzka, W. Neff, P. C. Novelli, C. Sweeney, J. C. Turnbull, D. E. Wolfe, P. P. Tans, K. R. Gurney, and T. P. Guilderson
Atmos. Chem. Phys., 13, 11101–11120, https://doi.org/10.5194/acp-13-11101-2013, https://doi.org/10.5194/acp-13-11101-2013, 2013
V. V. S. S. Sarma, A. Lenton, R. M. Law, N. Metzl, P. K. Patra, S. Doney, I. D. Lima, E. Dlugokencky, M. Ramonet, and V. Valsala
Biogeosciences, 10, 7035–7052, https://doi.org/10.5194/bg-10-7035-2013, https://doi.org/10.5194/bg-10-7035-2013, 2013
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
M. Lopez, M. Schmidt, M. Delmotte, A. Colomb, V. Gros, C. Janssen, S. J. Lehman, D. Mondelain, O. Perrussel, M. Ramonet, I. Xueref-Remy, and P. Bousquet
Atmos. Chem. Phys., 13, 7343–7358, https://doi.org/10.5194/acp-13-7343-2013, https://doi.org/10.5194/acp-13-7343-2013, 2013
A. Fraser, P. I. Palmer, L. Feng, H. Boesch, A. Cogan, R. Parker, E. J. Dlugokencky, P. J. Fraser, P. B. Krummel, R. L. Langenfelds, S. O'Doherty, R. G. Prinn, L. P. Steele, M. van der Schoot, and R. F. Weiss
Atmos. Chem. Phys., 13, 5697–5713, https://doi.org/10.5194/acp-13-5697-2013, https://doi.org/10.5194/acp-13-5697-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
In situ ozone production is highly sensitive to volatile organic compounds in Delhi, India
Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions
Dynamics of gaseous oxidized mercury at Villum Research Station during the High Arctic summer
Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes
Opinion: Papers that shaped tropospheric chemistry
Measurement report: Source apportionment of volatile organic compounds at the remote high-altitude Maïdo observatory
Shipborne measurements of methane and carbon dioxide in the Middle East and Mediterranean areas and the contribution from oil and gas emissions
Observations of iodine monoxide over three summers at the Indian Antarctic bases of Bharati and Maitri
Unexplored volatile organic compound emitted from petrochemical facilities: implications for ozone production and atmospheric chemistry
Atmospheric gaseous hydrochloric and hydrobromic acid in urban Beijing, China: detection, source identification and potential atmospheric impacts
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom
Spectrometric measurements of atmospheric propane (C3H8)
Air–sea exchange of acetone, acetaldehyde, DMS and isoprene at a UK coastal site
Measurement report: Emissions of intermediate-volatility organic compounds from vehicles under real-world driving conditions in an urban tunnel
Investigations on the anthropogenic reversal of the natural ozone gradient between northern and southern midlatitudes
Measurement report: Molecular composition and volatility of gaseous organic compounds in a boreal forest – from volatile organic compounds to highly oxygenated organic molecules
Boreal forest fire CO and CH4 emission factors derived from tower observations in Alaska during the extreme fire season of 2015
Chemical characterization of oxygenated organic compounds in the gas phase and particle phase using iodide CIMS with FIGAERO in urban air
New approach to evaluate satellite-derived XCO2 over oceans by integrating ship and aircraft observations
Central role of nitric oxide in ozone production in the upper tropical troposphere over the Atlantic Ocean and western Africa
Sesquiterpenes and oxygenated sesquiterpenes dominate the VOC (C5–C20) emissions of downy birches
Measurement report: Online measurement of gas-phase nitrated phenols utilizing a CI-LToF-MS: primary sources and secondary formation
Measurement report: In situ observations of deep convection without lightning during the tropical cyclone Florence 2018
Measurement Report: Variability in the composition of biogenic volatile organic compounds in a southeastern US forest and their role in atmospheric reactivity
Reactive nitrogen around the Arabian Peninsula and in the Mediterranean Sea during the 2017 AQABA ship campaign
Stratospheric carbon isotope fractionation and tropospheric histories of CFC-11, CFC-12, and CFC-113 isotopologues
Isotopic compositions of atmospheric total gaseous mercury in 10 Chinese cities and implications for land surface emissions
Formation of condensable organic vapors from anthropogenic and biogenic VOCs is strongly perturbed by NOx in eastern China
Observations of speciated isoprene nitrates in Beijing: implications for isoprene chemistry
Contributions 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) 2016
Total OH reactivity over the Amazon rainforest: variability with temperature, wind, rain, altitude, time of day, season, and an overall budget closure
Where there is smoke there is mercury: Assessing boreal forest fire mercury emissions using aircraft and highlighting uncertainties associated with upscaling emissions estimates
Temporary pause in the growth of atmospheric ethane and propane in 2015–2018
Formation of nighttime sulfuric acid from the ozonolysis of alkenes in Beijing
Spatiotemporal variation, sources, and secondary transformation potential of volatile organic compounds in Xi'an, China
Identifying and quantifying source contributions of air quality contaminants during unconventional shale gas extraction
Observed decreases in on-road CO2 concentrations in Beijing during COVID-19 restrictions
Investigation of several proxies to estimate sulfuric acid concentration under volcanic plume conditions
Measurement report: Exploring NH3 behavior in urban and suburban Beijing: comparison and implications
Atmospheric organic vapors in two European pine forests measured by a Vocus PTR-TOF: insights into monoterpene and sesquiterpene oxidation processes
Speciation of VOC emissions related to offshore North Sea oil and gas production
Origins and characterization of CO and O3 in the African upper troposphere
Halogen activation in the plume of Masaya volcano: field observations and box model investigations
Decoupling of urban CO2 and air pollutant emission reductions during the European SARS-CoV-2 lockdown
Atmospheric VOC measurements at a High Arctic site: characteristics and source apportionment
Evaluating the sensitivity of radical chemistry and ozone formation to ambient VOCs and NOx in Beijing
Global trends and European emissions of tetrafluoromethane (CF4), hexafluoroethane (C2F6) and octafluoropropane (C3F8)
Non-target and suspect characterisation of organic contaminants in ambient air – Part 1: Combining a novel sample clean-up method with comprehensive two-dimensional gas chromatography
Low-NO atmospheric oxidation pathways in a polluted megacity
Seasonal variation and origins of volatile organic compounds observed during 2 years at a western Mediterranean remote background site (Ersa, Cape Corsica)
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, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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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, https://doi.org/10.5194/acp-21-13333-2021, https://doi.org/10.5194/acp-21-13333-2021, 2021
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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, https://doi.org/10.5194/acp-21-13287-2021, https://doi.org/10.5194/acp-21-13287-2021, 2021
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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, 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.
Paul S. Monks, A. R. Ravishankara, Erika von Schneidemesser, and Roberto Sommariva
Atmos. Chem. Phys., 21, 12909–12948, https://doi.org/10.5194/acp-21-12909-2021, https://doi.org/10.5194/acp-21-12909-2021, 2021
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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, https://doi.org/10.5194/acp-21-12965-2021, https://doi.org/10.5194/acp-21-12965-2021, 2021
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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, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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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, https://doi.org/10.5194/acp-21-11829-2021, https://doi.org/10.5194/acp-21-11829-2021, 2021
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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, https://doi.org/10.5194/acp-21-11505-2021, https://doi.org/10.5194/acp-21-11505-2021, 2021
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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, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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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, 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.
Geoffrey C. Toon, Jean-Francois L. Blavier, Keeyoon Sung, and Katelyn Yu
Atmos. Chem. Phys., 21, 10727–10743, https://doi.org/10.5194/acp-21-10727-2021, https://doi.org/10.5194/acp-21-10727-2021, 2021
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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, https://doi.org/10.5194/acp-21-10111-2021, https://doi.org/10.5194/acp-21-10111-2021, 2021
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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, https://doi.org/10.5194/acp-21-10005-2021, https://doi.org/10.5194/acp-21-10005-2021, 2021
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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.
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, https://doi.org/10.5194/acp-21-9669-2021, https://doi.org/10.5194/acp-21-9669-2021, 2021
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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.
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, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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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, https://doi.org/10.5194/acp-21-8557-2021, https://doi.org/10.5194/acp-21-8557-2021, 2021
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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, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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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, 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.
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, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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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, https://doi.org/10.5194/acp-21-8045-2021, https://doi.org/10.5194/acp-21-8045-2021, 2021
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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, https://doi.org/10.5194/acp-21-7917-2021, https://doi.org/10.5194/acp-21-7917-2021, 2021
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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, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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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.
Deborah F. McGlynn, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-416, https://doi.org/10.5194/acp-2021-416, 2021
Preprint under review for ACP
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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, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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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, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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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, https://doi.org/10.5194/acp-21-6721-2021, https://doi.org/10.5194/acp-21-6721-2021, 2021
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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.
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. Discuss., https://doi.org/10.5194/acp-2021-364, https://doi.org/10.5194/acp-2021-364, 2021
Revised manuscript accepted for ACP
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Oxygenated organic molecules (OOMs) are the crucial intermediates linking volatile organic compounds to secondary organic aerosol. Here, we investigated OOMs measured by nitrate TOF-CIMS in eastern China, though performing positive matrix factorization on binned mass spectra. We reconstructed more than 1000 molecules from 14 derived PMF factors and identified 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of nitrogen chemistry on OOMs formation in populated areas.
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, https://doi.org/10.5194/acp-21-6315-2021, https://doi.org/10.5194/acp-21-6315-2021, 2021
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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, https://doi.org/10.5194/acp-21-6331-2021, https://doi.org/10.5194/acp-21-6331-2021, 2021
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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, https://doi.org/10.5194/acp-21-6231-2021, https://doi.org/10.5194/acp-21-6231-2021, 2021
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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, https://doi.org/10.5194/acp-21-5635-2021, https://doi.org/10.5194/acp-21-5635-2021, 2021
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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.
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. Discuss., https://doi.org/10.5194/acp-2021-285, https://doi.org/10.5194/acp-2021-285, 2021
Revised manuscript accepted for ACP
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After a multi-decade global decline in atmospheric concentrations of ethane and propane (precursors to 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.
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, https://doi.org/10.5194/acp-21-5499-2021, https://doi.org/10.5194/acp-21-5499-2021, 2021
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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, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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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, https://doi.org/10.5194/acp-21-4729-2021, https://doi.org/10.5194/acp-21-4729-2021, 2021
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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, https://doi.org/10.5194/acp-21-4599-2021, https://doi.org/10.5194/acp-21-4599-2021, 2021
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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, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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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, https://doi.org/10.5194/acp-21-4561-2021, https://doi.org/10.5194/acp-21-4561-2021, 2021
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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, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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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, https://doi.org/10.5194/acp-21-3741-2021, https://doi.org/10.5194/acp-21-3741-2021, 2021
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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.
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. Discuss., https://doi.org/10.5194/acp-2021-115, https://doi.org/10.5194/acp-2021-115, 2021
Revised manuscript accepted for ACP
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African intertropical troposphere is one of the world areas where the increase in ozone mixing ratio is most marked 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.
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393, https://doi.org/10.5194/acp-21-3371-2021, https://doi.org/10.5194/acp-21-3371-2021, 2021
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We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
Christian Lamprecht, Martin Graus, Marcus Striednig, Michael Stichaner, and Thomas Karl
Atmos. Chem. Phys., 21, 3091–3102, https://doi.org/10.5194/acp-21-3091-2021, https://doi.org/10.5194/acp-21-3091-2021, 2021
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The first European SARS-CoV-2 (severe acute respiratory syndrome coronavirus 2) wave and associated lockdown provided a unique sensitivity experiment to study air pollution. We find significantly different emission trajectories between classical air pollution and climate gases (e.g., carbon dioxide). The analysis suggests that European policies, shifting residential, public, and commercial energy demand towards cleaner combustion, have helped to improve air quality more than expected.
Jakob B. Pernov, Rossana Bossi, Thibaut Lebourgeois, Jacob K. Nøjgaard, Rupert Holzinger, Jens L. Hjorth, and Henrik Skov
Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, https://doi.org/10.5194/acp-21-2895-2021, 2021
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Volatile organic compounds (VOCs) are an important constituent in the Arctic atmosphere due to their effect on aerosol and ozone formation. However, an understanding of their sources is lacking. This research presents a multiseason high-time-resolution dataset of VOCs in the Arctic and details their temporal characteristics and source apportionment. Four sources were identified: biomass burning, marine cryosphere, background, and Arctic haze.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
Laura Röhler, Pernilla Bohlin-Nizzetto, Pawel Rostkowski, Roland Kallenborn, and Martin Schlabach
Atmos. Chem. Phys., 21, 1697–1716, https://doi.org/10.5194/acp-21-1697-2021, https://doi.org/10.5194/acp-21-1697-2021, 2021
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A novel non-destructive, sulfuric-acid-free clean-up method for high-volume air samples was developed and evaluated with organic chemicals covering a wide range of polarities (logP 2–11). This method, providing quantitative results of comparable quality to traditional methods, was combined with newly developed data treatment strategies for simultaneous suspect and non-target screening. The application to air samples from southern Norway revealed 90 new potential chemicals of emerging concern.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Cécile Debevec, Stéphane Sauvage, Valérie Gros, Thérèse Salameh, Jean Sciare, François Dulac, and Nadine Locoge
Atmos. Chem. Phys., 21, 1449–1484, https://doi.org/10.5194/acp-21-1449-2021, https://doi.org/10.5194/acp-21-1449-2021, 2021
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This study provides a better characterization of the seasonal variations in VOC sources impacting the western Mediterranean region, based on a comprehensive chemical composition measured over 25 months at a representative receptor site (Ersa) and by determining factors controlling their temporal variations. Some insights into dominant drivers for VOC concentration variations in Europe are also provided, built on comparisons of Ersa observations with the concomitant ones of 17 European sites.
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Short summary
To understand South Korea's CO2 emissions and sinks as well as those of the surrounding region, we used flask-air samples collected for 2 years at Anmyeondo (36.53° N, 126.32° E; 46 m a.s.l.), South Korea, for analysis of observed 14C in atmospheric CO2 as a tracer of fossil fuel CO2 contribution (Cff). Here, we showed our observation result of 14C and Cff. SF6 and CO can be good proxies of Cff in this study, and the ratio of CO to Cff was compared to a bottom-up inventory.
To understand South Korea's CO2 emissions and sinks as well as those of the surrounding region,...
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