Articles | Volume 15, issue 9
11 May 2015
Research article | 11 May 2015
Origin of springtime ozone enhancements in the lower troposphere over Beijing: in situ measurements and model analysis
J. Huang et al.
No articles found.
Brendan Byrne, David F. Baker, Sourish Basu, Michael Bertolacci, Kevin W. Bowman, Dustin Carroll, Abhishek Chatterjee, Frédéric Chevallier, Philippe Ciais, Noel Cressie, David Crisp, Sean Crowell, Feng Deng, Zhu Deng, Nicholas M. Deutscher, Manvendra Dubey, Sha Feng, Omaira García, David W. T. Griffith, Benedikt Herkommer, Lei Hu, Andrew R. Jacobson, Rajesh Janardanan, Sujong Jeong, Matthew S. Johnson, Dylan B. A. Jones, Rigel Kivi, Junjie Liu, Zhiqiang Liu, Shamil Maksyutov, John B. Miller, Scot M. Miller, Isamu Morino, Justus Notholt, Tomohiro Oda, Christopher W. O’Dell, Young-Suk Oh, Hirofumi Ohyama, Prabir K. Patra, Hélène Peiro, Christof Petri, Sajeev Philip, David F. Pollard, Benjamin Poulter, Marine Remaud, Andrew Schuh, Mahesh K. Sha, Kei Shiomi, Kimberly Strong, Colm Sweeney, Yao Té, Hanqin Tian, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, John R. Worden, Debra Wunch, Yuanzhi Yao, Jeongmin Yun, Andrew Zammit-Mangion, and Ning Zeng
Earth Syst. Sci. Data Discuss.,
Preprint under review for ESSDShort summary
Changes in the carbon stocks of terrestrial ecosystems result in emissions and removals of CO2. These can be driven by anthropogenic activities (e.g., deforestation), natural processes (e.g., fires) or in response to rising CO2 (e.g., CO2 fertilization). This paper describes a dataset of CO2 emissions and removals derived from atmospheric CO2 observations. This pilot dataset informs current capabilities and future developments towards top-down monitoring and verification systems.
Weichao Han, Tai-Long He, Zhaojun Tang, Min Wang, Dylan Jones, and Zhe Jiang
Geosci. Model Dev., 15, 4225–4237,Short summary
We present an application of a hybrid deep learning (DL) model on prediction of surface CO in China from 2015 to 2020, which utilizes both convolutional neural networks and long short-term memory neural networks. The DL model performance is better than a Kalman filter (KF) system in the training period (2005–2018). Furthermore, the DL model demonstrates good temporal extensibility: the mean bias and correlation coefficients are 95.7 ppb and 0.93 in the test period (2019–2020) over eastern China.
Weilun Zhao, Gang Zhao, Ying Li, Song Guo, Nan Ma, Lizi Tang, Zirui Zhang, and Chunsheng Zhao
Atmos. Meas. Tech. Discuss.,
Preprint under review for AMTShort summary
A new method to determine black carbon mass size distribution (BCMSD) was proposed using size-resolved absorption coefficient measured by an aerodynamic aerosol classifer in tandem with an aethaelometer. This new method fills the gap in the high-time-resolution measurement of BCMSD ranging from upper submicron to larger than 1 micron. This method can be applied to field measurement of BCMSD extensively for better understanding the BC aging and better estimating BC climate effect.
Tai-Long He, Dylan B. A. Jones, Kazuyuki Miyazaki, Kevin W. Bowman, Zhe Jiang, Xiaokang Chen, Rui Li, Yuxiang Zhang, and Kunna Li
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
We use a deep learning (DL) model to estimate Chinese NOx emissions by combining satellite analysis and in situ measuremements. Our results are consistent with conventional analyses of Chinese NOx emissions. Comparison with mobility data shows that the DL model has a better capability to capture changes in NOx. We analyze Chinese NOx emissions during the COVID-19 pandemic period. Our results illustrate the potential utility of DL as a complementary tool for conventional air quality studies.
Kevin J. Sanchez, Bo Zhang, Hongyu Liu, Matthew D. Brown, Ewan C. Crosbie, Francesca Gallo, Johnathan W. Hair, Chris A. Hostetler, Carolyn E. Jordan, Claire E. Robinson, Amy Jo Scarino, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Elizabeth B. Wiggins, Edward L. Winstead, Luke D. Ziemba, Georges Saliba, Savannah L. Lewis, Lynn M. Russell, Patricia K. Quinn, Timothy S. Bates, Jack Porter, Thomas G. Bell, Peter Gaube, Eric S. Saltzman, Michael J. Behrenfeld, and Richard H. Moore
Atmos. Chem. Phys., 22, 2795–2815,Short summary
Atmospheric particle concentrations impact clouds, which strongly impact the amount of sunlight reflected back into space and the overall climate. Measurements of particles over the ocean are rare and expensive to collect, so models are necessary to fill in the gaps by simulating both particle and clouds. However, some measurements are needed to test the accuracy of the models. Here, we measure changes in particles in different weather conditions, which are ideal for comparison with models.
Heba S. Marey, James R. Drummond, Dylan B. A. Jones, Helen Worden, Merritt N. Deeter, John Gille, and Debbie Mao
Atmos. Meas. Tech., 15, 701–719,Short summary
In this study, an analysis has been performed to understand the improvements in observational coverage over Canada in the new MOPITT V9 product. Temporal and spatial analysis of V9 indicates a general coverage gain of 15–20 % relative to V8, which varies regionally and seasonally; e.g., the number of successful MOPITT retrievals in V9 was doubled over Canada in winter. Also, comparison with the corresponding IASI instrument indicated generally good agreement, with about a 5–10 % positive bias.
Sabour Baray, Daniel J. Jacob, Joannes D. Maasakkers, Jian-Xiong Sheng, Melissa P. Sulprizio, Dylan B. A. Jones, A. Anthony Bloom, and Robert McLaren
Atmos. Chem. Phys., 21, 18101–18121,Short summary
We use 2010–2015 surface and satellite observations to disentangle methane from anthropogenic and natural sources in Canada. Using a chemical transport model (GEOS-Chem), the mismatch between modelled and observed methane concentrations can be used to infer emissions according to Bayesian statistics. Compared to prior knowledge, we show higher anthropogenic emissions attributed to energy and/or agriculture in Western Canada and lower natural emissions from Boreal wetlands.
Gang Zhao, Tianyi Tan, Yishu Zhu, Min Hu, and Chunsheng Zhao
Atmos. Chem. Phys., 21, 18055–18063,Short summary
In this study, the black carbon (BC) mixing state index (χ) is developed to quantify the dispersion of ambient black carbon aerosol mixing states based on binary systems of BC and other non-black carbon components. We demonstrate that the BC light absorption enhancement increases with χ for the same MR, which indicates that χ can be employed as a factor to constrain the light absorption enhancement of ambient BC.
Erika Brattich, Hongyu Liu, Bo Zhang, Miguel Ángel Hernández-Ceballos, Jussi Paatero, Darko Sarvan, Vladimir Djurdjevic, Laura Tositti, and Jelena Ajtić
Atmos. Chem. Phys., 21, 17927–17951,Short summary
In this study we analyse the output of a chemistry and transport model together with observations of different meteorological and compositional variables to demonstrate the link between sudden stratospheric warming and transport of stratospheric air to the surface in the subpolar regions of Europe during the cold season. Our findings have particular implications for atmospheric composition since climate projections indicate more frequent sudden stratospheric warming under a warmer climate.
Hazel Vernier, Neeraj Rastogi, Hongyu Liu, Amit Kumar Pandit, Kris Bedka, Anil Patel, Madineni Venkat Ratnam, Buduru Suneel Kumar, Bo Zhang, Harish Gadhavi, Frank G. Wienhold, Gwenael Berthet, and Jean-Paul Vernier
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The chemical composition of the stratospheric aerosols collected onboard high-altitude balloons above the Summer Asian Monsoon reveals the presence of nitrate/nitrite. Using numerical simulations and satellite observations, we found that pollution as well as lightinning could explain some of our observations.
Hossein Dadashazar, Majid Alipanah, Miguel Ricardo A. Hilario, Ewan Crosbie, Simon Kirschler, Hongyu Liu, Richard H. Moore, Andrew J. Peters, Amy Jo Scarino, Michael Shook, K. Lee Thornhill, Christiane Voigt, Hailong Wang, Edward Winstead, Bo Zhang, Luke Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 21, 16121–16141,Short summary
This study investigates precipitation impacts on long-range transport of North American outflow over the western North Atlantic Ocean (WNAO). Results demonstrate that precipitation scavenging plays a significant role in modifying surface aerosol concentrations over the WNAO, especially in winter and spring due to large-scale scavenging processes. This study highlights how precipitation impacts surface aerosol properties with relevance for other marine regions vulnerable to continental outflow.
Beata Bukosa, Jenny Fisher, Nicholas Deutscher, and Dylan Jones
Geosci. Model Dev. Discuss.,
Revised manuscript not acceptedShort summary
Human activities led to rising levels of greenhouse gases (carbon dioxide (CO2), methane (CH4), carbon monoxide (CO)) in the atmosphere, threatening our future. We use models and measurements to predict and understand the climatological impact of these gases. Here, we describe a new simulation in the GEOS-Chem model that uses a more accurate method to simulate CO2, CH4 and CO, through their chemical dependence. Relative to the original simulations our results agree better with measurements.
Hossein Dadashazar, David Painemal, Majid Alipanah, Michael Brunke, Seethala Chellappan, Andrea F. Corral, Ewan Crosbie, Simon Kirschler, Hongyu Liu, Richard H. Moore, Claire Robinson, Amy Jo Scarino, Michael Shook, Kenneth Sinclair, K. Lee Thornhill, Christiane Voigt, Hailong Wang, Edward Winstead, Xubin Zeng, Luke Ziemba, Paquita Zuidema, and Armin Sorooshian
Atmos. Chem. Phys., 21, 10499–10526,Short summary
This study investigates the seasonal cycle of cloud drop number concentration (Nd) over the western North Atlantic Ocean (WNAO) using multiple datasets. Reasons for the puzzling discrepancy between the seasonal cycles of Nd and aerosol concentration were identified. Results indicate that Nd is highest in winter (when aerosol proxy values are often lowest) due to conditions both linked to cold-air outbreaks and that promote greater droplet activation.
Jie Qiu, Wangshu Tan, Gang Zhao, Yingli Yu, and Chunsheng Zhao
Atmos. Meas. Tech., 14, 4879–4891,Short summary
Considering nephelometers' major problems of a nonideal Lambertian light source and angle truncation, a new correction method based on a machine learning model is proposed. Our method has the advantage of obtaining data with high accuracy while achieving self-correction, which means that researchers can get more accurate scattering coefficients without the need for additional observation data. This method provides a more precise estimation of the aerosol’s direct radiative forcing.
Gang Zhao, Yishu Zhu, Zhijun Wu, Taomou Zong, Jingchuan Chen, Tianyi Tan, Haichao Wang, Xin Fang, Keding Lu, Chunsheng Zhao, and Min Hu
Atmos. Chem. Phys., 21, 9995–10004,Short summary
New particle formation is thought to contribute half of the global cloud condensation nuclei. We find that the new particle formation is more likely to happen in the upper boundary layer than that at the ground, which can be partially explained by the aerosol–radiation interaction. Our study emphasizes the influence of aerosol–radiation interaction on the NPF.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572,Short summary
We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Vikram Khade, Saroja M. Polavarapu, Michael Neish, Pieter L. Houtekamer, Dylan B. A. Jones, Seung-Jong Baek, Tai-Long He, and Sylvie Gravel
Geosci. Model Dev., 14, 2525–2544,Short summary
A new modeling system has been developed at Environment and Climate Change Canada to ingest observations of carbon monoxide (CO) into a coupled weather and constituent transport model. We show that accounting for the uncertainty in surface flux leads to a better estimate of CO distributions. The benefit of assimilating observations from different simulated networks varies with region. This is the first step towards developing a state and flux estimation system for greenhouse gases.
Weilun Zhao, Wangshu Tan, Gang Zhao, Chuanyang Shen, Yingli Yu, and Chunsheng Zhao
Atmos. Meas. Tech., 14, 1319–1331,
Chuanyang Shen, Gang Zhao, and Chunsheng Zhao
Atmos. Meas. Tech., 14, 1293–1301,Short summary
Aerosol hygroscopicity measured by the humidified tandem differential mobility analyzer (HTDMA) is affected by multiply charged particles from two aspects: (1) number contribution and (2) the weakening effect. An algorithm is proposed to do the multi-charge correction and applied to a field measurement. Results show that the difference between corrected and measured size-resolved κ can reach 0.05, highlighting that special attention needs to be paid to the multi-charge effect when using HTDMA.
Betty Croft, Randall V. Martin, Richard H. Moore, Luke D. Ziemba, Ewan C. Crosbie, Hongyu Liu, Lynn M. Russell, Georges Saliba, Armin Wisthaler, Markus Müller, Arne Schiller, Martí Galí, Rachel Y.-W. Chang, Erin E. McDuffie, Kelsey R. Bilsback, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 1889–1916,Short summary
North Atlantic Aerosols and Marine Ecosystems Study measurements combined with GEOS-Chem-TOMAS modeling suggest that several not-well-understood key factors control northwest Atlantic aerosol number and size. These synergetic and climate-relevant factors include particle formation near and above the marine boundary layer top, particle growth by marine secondary organic aerosol on descent, particle formation/growth related to dimethyl sulfide, sea spray aerosol, and ship emissions.
Bo Zhang, Hongyu Liu, James H. Crawford, Gao Chen, T. Duncan Fairlie, Scott Chambers, Chang-Hee Kang, Alastair G. Williams, Kai Zhang, David B. Considine, Melissa P. Sulprizio, and Robert M. Yantosca
Atmos. Chem. Phys., 21, 1861–1887,Short summary
We simulate atmospheric 222Rn using the GEOS-Chem model to improve understanding of 222Rn emissions and characterize convective transport in the model. We demonstrate the potential of a customized global 222Rn emission scenario to improve simulated surface 222Rn concentrations and seasonality. We assess convective transport using observed 222Rn vertical profiles. Results have important implications for using chemical transport models to interpret the transport of trace gases and aerosols.
Shoma Yamanouchi, Camille Viatte, Kimberly Strong, Erik Lutsch, Dylan B. A. Jones, Cathy Clerbaux, Martin Van Damme, Lieven Clarisse, and Pierre-Francois Coheur
Atmos. Meas. Tech., 14, 905–921,Short summary
Ammonia (NH3) is a major source of pollution in the air. As such, there have been increasing efforts to measure the atmospheric abundance of NH3 and its spatial and temporal variability. In this study, long-term measurements of NH3 over Toronto, Canada, derived from multiscale datasets are examined. These NH3 datasets were compared to each other and to a model to better understand NH3 variability and to assess model performance.
Chuanyang Shen, Gang Zhao, Weilun Zhao, Ping Tian, and Chunsheng Zhao
Atmos. Chem. Phys., 21, 1375–1388,Short summary
Submicron particles larger than 300 nm dominate the aerosol light extinction and mass concentration in the urban environment. Aerosol hygroscopic properties extended to 600 nm were investigated at an urban site. Our results find that there exists a large fraction of a less hygroscopic group above 300 nm, and the hygroscopicity in this size range is enhanced significantly with the development of pollution levels. The hygroscopicity variation contributes greatly to the low visibility.
Kevin J. Sanchez, Bo Zhang, Hongyu Liu, Georges Saliba, Chia-Li Chen, Savannah L. Lewis, Lynn M. Russell, Michael A. Shook, Ewan C. Crosbie, Luke D. Ziemba, Matthew D. Brown, Taylor J. Shingler, Claire E. Robinson, Elizabeth B. Wiggins, Kenneth L. Thornhill, Edward L. Winstead, Carolyn Jordan, Patricia K. Quinn, Timothy S. Bates, Jack Porter, Thomas G. Bell, Eric S. Saltzman, Michael J. Behrenfeld, and Richard H. Moore
Atmos. Chem. Phys., 21, 831–851,Short summary
Models describing atmospheric airflow were combined with satellite measurements representative of marine phytoplankton and other meteorological variables. These combined variables were compared to measured aerosol to identify upwind influences on aerosol concentrations. Results indicate that phytoplankton production rates upwind impact the aerosol mass. Also, results suggest that the condensation of mass onto short-lived large sea spray particles may be a significant sink of aerosol mass.
Erik Lutsch, Kimberly Strong, Dylan B. A. Jones, Thomas Blumenstock, Stephanie Conway, Jenny A. Fisher, James W. Hannigan, Frank Hase, Yasuko Kasai, Emmanuel Mahieu, Maria Makarova, Isamu Morino, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Anatoly V. Poberovskii, Ralf Sussmann, and Thorsten Warneke
Atmos. Chem. Phys., 20, 12813–12851,Short summary
This paper describes the use of a network of 10 Arctic and midlatitude ground-based FTIR measurement sites to detect enhancements of the wildfire tracers carbon monoxide, hydrogen cyanide, and ethane from 2003 to 2018. A tagged CO GEOS-Chem simulation is used for source attribution and to evaluate the relative contribution of CO sources to the FTIR measurements. The use of FTIR measurements allowed for the emission ratios of hydrogen cyanide and ethane to be quantified.
Holger Vömel, Herman G. J. Smit, David Tarasick, Bryan Johnson, Samuel J. Oltmans, Henry Selkirk, Anne M. Thompson, Ryan M. Stauffer, Jacquelyn C. Witte, Jonathan Davies, Roeland van Malderen, Gary A. Morris, Tatsumi Nakano, and Rene Stübi
Atmos. Meas. Tech., 13, 5667–5680,Short summary
The time response of electrochemical concentration cell (ECC) ozonesondes points to at least two distinct reaction pathways with time constants of approximately 20 s and 25 min. Properly considering these time constants eliminates the need for a poorly defined "background" and allows reducing ad hoc corrections based on laboratory tests. This reduces the uncertainty of ECC ozonesonde measurements throughout the profile and especially in regions of low ozone and strong gradients of ozone.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Geosci. Model Dev., 13, 3839–3862,Short summary
Systematic errors in atmospheric models pose a challenge for inverse modeling studies of methane (CH4) emissions. We evaluated the CH4 simulation in the GEOS-Chem model at the horizontal resolutions of 4° × 5° and 2° × 2.5°. Our analysis identified resolution-dependent biases in the model, which we attributed to discrepancies between the two model resolutions in vertical transport in the troposphere and in stratosphere–troposphere exchange.
Matthew J. Cooper, Randall V. Martin, Daven K. Henze, and Dylan B. A. Jones
Atmos. Chem. Phys., 20, 7231–7241,Short summary
Comparisons between satellite-retrieved and model-simulated NO2 columns are affected by differences between the model vertical profile and the assumed profile used in the retrieval process. We examine how such differences impact NOx emission estimates from satellite observations. Larger differences between the simulated and assumed profile shape correspond to larger emission errors. This reveals the importance of using consistent profile information when comparing satellite columns to models.
Quan Liu, Dantong Liu, Qian Gao, Ping Tian, Fei Wang, Delong Zhao, Kai Bi, Yangzhou Wu, Shuo Ding, Kang Hu, Jiale Zhang, Deping Ding, and Chunsheng Zhao
Atmos. Chem. Phys., 20, 3931–3944,Short summary
We present a series of aircraft-based in situ measurements of aerosol chemical components and size distributions over the North China Plain, and the hygroscopicity is derived from aerosol chemical composition. These results reveal the vertical characteristics of aerosol hygroscopicity, and we investigated their impacts on optical properties and activation under different moisture and pollution conditions over this polluted region.
Ping Tian, Dantong Liu, Delong Zhao, Chenjie Yu, Quan Liu, Mengyu Huang, Zhaoze Deng, Liang Ran, Yunfei Wu, Shuo Ding, Kang Hu, Gang Zhao, Chunsheng Zhao, and Deping Ding
Atmos. Chem. Phys., 20, 2603–2622,Short summary
This study paints a full picture of the evolution of vertical characteristics of aerosol optical properties and shortwave heating impacts of carbonaceous aerosols during different stages of pollution events over the Beijing region and highlights the increased contribution of brown carbon absorption, especially at higher levels, during pollution.
Yu Wang, Ying Chen, Zhijun Wu, Dongjie Shang, Yuxuan Bian, Zhuofei Du, Sebastian H. Schmitt, Rong Su, Georgios I. Gkatzelis, Patrick Schlag, Thorsten Hohaus, Aristeidis Voliotis, Keding Lu, Limin Zeng, Chunsheng Zhao, M. Rami Alfarra, Gordon McFiggans, Alfred Wiedensohler, Astrid Kiendler-Scharr, Yuanhang Zhang, and Min Hu
Atmos. Chem. Phys., 20, 2161–2175,Short summary
Severe haze events, with high particulate nitrate (pNO3−) burden, frequently prevail in Beijing. In this study, we demonstrate a mutual-promotion effect between aerosol water uptake and pNO3− formation backed up by theoretical calculations and field observations throughout a typical pNO3−-dominated haze event in Beijing wintertime. This self-amplified mutual-promotion effect between aerosol water content and particulate nitrate can rapidly deteriorate air quality and degrade visibility.
Ye Kuang, Yao He, Wanyun Xu, Pusheng Zhao, Yafang Cheng, Gang Zhao, Jiangchuan Tao, Nan Ma, Hang Su, Yanyan Zhang, Jiayin Sun, Peng Cheng, Wenda Yang, Shaobin Zhang, Cheng Wu, Yele Sun, and Chunsheng Zhao
Atmos. Chem. Phys., 20, 865–880,Short summary
A new method was developed to calculate hygroscopicity parameter κ of organic aerosols (κOA) based on aerosol light-scattering measurements and bulk aerosol chemical-composition measurements. Derived high-time-resolution κOA varied in a wide range (near 0 to 0.25), and the organic aerosol oxidation degree significantly impacts variations in κOA. Distinct diurnal variation in κOA is found, and its relationship with oxygenated organic aerosol is discussed.
Gang Zhao, Jiangchuan Tao, Ye Kuang, Chuanyang Shen, Yingli Yu, and Chunsheng Zhao
Atmos. Chem. Phys., 19, 13175–13188,Short summary
Characteristics of the black carbon size distribution (BCMSD) are studied by using our developed measurement system. Results show that the BCMSDs have two modes and the mean peak diameters are 150 nm and 503 nm, respectively. The coarser mode varies significantly under different pollution conditions, which gives rise to significant variation in aerosol bulk optical properties. Our study reveals that the BCMSD as well as the mixing state in estimating aerosol radiative forcing matters.
Brendan Byrne, Dylan B. A. Jones, Kimberly Strong, Saroja M. Polavarapu, Anna B. Harper, David F. Baker, and Shamil Maksyutov
Atmos. Chem. Phys., 19, 13017–13035,Short summary
Interannual variations in net ecosystem exchange (NEE) estimated from the Greenhouse Gases Observing Satellite (GOSAT) XCO2 measurements are shown to be correlated (P < 0.05) with temperature and FLUXCOM NEE anomalies. Furthermore, the GOSAT-informed NEE anomalies are found to be better correlated with temperature and FLUXCOM anomalies than NEE estimates from most terrestrial biosphere models, suggesting that GOSAT CO2 measurements provide a useful constraint on NEE interannual variability.
Jacob K. Hedelius, Tai-Long He, Dylan B. A. Jones, Bianca C. Baier, Rebecca R. Buchholz, Martine De Mazière, Nicholas M. Deutscher, Manvendra K. Dubey, Dietrich G. Feist, David W. T. Griffith, Frank Hase, Laura T. Iraci, Pascal Jeseck, Matthäus Kiel, Rigel Kivi, Cheng Liu, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Sébastien Roche, Coleen M. Roehl, Matthias Schneider, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Colm Sweeney, Yao Té, Osamu Uchino, Voltaire A. Velazco, Wei Wang, Thorsten Warneke, Paul O. Wennberg, Helen M. Worden, and Debra Wunch
Atmos. Meas. Tech., 12, 5547–5572,Short summary
We seek ways to improve the accuracy of column measurements of carbon monoxide (CO) – an important tracer of pollution – made from the MOPITT satellite instrument. We devise a filtering scheme which reduces the scatter and also eliminates bias among the MOPITT detectors. Compared to ground-based observations, MOPITT measurements are about 6 %–8 % higher. When MOPITT data are implemented in a global assimilation model, they tend to reduce the model mismatch with aircraft measurements.
Gang Zhao, Tianyi Tan, Weilun Zhao, Song Guo, Ping Tian, and Chunsheng Zhao
Atmos. Chem. Phys., 19, 12875–12885,Short summary
Traditionally, the real part of the refractive index (RRI) of ambient aerosols is calculated by their chemical components. In this study, we demonstrate that the RRI is highly related to effective density rather than chemical components using field measurements. For the first time, a parameterization scheme for ambient aerosol RRI using effective density is proposed. This simple scheme is more reliable and ready to use in the calculation of aerosol optics and radiation.
Wanyun Xu, Ye Kuang, Chunsheng Zhao, Jiangchuan Tao, Gang Zhao, Yuxuan Bian, Wen Yang, Yingli Yu, Chuanyang Shen, Linlin Liang, Gen Zhang, Weili Lin, and Xiaobin Xu
Atmos. Chem. Phys., 19, 10557–10570,Short summary
The study of HONO, the primary source of OH radicals, is crucial for atmospheric photochemistry and heterogeneous chemistry. Heterogeneous NO2 conversion was shown to be one of the missing sources of HONO on the North China Plain, but the reaction path is still under debate. In this work, evidence was found that NH3 was the key factor that promoted the hydrolysis of NO2, leading to the explosive growth of HONO and nitrate, suggesting that NH3 emission control measures are urgently needed.
Shima Bahramvash Shams, Von P. Walden, Irina Petropavlovskikh, David Tarasick, Rigel Kivi, Samuel Oltmans, Bryan Johnson, Patrick Cullis, Chance W. Sterling, Laura Thölix, and Quentin Errera
Atmos. Chem. Phys., 19, 9733–9751,Short summary
The Arctic plays a very important role in the global ozone cycle. We use balloon-borne sampling and satellite data to create a high-quality dataset of the vertical profile of ozone from 2005 to 2017 to analyze ozone variations over four high-latitude Arctic locations. No significant annual trend is found at any of the studied locations. We develop a mathematical model to understand how deseasonalized ozone fluctuations can be influenced by various parameters.
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,Short summary
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.
Wangshu Tan, Gang Zhao, Yingli Yu, Chengcai Li, Jian Li, Ling Kang, Tong Zhu, and Chunsheng Zhao
Atmos. Meas. Tech., 12, 3825–3839,Short summary
A new method to retrieve CCN number concentrations using multiwavelength Raman lidars is proposed. The method implements hygroscopic enhancements of backscatter and extinction with relative humidity to represent particle hygroscopicity. The retrieved CCN number concentrations are in good agreement with theoretical calculated values. Sensitivity tests indicate that retrieval error in CCN arises mostly from uncertainties in extinction coefficients and RH profiles.
Gang Zhao, Weilun Zhao, and Chunsheng Zhao
Atmos. Meas. Tech., 12, 3541–3550,Short summary
A new method is proposed to retrieve the size-resolved real part of the refractive index (RRI). The main principle of deriving the RRI is measuring the scattering intensity by a single-particle soot photometer of a size-selected aerosol. This method is validated by a series of calibration experiments using the components of the known RI. The retrieved size-resolved RRI covers a wide range, from 200 nm to 450 nm, with uncertainty of less than 0.02.
Debra Wunch, Dylan B. A. Jones, Geoffrey C. Toon, Nicholas M. Deutscher, Frank Hase, Justus Notholt, Ralf Sussmann, Thorsten Warneke, Jeroen Kuenen, Hugo Denier van der Gon, Jenny A. Fisher, and Joannes D. Maasakkers
Atmos. Chem. Phys., 19, 3963–3980,Short summary
We used five atmospheric observatories in Europe measuring total column dry-air mole fractions of methane and carbon monoxide to infer methane emissions in the area between the observatories. We find that the methane emissions are overestimated by the state-of-the-art inventories, and that this is likely due, at least in part, to the inventory disaggregation. We find that there is significant uncertainty in the carbon monoxide inventories that requires further investigation.
Gang Zhao, Chunsheng Zhao, Ye Kuang, Yuxuan Bian, Jiangchuan Tao, Chuanyang Shen, and Yingli Yu
Atmos. Chem. Phys., 18, 9049–9060,Short summary
The aerosol asymmetry factor (g) is one of the most important factors for assessing direct aerosol radiative forcing (DARF) and remote sensing. So far, few studies have focused on the measurements and parameterization of g. Our study shows that relative humidity has significant impacts on g and DARF due to aerosol hygroscopic growth. For the first time, a novel method based on measurements from the humidified nephelometer system is proposed to calculate g accurately with high time resolution.
Chance W. Sterling, Bryan J. Johnson, Samuel J. Oltmans, Herman G. J. Smit, Allen F. Jordan, Patrick D. Cullis, Emrys G. Hall, Anne M. Thompson, and Jacquelyn C. Witte
Atmos. Meas. Tech., 11, 3661–3687,Short summary
The electrochemical concentration cell ozonesonde is a balloon-borne instrument that measures ozone to an altitude of ~30 km. This work summarizes the National Oceanic and Atmospheric Administration's 50+ year, eight-site ozonesonde network history, the processing techniques utilized to account for instrumental changes, and the uncertainty of the measurement. The ozonesonde measurements were compared to satellite measurements and agreed well. This important data set is more useful and robust.
Ye Kuang, Chun Sheng Zhao, Gang Zhao, Jiang Chuan Tao, Wanyun Xu, Nan Ma, and Yu Xuan Bian
Atmos. Meas. Tech., 11, 2967–2982,Short summary
Aerosol water has become an important topic recently because of its implications for multiphase secondary aerosol formation during severe haze events in Asia. This is a timely paper on this topic; a novel method is proposed to calculate ambient aerosol liquid water contents based only on measurements of a three-wavelength humidified nephelometer system. The advantage of this method is that this technique can provide continuous measurements of the changing ambient conditions.
Jing Li, Chengcai Li, and Chunsheng Zhao
Atmos. Chem. Phys., 18, 3289–3298,Short summary
Our study investigates the long-term trends of extreme aerosol pollution in China over the past ~ 30 years. In the 1980s, an overall positive trend is found throughout China with the extreme trend exceeding the mean trend, except for Northwest China and the North China Plain. In the 1990s, the extreme trends continued to dominate in the south while they yield to the mean trend in the north. After 2000, the extreme trend became weaker than the mean trend overall.
Bakr Badawy, Saroja Polavarapu, Dylan B. A. Jones, Feng Deng, Michael Neish, Joe R. Melton, Ray Nassar, and Vivek K. Arora
Geosci. Model Dev., 11, 631–663,Short summary
We assess the impact of using the meteorological fields from GEM-MACH-GHG to drive CLASS-CTEM. This coupling is considered an important step toward understanding how meteorological uncertainties affect both CO2 flux estimates and modeled atmospheric transport. Ultimately, such an approach will provide more direct feedback to the CLASS-CTEM developers and thus help to improve the performance of CLASS-CTEM by identifying the model limitations based on atmospheric constraints.
Jiangchuan Tao, Chunsheng Zhao, Ye Kuang, Gang Zhao, Chuanyang Shen, Yingli Yu, Yuxuan Bian, and Wanyun Xu
Atmos. Meas. Tech., 11, 895–906,Short summary
Existing chamber technologies for direct measurements of number concentration of cloud condensation nuclei (NCCN) are sophisticated and expensive. In this paper, a new method is proposed to calculate NCCN based only on measurements of a humidified nephelometer system which have accounted for influences of both aerosol size and aerosol hygroscopicity on NCCN calculation. This new method makes NCCN measurements more convenient and is capable of obtaining NCCN at lower supersaturations.
Wanyun Xu, Xiaobin Xu, Meiyun Lin, Weili Lin, David Tarasick, Jie Tang, Jianzhong Ma, and Xiangdong Zheng
Atmos. Chem. Phys., 18, 773–798,Short summary
The impact of anthropogenic emissions and climate variability on the long-term trends and periodicity of surface ozone measured at Mt Waliguan (WLG) for the period of 1994–2013 is studied. STT ozone and rising emissions in eastern China contribute to spring and autumnal increasing trends, respectively. The 2–3-, 3–7-, and 11-year periodicities in the ozone data are linked to the QBO, EASMI, and sunspot cycle, respectively. An empirical model is obtained for normalised monthly ozone at WLG.
Jenny A. Fisher, Lee T. Murray, Dylan B. A. Jones, and Nicholas M. Deutscher
Geosci. Model Dev., 10, 4129–4144,Short summary
Carbon monoxide (CO) simulation in atmospheric chemistry models is used for source–receptor analysis, emission inversion, and interpretation of observations. We introduce a major update to CO simulation in the GEOS-Chem chemical transport model that removes fundamental inconsistencies relative to the standard model, resolving biases of more than 100 ppb and errors in vertical structure. We also add source tagging of secondary CO and demonstrate it provides added value in low-emission regions.
Gang Zhao, Chunsheng Zhao, Ye Kuang, Jiangchuan Tao, Wangshu Tan, Yuxuan Bian, Jing Li, and Chengcai Li
Atmos. Chem. Phys., 17, 12133–12143,Short summary
In this paper, influences of aerosol hygroscopic growth on the lidar ratio are studied. Results indicate that both the magnitude and vertical structures of the retrieved aerosol extinction coefficient (σext) profile from lidar signals are significantly biased. This study proposes a feasible method for reducing the bias of retrieving the σext profile and this method can be implemented in operational retrieval of the aerosol σext profile and for pollution monitoring.
Hyun-Deok Choi, Hongyu Liu, James H. Crawford, David B. Considine, Dale J. Allen, Bryan N. Duncan, Larry W. Horowitz, Jose M. Rodriguez, Susan E. Strahan, Lin Zhang, Xiong Liu, Megan R. Damon, and Stephen D. Steenrod
Atmos. Chem. Phys., 17, 8429–8452,Short summary
We evaluate global ozone–carbon monoxide (O3–CO) correlations in a chemistry and transport model during July–August with TES-Aura satellite observations and examine the sensitivity of model simulations to input meteorological data and emissions. Results show that O3–CO correlations may be used effectively to constrain the sources of regional tropospheric O3 in global 3-D models, especially for those regions where convective transport of pollution plays an important role.
Yuxuan Bian, Chunsheng Zhao, Wanyun Xu, Gang Zhao, Jiangchuan Tao, and Ye Kuang
Atmos. Meas. Tech., 10, 2313–2322,Short summary
Aerosol phase function is crucial for understanding the climate effects of aerosols. So far, there is a lack of instruments for measuring the aerosol phase function directly and accurately in laboratory studies and in situ measurements. A novel portable instrument with high angular range and resolution named
charge-coupled device-laser aerosol detective system(CCD-LADS) has been developed and validated for the measurement of the phase function of ambient aerosols in this study.
Ye Kuang, Chunsheng Zhao, Jiangchuan Tao, Yuxuan Bian, Nan Ma, and Gang Zhao
Atmos. Chem. Phys., 17, 6651–6662,Short summary
A novel approach is proposed in this research to derive the aerosol hygroscopicity parameter based only on measurements from a humidified nephelometer system without any additional information about particle number size distribution and black carbon. New findings in this research can bridge the gap between κ-Köhler theory and the aerosol light-scattering enhancement factor and will make the humidified nephelometer system more convenient when it comes to aerosol hygroscopicity research.
Zhe Jiang, Helen Worden, John R. Worden, Daven K. Henze, Dylan B. A. Jones, Avelino F. Arellano, Emily V. Fischer, Liye Zhu, Kazuyuki Miyazaki, K. Folkert Boersma, and Vivienne H. Payne
Atmos. Chem. Phys. Discuss.,
Preprint withdrawnShort summary
We investigated the variation of US tropospheric NO2 in the past decade. We demonstrated significant divergence between the time variation in tropospheric NO2 columns from OMI retrievals and surface measurements. Our analysis suggests limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, and indicates possible important contributions from long-range transport of Asian emissions that are modulated by ENSO.
Zhe Jiang, John R. Worden, Helen Worden, Merritt Deeter, Dylan B. A. Jones, Avelino F. Arellano, and Daven K. Henze
Atmos. Chem. Phys., 17, 4565–4583,Short summary
We constrain the long-term variation in global CO emissions for 2001–2015. Our results confirm that the decreasing trend of tropospheric CO in the Northern Hemisphere is due to decreasing CO emissions from anthropogenic and biomass burning sources. In particular, we find decreasing CO emissions from the United States and China in the past 15 years, unchanged anthropogenic CO emissions from Europe since 2008, and likely a positive trend from India and southeast Asia.
Erika Brattich, Hongyu Liu, Laura Tositti, David B. Considine, and James H. Crawford
Atmos. Chem. Phys., 17, 1061–1080,Short summary
We apply the GMI chemistry and transport model to simulate the seasonal variations of two radionuclide aerosol tracers (terrigenous 210Pb and cosmogenic 7Be) at the WMO-GAW station of Mt. Cimone during 2005, with an aim to understand the roles of transport and precipitation scavenging processes in controlling their seasonality. Results show a dominant role of precipitation scavenging in controlling the seasonality of 210Pb and 7Be concentrations at Mt. Cimone.
Hervé Petetin, Valérie Thouret, Alain Fontaine, Bastien Sauvage, Giles Athier, Romain Blot, Damien Boulanger, Jean-Marc Cousin, and Philippe Nédélec
Atmos. Chem. Phys., 16, 15147–15163,Short summary
Ozone (O3) and carbon monoxide (CO) are two compounds of major importance in the atmosphere. In this paper we investigated their variability and trends at Frankfurt based on the MOZAIC–IAGOS dataset, a unique dataset of about 21 300 vertical profiles recorded by commercial aircraft. The CO concentrations have been decreasing since 2002, while no strong tendency is observed for O3 since 1994. However, the O3 seasonal variations are changing, with the spring maximum occurring earlier and earlier.
Dale F. Hurst, William G. Read, Holger Vömel, Henry B. Selkirk, Karen H. Rosenlof, Sean M. Davis, Emrys G. Hall, Allen F. Jordan, and Samuel J. Oltmans
Atmos. Meas. Tech., 9, 4447–4457,Short summary
This study compares stratospheric water vapor measurements by the Aura Microwave Limb Sounder (MLS) and balloon-borne frost point hygrometers (FPs) at five sites that launch two different types of FPs. The results demonstrate that FP and MLS measurements have been diverging at statistically significant rates of 0.6 to 1.5 % per year since approximately 2010. Similarities in the divergences at different sites suggest a positive drift in MLS retrievals since approximately 2010.
Emrys G. Hall, Allen F. Jordan, Dale F. Hurst, Samuel J. Oltmans, Holger Vömel, Benjamin Kühnreich, and Volker Ebert
Atmos. Meas. Tech., 9, 4295–4310,Short summary
This work focuses on the balloon borne NOAA frost point hygrometer (FPH) instrument flown at three locations around the world: Boulder, Colorado, Lauder, New Zealand, and Hilo, Hawaii. The ongoing 36-year record is the longest continuous water vapor record with profiles reaching 28 km. Significant instrument updates in 2008 decreased the weight, cost, power consumption, and manufacturing time offering greater precision and ease of use.
Mohammed K. Osman, David W. Tarasick, Jane Liu, Omid Moeini, Valerie Thouret, Vitali E. Fioletov, Mark Parrington, and Philippe Nédélec
Atmos. Chem. Phys., 16, 10263–10282,Short summary
A new 3-D gridded climatology of CO has been developed by trajectory mapping of global MOZAIC-IAGOS in situ aircraft measurements. The dataset is archived monthly from 2001–2012 on a grid of 5 × 5deg × 1 km altitude. The dataset facilitates comparison of different years and seasons and offers insight into the global variation and trends of CO. Major CO sources are clearly visible. The dataset can be used as an a priori data for satellite retrieval and for air quality model validation and initialization.
Xiaolu Yan, Jonathon S. Wright, Xiangdong Zheng, Nathaniel J. Livesey, Holger Vömel, and Xiuji Zhou
Atmos. Meas. Tech., 9, 3547–3566,Short summary
We evaluate Aura Microwave Limb Sounder retrievals of temperature, water vapour and ozone over the eastern Tibetan Plateau against measurements from balloon-borne instruments. The newest version of the retrievals (v4) represents a slight improvement over the previous version, particularly with respect to data yields and upper tropospheric ozone. We identify several biases that did not appear in evaluations conducted elsewhere, highlighting the unique challenges of remote sensing in this region.
Nan Ma, Chunsheng Zhao, Jiangchuan Tao, Zhijun Wu, Simonas Kecorius, Zhibin Wang, Johannes Größ, Hongjian Liu, Yuxuan Bian, Ye Kuang, Monique Teich, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Hartmut Herrmann, Min Hu, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 8593–8607,Short summary
New particle formation (NPF) is one of main sources of cloud condensation nuclei (CCN) in the atmosphere. Based on in situ measurements, we found that CCN activity of newly formed particles largely differs in different NPF events. It is therefore difficult to find a simple parameterization of CCN activity for NPF events. Using a fixed size-resolved activation ratio curve or critical diameter is very likely to result in large biases up to 50 % in the calculated NCCN during NPF events.
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294,Short summary
We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
Zhe Jiang, Kazuyuki Miyazaki, John R. Worden, Jane J. Liu, Dylan B. A. Jones, and Daven K. Henze
Atmos. Chem. Phys., 16, 6537–6546,Short summary
We quantify the impacts of anthropogenic and natural sources on free tropospheric ozone over the Middle East, using the adjoint of the GEOS-Chem model with updated NOx emissions estimates from an ensemble Kalman filter. We show that the global total contribution of lightning NOx on free tropospheric O3 over the Middle East is about 2 times larger than that from global anthropogenic sources. The summertime free tropospheric O3 enhancement is primarily due to Asian NOx emissions.
Alicia Gressent, Bastien Sauvage, Daniel Cariolle, Mathew Evans, Maud Leriche, Céline Mari, and Valérie Thouret
Atmos. Chem. Phys., 16, 5867–5889,Short summary
In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
Lei Huang, Jonathan H. Jiang, Lee T. Murray, Megan R. Damon, Hui Su, and Nathaniel J. Livesey
Atmos. Chem. Phys., 16, 5641–5663,Short summary
This study evaluates the distribution and variation of carbon monoxide (CO) in the upper troposphere and lower stratosphere (UTLS) during 2004–2012 on global and regional scales as simulated by two chemical transport models (GMI and GEOS-Chem), using the latest version (V4) of Aura Microwave Limb Sounder (MLS) observations. The impacts of surface emissions and convection on CO concentrations in the UTLS over different regions are investigated, using both model simulations and MLS observations.
Hongyu Liu, David B. Considine, Larry W. Horowitz, James H. Crawford, Jose M. Rodriguez, Susan E. Strahan, Megan R. Damon, Stephen D. Steenrod, Xiaojing Xu, Jules Kouatchou, Claire Carouge, and Robert M. Yantosca
Atmos. Chem. Phys., 16, 4641–4659,Short summary
We assess the utility of cosmogenic beryllium-7, a natural aerosol tracer, for evaluating cross-tropopause transport in global models. We show that model excessive cross-tropopause transport of beryllium-7 corresponds to overestimated stratospheric contribution to tropospheric ozone. We conclude that the observational constraints for beryllium-7 and observed beryllium-7 total deposition fluxes can be used routinely as a first-order assessment of cross-tropopause transport in global models.
D. W. Tarasick, J. Davies, H. G. J. Smit, and S. J. Oltmans
Atmos. Meas. Tech., 9, 195–214,Short summary
Changes to measurement methods over Canada's 48-year ozonesonde record have been characterized and corrections applied. An estimate of the altitude-dependent uncertainty is added to each profile. The re-evaluated time series show negative trends in the lower stratosphere of up to 5 % per decade for the period 1966–2013. In the troposphere trends for the 48-year period are generally not significant. This suggests that free tropospheric ozone levels over Canada have not changed in nearly 50 years.
F. Deng, D. B. A. Jones, T. W. Walker, M. Keller, K. W. Bowman, D. K. Henze, R. Nassar, E. A. Kort, S. C. Wofsy, K. A. Walker, A. E. Bourassa, and D. A. Degenstein
Atmos. Chem. Phys., 15, 11773–11788,Short summary
The upper troposphere and lower stratosphere (UTLS) is characterized by strong gradients in the distribution of long-lived tracers, which are sensitive to discrepancies in transport in models. We found that our model overestimates CO2 in the polar UTLS through comparison of modeled CO2 with aircraft observations. We then corrected the modeled CO2 and quantified the impact of the correction on the flux estimates using an atmospheric model together with atmospheric CO2 measured from a satellite.
P. S. Monks, A. T. Archibald, A. Colette, O. Cooper, M. Coyle, R. Derwent, D. Fowler, C. Granier, K. S. Law, G. E. Mills, D. S. Stevenson, O. Tarasova, V. Thouret, E. von Schneidemesser, R. Sommariva, O. Wild, and M. L. Williams
Atmos. Chem. Phys., 15, 8889–8973,Short summary
Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, and yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models.
Y. H. Mao, Q. B. Li, D. K. Henze, Z. Jiang, D. B. A. Jones, M. Kopacz, C. He, L. Qi, M. Gao, W.-M. Hao, and K.-N. Liou
Atmos. Chem. Phys., 15, 7685–7702,
L. J. Kramer, D. Helmig, J. F. Burkhart, A. Stohl, S. Oltmans, and R. E. Honrath
Atmos. Chem. Phys., 15, 6827–6849,
Z. Jiang, D. B. A. Jones, J. Worden, H. M. Worden, D. K. Henze, and Y. X. Wang
Atmos. Chem. Phys., 15, 6801–6814,Short summary
We present a high-resolution (0.5 x 0.667) regional CO inversion over North America in the period of June 2004–May 2005, using a combination of GEOS-Chem model and MOPITT CO observations. With optimized lateral boundary conditions, we show that regional inversion analyses can reduce the sensitivity of the CO source estimates to errors in long-range transport and in the distributions of the hydroxyl radical (OH), and consequently, provide better quantification on regional CO source estimates.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744,Short summary
Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
Y. Kuang, C. S. Zhao, J. C. Tao, and N. Ma
Atmos. Chem. Phys., 15, 5761–5772,Short summary
In this paper, it is found that the diurnal variations of single scattering albedo (SSA) and asymmetry factor (g) for ambient aerosol are both evident and far different from those of dry state aerosol in the North China Plain (NCP. The diurnal changes of SSA and g have significant impacts on the estimation of daily average direct aerosol radiative effect (DARE) at the top of the atmosphere. In addition, several suggestions are proposed to improve the accurate prediction of DARE in the NCP.
A. Inness, A.-M. Blechschmidt, I. Bouarar, S. Chabrillat, M. Crepulja, R. J. Engelen, H. Eskes, J. Flemming, A. Gaudel, F. Hendrick, V. Huijnen, L. Jones, J. Kapsomenakis, E. Katragkou, A. Keppens, B. Langerock, M. de Mazière, D. Melas, M. Parrington, V. H. Peuch, M. Razinger, A. Richter, M. G. Schultz, M. Suttie, V. Thouret, M. Vrekoussis, A. Wagner, and C. Zerefos
Atmos. Chem. Phys., 15, 5275–5303,Short summary
The paper presents results from data assimilation studies with the new Composition-IFS model developed in the MACC project. This system was used in MACC to produce daily analyses and 5-day forecasts of atmospheric composition and is now run daily in the EU’s Copernicus Atmosphere Monitoring Service. The paper looks at the quality of the CO, O3 and NO2 analysis fields obtained with this system, comparing them against observations, a control run and an older version of the model.
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603,Short summary
Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
Z. Jiang, D. B. A. Jones, H. M. Worden, and D. K. Henze
Atmos. Chem. Phys., 15, 1521–1537,Short summary
Using MOPITT (version 5) tropospheric profile and surface layer retrievals, we constrain global CO emissions in the period of June 2004 – May 2005. The inversions suggest a reduction in CO emission in the tropics and an increase in emissions at middle and high latitudes. The results demonstrate that the use of the surface layer retrievals from MOPITT can significantly mitigate the potential impacts of model bias in OH and long-range transport on CO emission estimates.
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429,Short summary
High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112,Short summary
We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
J. C. Tao, C. S. Zhao, N. Ma, and P. F. Liu
Atmos. Chem. Phys., 14, 12055–12067,
M. Müller, T. Mikoviny, S. Feil, S. Haidacher, G. Hanel, E. Hartungen, A. Jordan, L. Märk, P. Mutschlechner, R. Schottkowsky, P. Sulzer, J. H. Crawford, and A. Wisthaler
Atmos. Meas. Tech., 7, 3763–3772,Short summary
This paper describes a new airborne instrument for measuring the trace gas composition of the atmosphere.
G. Q. Fu, W. Y. Xu, R. F. Yang, J. B. Li, and C. S. Zhao
Atmos. Chem. Phys., 14, 11949–11958,
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895,
J. Chen, C. S. Zhao, N. Ma, and P. Yan
Atmos. Chem. Phys., 14, 8105–8118,
W. Y. Xu, C. S. Zhao, L. Ran, W. L. Lin, P. Yan, and X. B. Xu
Atmos. Chem. Phys., 14, 7757–7768,
S. J. Oltmans, A. Karion, R. C. Schnell, G. Pétron, C. Sweeney, S. Wolter, D. Neff, S. A. Montzka, B. R. Miller, D. Helmig, B. J. Johnson, and J. Hueber
Atmos. Chem. Phys. Discuss.,
Revised manuscript not accepted
Y. X. Bian, C. S. Zhao, N. Ma, J. Chen, and W. Y. Xu
Atmos. Chem. Phys., 14, 6417–6426,
N. Ma, W. Birmili, T. Müller, T. Tuch, Y. F. Cheng, W. Y. Xu, C. S. Zhao, and A. Wiedensohler
Atmos. Chem. Phys., 14, 6241–6259,
J. Ma, W. L. Lin, X. D. Zheng, X. B. Xu, Z. Li, and L. L Yang
Atmos. Chem. Phys., 14, 5311–5325,
F. Deng, D. B. A. Jones, D. K. Henze, N. Bousserez, K. W. Bowman, J. B. Fisher, R. Nassar, C. O'Dell, D. Wunch, P. O. Wennberg, E. A. Kort, S. C. Wofsy, T. Blumenstock, N. M. Deutscher, D. W. T. Griffith, F. Hase, P. Heikkinen, V. Sherlock, K. Strong, R. Sussmann, and T. Warneke
Atmos. Chem. Phys., 14, 3703–3727,
H. J. Liu, C. S. Zhao, B. Nekat, N. Ma, A. Wiedensohler, D. van Pinxteren, G. Spindler, K. Müller, and H. Herrmann
Atmos. Chem. Phys., 14, 2525–2539,
C.-C. Chang, M. Shao, C. C. K. Chou, S.-C. Liu, J.-L. Wang, K.-Z. Lee, C.-H. Lai, T. Zhu, and P.-H. Lin
Atmos. Chem. Phys. Discuss.,
Revised manuscript not accepted
Z. Z. Deng, C. S. Zhao, N. Ma, L. Ran, G. Q. Zhou, D. R. Lu, and X. J. Zhou
Atmos. Chem. Phys., 13, 6227–6237,
F. Hasebe, Y. Inai, M. Shiotani, M. Fujiwara, H. Vömel, N. Nishi, S.-Y. Ogino, T. Shibata, S. Iwasaki, N. Komala, T. Peter, and S. J. Oltmans
Atmos. Chem. Phys., 13, 4393–4411,
M. Huang, G. R. Carmichael, T. Chai, R. B. Pierce, S. J. Oltmans, D. A. Jaffe, K. W. Bowman, A. Kaduwela, C. Cai, S. N. Spak, A. J. Weinheimer, L. G. Huey, and G. S. Diskin
Atmos. Chem. Phys., 13, 359–391,
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Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)A renewed rise in global HCFC-141b emissions between 2017–2021A model for simultaneous evaluation of NO2, O3, and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysisTechnical note: Entrainment-limited kinetics of bimolecular reactions in cloudsImproving NOx emission estimates in Beijing using network observations and a perturbed emissions ensembleObservation-based analysis of ozone production sensitivity for two persistent ozone episodes in Guangdong, ChinaA machine learning approach to quantify meteorological drivers of ozone pollution in China from 2015 to 2019Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurementsPotential environmental impact of bromoform from Asparagopsis farming in AustraliaSatellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 2: Sensitivity to dry-deposition parameterizationsThe impacts of marine-emitted halogens on OH radicals in East Asia during summerImpact of eastern and central Pacific El Niño on lower tropospheric ozone in ChinaContribution of Asian emissions to upper tropospheric CO over the remote PacificImpact of a subtropical high and a typhoon on a severe ozone pollution episode in the Pearl River Delta, ChinaAn ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievalsA process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018Estimation of mechanistic parameters in the gas-phase reactions of ozone with alkenes for use in automated mechanism constructionProjections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policiesQuantification of methane emissions from hotspots and during COVID-19 using a global atmospheric inversionModel evaluation of short-lived climate forcers for the Arctic Monitoring and Assessment Programme: a multi-species, multi-model studyGlobal simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion productsInfluence of photochemical loss of volatile organic compounds on understanding ozone formation mechanismNorth China Plain as a hot spot of ozone pollution exacerbated by extreme high temperaturesBayesian assessment of chlorofluorocarbon (CFC), hydrochlorofluorocarbon (HCFC) and halon banks suggest large reservoirs still present in old equipmentPhotochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidantsImpact of biomass burning and stratospheric intrusions in the remote South Pacific Ocean troposphereInfluence of total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODEs) in the AntarcticChanges in anthropogenic precursor emissions drive shifts in the ozone seasonal cycle throughout the northern midlatitude troposphereAmplified role of potential HONO sources in O3 formation in North China Plain during autumn haze aggravating processesContinental-scale contributions to the global CFC-11 emission increase between 2012 and 2017Surface ozone impacts on major crop production in China from 2010 to 2017Enhanced summertime ozone and SOA from biogenic volatile organic compound (BVOC) emissions due to vegetation biomass variability during 1981–2018 in ChinaPyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formationTropospheric ozone changes and ozone sensitivity from the present day to the future under shared socio-economic pathwaysAn integrated analysis of contemporary methane emissions and concentration trends over China using in situ and satellite observations and model simulationsAn assessment of the tropospherically accessible photo-initiated ground state chemistry of organic carbonylsMethane emissions in the United States, Canada, and Mexico: evaluation of national methane emission inventories and 2010–2017 sectoral trends by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric observationsEvaluation of SO2, SO42− and an updated SO2 dry deposition parameterization in the United Kingdom Earth System ModelDevelopment and evaluation of a new compact mechanism for aromatic oxidation in atmospheric modelsOzone deposition impact assessments for forest canopies require accurate ozone flux partitioning on diurnal timescalesUnraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMIModel Output Statistics (MOS) applied to CAMS O3 forecasts: trade-offs between continuous and categorical skill scoresCloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of BorneoImproving predictability of high-ozone episodes through dynamic boundary conditions, emission refresh and chemical data assimilation during the Long Island Sound Tropospheric Ozone Study (LISTOS) field campaignAtmospheric observations consistent with reported decline in the UK's methane emissions (2013–2020)Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO2 in CESM2Technical note: Quality assessment of ozone reanalysis products and gap-filling over subarctic Europe for vegetation risk mappingEvolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A modelImpact of pyruvic acid photolysis on acetaldehyde and peroxy radical formation in the boreal forest: theoretical calculations and model resultsEvaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimationGlobal tropospheric halogen (Cl, Br, I) chemistry and its impact on oxidants
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616,Short summary
The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
Atmos. Chem. Phys., 22, 9111–9127,Short summary
A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easily interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants, even when having missing data.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015,Short summary
Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Le Yuan, Olalekan A. M. Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys., 22, 8617–8637,Short summary
Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing inventories using air quality models and routine in situ observations. Using this approach, we derived improved estimates of NOx emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416,Short summary
We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402,Short summary
We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826,Short summary
We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646,Short summary
In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487,Short summary
This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351,Short summary
We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.
Zhongjing Jiang and Jing Li
Atmos. Chem. Phys., 22, 7273–7285,Short summary
This study investigates the changes of tropospheric ozone in China associated with EP and CP El Niño, using satellite observations and the GEOS-Chem model. We found that El Niño generally leads to lower tropospheric ozone (LTO) decrease over most parts of China; La Niña acts the opposite. The difference between LTO changes during EP and CP El Niño primarily lies in southern China. Regional transport and chemical processes play the leading and secondary roles in driving the LTO changes.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206,Short summary
Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Shanshan Ouyang, Tao Deng, Run Liu, Jingyang Chen, Guowen He, Jeremy Cheuk-Hin Leung, Nan Wang, and Shaw Chen Liu
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
A record-breaking severe O3 pollution episode occurred under the influence of a Pacific subtropical high followed by Typhoon Mina in the Pearl River Delta (PRD) in early Autumn 2019. Through the WRF-CMAQ model simulations, we propose that the enhanced photochemical production of O3 during the episode is a major cause of the most severe O3 pollution year since the official O3 observation started in PRD in 2006.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624,Short summary
Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289,Short summary
We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195,Short summary
Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101,Short summary
The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Luca Cantarello, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 5961–5981,Short summary
Concentrations of atmospheric methane continue to grow, in recent years at an increasing rate, for unknown reasons. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high resolution. Results show that the system can accurately report on biases in national inventories and is used to conclude that the early COVID-19 slowdown period (March–June 2020) had little impact on global methane emissions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828,Short summary
Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494,Short summary
Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851,Short summary
The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719,Short summary
China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Halocarbons contained in equipment continue to be emitted after production has ceased. These ‘banks’ must be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone hole recovery if left unrecovered.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275,Short summary
Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099,Short summary
Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890,Short summary
We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524,Short summary
A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302,Short summary
This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907,Short summary
The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638,Short summary
In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364,Short summary
Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963,Short summary
This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227,Short summary
Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249,Short summary
Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Keiran N. Rowell, Scott H. Kable, and Meredith J. T. Jordan
Atmos. Chem. Phys., 22, 929–949,Short summary
Sunlight drives chemical reactions in the atmosphere by breaking chemical bonds. Motivated by the knowledge that if we can better understand the fundamental chemistry, we will be better able to predict atmospheric composition and model any future changes, we use quantum chemistry to investigate new classes of atmospheric reactions. We identify several potentially important reaction classes that will have implications for the atmospheric production of organic acids and molecular hydrogen.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418,Short summary
We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497,Short summary
We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374,Short summary
Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411,Short summary
Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245,Short summary
The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study investigates to which extent ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts, while highlighting at the same time the complexity of improving the detection of highest O3 concentrations.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984,Short summary
Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553,Short summary
Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276,Short summary
We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys., 21, 16093–16120,Short summary
Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations (or mixing ratios) decreased by 46 %, 41 %, and 22 % in Europe, the USA, and China, respectively. Fe chemistry and HOx chemistry contributed more to SO2 oxidation than N chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Stefanie Falk, Ane V. Vollsnes, Aud B. Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys., 21, 15647–15661,Short summary
We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level, underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well, still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 76 % accuracy compared to the regional model (80 %).
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669,Short summary
We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349,Short summary
We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401,Short summary
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 of these data is necessary.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996,Short summary
Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
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High ozone concentrations (up to 94.7ppbv) were frequently observed at an altitude of ~1.5--2km over Beijing during April--May 2005. Ozone due to Asian anthropogenic pollution made major contributions to the observed ozone enhancements. These enhancements typically occurred under southerly wind and warmer conditions. An earlier onset of the Asian summer monsoon would cause more ozone enhancement events in the lower troposphere over the North China Plain in late spring and early summer.
High ozone concentrations (up to 94.7ppbv) were frequently observed at an altitude of ~1.5--2km...