Articles | Volume 19, issue 9
https://doi.org/10.5194/acp-19-6481-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-6481-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Assessment of dicarbonyl contributions to secondary organic aerosols over China using RAMS-CMAQ
Jialin Li
State Key Laboratory of Atmospheric Boundary Layer Physics and
Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of
Sciences, Beijing 100029, China
State Key Laboratory of Atmospheric Boundary Layer Physics and
Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of
Sciences, Beijing 100029, China
Center for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
University of Chinese Academy of Sciences, Beijing 100049, China
Guiqian Tang
State Key Laboratory of Atmospheric Boundary Layer Physics and
Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of
Sciences, Beijing 100029, China
State Key Laboratory of Atmospheric Boundary Layer Physics and
Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of
Sciences, Beijing 100029, China
Center for Excellence in Regional Atmospheric Environment, Institute
of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China
University of Chinese Academy of Sciences, Beijing 100049, China
Fangkun Wu
State Key Laboratory of Atmospheric Boundary Layer Physics and
Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of
Sciences, Beijing 100029, China
Yongfu Xu
State Key Laboratory of Atmospheric Boundary Layer Physics and
Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of
Sciences, Beijing 100029, China
University of Chinese Academy of Sciences, Beijing 100049, China
Related authors
No articles found.
Yi Zhang, Weiqi Xu, Yan Li, Guohua Zhang, Dantong Liu, Ye Kuang, Yu Zhang, Wei Zhou, Xiaocong Peng, Bojiang Su, Weihong Huang, Zijun Zhang, Liu Yang, Yangzhou Wu, Siyuan Li, Shitong Zhao, Lanzhong Liu, Xiaole Pan, Zifa Wang, Xinhui Bi, Mikael Ehn, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 26, 5617–5634, https://doi.org/10.5194/acp-26-5617-2026, https://doi.org/10.5194/acp-26-5617-2026, 2026
Short summary
Short summary
This study explores how clouds influence the chemical composition of air particles through field research at a high-altitude station in southeastern China across different seasons. We found that different cloud types cause varying degrees of chemical changes in these particles. These findings enhance our understanding of the impact of clouds on air quality and contribute to improving climate models.
Jingye Ren, Songjian Zou, Honghao Xu, Guiquan Liu, Zhe Wang, Anran Zhang, Chuanfeng Zhao, Min Hu, Dongjie Shang, Lizi Tang, Ru-Jin Huang, Yele Sun, and Fang Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2026-1347, https://doi.org/10.5194/egusphere-2026-1347, 2026
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
Short summary
Short summary
In this study, a new framework of cloud condensation nuclei (CCN) prediction in polluted region has been developed and it achieves well prediction of hourly-to-yearly scale across North China Plain. The study reveals the machine learning model can largely reduce the uncertainty in simulating cloud radiative forcing, illustrating the high sensitivity of climate forcing to changes in CCN. This improvement of our new model would be helpful to aerosols climate effect assessment in models.
Xiaoying Li, Long Jia, and Yongfu Xu
Atmos. Chem. Phys., 26, 4479–4487, https://doi.org/10.5194/acp-26-4479-2026, https://doi.org/10.5194/acp-26-4479-2026, 2026
Short summary
Short summary
Nitrogen-containing organic aerosols can affect health, environment, and climate; however, their formation mechanism is still poorly understood. Based on Orbitrap-MS (mass spectrometer), our study reveals a previously unrecognized atmospheric reaction pathway in which ammonia can efficiently scavenge stable Criegee intermediates. This new reaction produces nitrogen-containing organic compounds with a reactive peroxide bond, which may pose health risks and alter the optical properties of aerosols.
Hongyi Li, Ting Yang, Yele Sun, and Zifa Wang
Atmos. Meas. Tech., 19, 2225–2244, https://doi.org/10.5194/amt-19-2225-2026, https://doi.org/10.5194/amt-19-2225-2026, 2026
Short summary
Short summary
We develop a physics-constrained deep-learning framework to retrieve vertical profiles of particulate matter <2.5 µm chemical components from lidar measurements. Comparisons with surface, tower, and aircraft measurements validate the performance of the framework. A six-year vertical profile dataset generated for Beijing reveals that organic matter and nitrate are dominant chemical components. This work offers a new perspective on the lidar inversion of chemical component profiles.
Jingye Ren, Wei Xu, Ru-Jin Huang, Fang Zhang, Ying Wang, Lu Chen, Jurgita Ovadnevaite, Darius Ceburnis, Colin O'Dowd, and Yele Sun
Atmos. Chem. Phys., 26, 2985–3000, https://doi.org/10.5194/acp-26-2985-2026, https://doi.org/10.5194/acp-26-2985-2026, 2026
Short summary
Short summary
Impact of mixing state on cloud condensation nuclei (CCN) was incorporated in limited modeling with simplified assumption. This study derived a mixing state index from hygroscopicity and systematically investigated the covariation between the mixing state and CCN activity in inland and coastal air. We propose a practical approach for estimating critical diameter from mixing state index, applicable when the aerosol particles are not highly aged.
Yali Jin, Hao Luo, Siqi Tang, Shuhui Xue, Chengyu Nie, Xiaocong Peng, Yan Zheng, Weiqi Xu, Guohua Zhang, Xiaole Pan, Yele Sun, Qi Chen, Lanzhong Liu, and Defeng Zhao
Atmos. Chem. Phys., 26, 2813–2830, https://doi.org/10.5194/acp-26-2813-2026, https://doi.org/10.5194/acp-26-2813-2026, 2026
Short summary
Short summary
Cloud substantially changes the compositions organic aerosol. How cloud processing of organics occur on molecular level remains unclear. We found that compared with cloud free particles, organics in cloud contains more large molecules likely due to accretion reactions and has more nitrogen-containing compounds. We identify some new compounds formed in cloud. Such modifications of the organics in cloud can further change its physicochemical properties, and impact on climate and human health.
Wei Zhou, Liu Yang, Siqi Zeng, Yunping Kan, Lirong Yang, Weihong Zhang, Weijie Wang, Zijun Zhang, Yan Li, Weiqi Xu, Yucheng Gu, Yaozong Wang, Zhengyan Zuo, Jie Li, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 26, 2425–2441, https://doi.org/10.5194/acp-26-2425-2026, https://doi.org/10.5194/acp-26-2425-2026, 2026
Short summary
Short summary
Northwest China, situated in an arid and semi-arid climate region; air quality issues in this area have received less attention compared to other Chinese metropolitan clusters. This research identify a significant shift towards the coupling PM2.5 and O3 relationships over the past decade in northwest China, highlighting the great importance of urban terpenes and aromatic oxidation in secondary organic aerosol formation.
Weibin Zhu, Sai Shang, Jieqi Wang, Yunfei Wu, Zhaoze Deng, Liang Ran, Ye Kuang, Guiqian Tang, Xiangpeng Huang, Xiaole Pan, Lanzhong Liu, Weiqi Xu, Yele Sun, Bo Hu, Zifa Wang, and Zirui Liu
Atmos. Chem. Phys., 26, 1947–1965, https://doi.org/10.5194/acp-26-1947-2026, https://doi.org/10.5194/acp-26-1947-2026, 2026
Short summary
Short summary
NPF (new particle formation) is a key global CCN (cloud condensation nuclei) source, but its contribution at the polluted boundary-layer top remains unclear. Based on mountaintop observations in the Yangtze River Delta, we show that under polluted conditions, NPF at the boundary-layer top is enhanced and accelerates its conversion to CCN. Ammonia plays a key role, and a newly defined "Time Window" metric highlights the importance of oxidation-driven growth and regional transport in this process.
Guochen Wang, Xuedong Cui, Bingye Xu, Can Wu, Minkang Zhi, Keliang Li, Liang Xu, Qi Yuan, Yuntao Wang, Yele Sun, Zongbo Shi, Akinori Ito, Shixian Zhai, and Weijun Li
Atmos. Chem. Phys., 26, 1483–1496, https://doi.org/10.5194/acp-26-1483-2026, https://doi.org/10.5194/acp-26-1483-2026, 2026
Short summary
Short summary
Iron acidification process is primarily driven by sulphuric acid in the upper mixing layer different from nitric acid at the ground-level. Enhanced atmospheric aging process contributes to high iron solubility in the upper mixing layer. Numerical models should consider vertical variations in iron dissolution to improve simulation accuracy.
Haoyuan Chen, Tao Song, Xiaodong Chen, Yinghong Wang, Mengtian Cheng, Kai Wang, Fuxin Liu, Baoxian Liu, Guiqian Tang, and Yuesi Wang
Atmos. Chem. Phys., 26, 1359–1371, https://doi.org/10.5194/acp-26-1359-2026, https://doi.org/10.5194/acp-26-1359-2026, 2026
Short summary
Short summary
The methane leakage from natural gas may offset the reduced CO2 emissions from its combustion, To quantify its effect, we established the flux observation platform in Beijing, the results showed that natural gas has become a common source of both after the transformation of energy structure, the natural gas could escape during production, storage and use. Although the natural gas leakage rate is not high (1.12 %), the greenhouse effect caused by natural gas leakage can not be ignored.
Jialu Xu, Yingjie Zhang, Yuying Wang, Xing Yan, Bin Zhu, Chunsong Lu, Yuanjian Yang, Yele Sun, Junhui Zhang, Xiaofan Zuo, Zhanghanshu Han, and Rui Zhang
Atmos. Chem. Phys., 25, 18599–18616, https://doi.org/10.5194/acp-25-18599-2025, https://doi.org/10.5194/acp-25-18599-2025, 2025
Short summary
Short summary
We conducted a year-long study in Nanjing to explore how the height of the atmospheric boundary layer affects fine particle pollution. We found that low boundary layers in winter trap pollutants like nitrate and primary particles, while higher layers in summer help form secondary pollutants like sulfate and organic aerosols. These findings show that boundary layer dynamics are key to understanding and managing seasonal air pollution.
Yutong Tian, Ting Yang, Hongyi Li, Ping Tian, Yifan Song, Jiancun He, Yining Tan, Yele Sun, and Zifa Wang
Atmos. Chem. Phys., 25, 17581–17594, https://doi.org/10.5194/acp-25-17581-2025, https://doi.org/10.5194/acp-25-17581-2025, 2025
Short summary
Short summary
This study examines how nitrate pollution varies with height and season to combat urban haze. Nitrate levels peak near the ground in spring/winter due to humidity and temperature, while wind and sunlight drive high-altitude pollution in late autumn. Winter shows unique daytime peaks linked to sunlight and nighttime chemistry. Findings help cities design targeted strategies, like timing emissions cuts, to improve air quality by addressing pollution at specific heights and times.
Junhui Zhang, Yuying Wang, Jialu Xu, Xiaofan Zuo, Chunsong Lu, Bin Zhu, Yuanjian Yang, Xing Yan, and Yele Sun
Atmos. Chem. Phys., 25, 17413–17428, https://doi.org/10.5194/acp-25-17413-2025, https://doi.org/10.5194/acp-25-17413-2025, 2025
Short summary
Short summary
We conducted a year-long study in Nanjing to understand how tiny airborne particles take up water, which affects air quality and climate. We found that particle water uptake varies by season and size, with lower values in summer due to more organic materials. Local pollution mainly influences smaller particles, while larger ones are shaped by air mass transport. These findings help improve climate models and support better air pollution control in fast-growing cities.
Wenqing Jiang, Lijuan Li, Lu Yu, Hwajin Kim, Yele Sun, and Qi Zhang
Atmos. Chem. Phys., 25, 16817–16832, https://doi.org/10.5194/acp-25-16817-2025, https://doi.org/10.5194/acp-25-16817-2025, 2025
Short summary
Short summary
We studied how sunlight changes natural organic matter in fog droplets and the tiny airborne particles formed after the water evaporation. Advanced analyses showed that sunlight makes this material more oxidized, nitrogen-enriched, chemically transformed, and different in light absorption and volatility. These sunlight-driven changes influence the particles’ behavior in the air, affecting air quality, climate, and how long they remain suspended in the atmosphere.
Huiyun Du, Jie Li, Xueshun Chen, Gabriele Curci, Fangqun Yu, Yele Sun, Xu Dao, Song Guo, Zhe Wang, Wenyi Yang, Lianfang Wei, and Zifa Wang
Atmos. Chem. Phys., 25, 5665–5681, https://doi.org/10.5194/acp-25-5665-2025, https://doi.org/10.5194/acp-25-5665-2025, 2025
Short summary
Short summary
Inadequate consideration of mixing states and coatings on black carbon (BC) hinders aerosol radiation forcing quantification. Core–shell mixing aligns well with observations, but partial internal mixing is a more realistic representation. We used a microphysics module to determine the fraction of embedded BC and coating aerosols, constraining the mixing state. This reduced absorption enhancement by 30 %–43 % in northern China, offering insights into BC's radiative effects.
Jingye Ren, Songjian Zou, Honghao Xu, Guiquan Liu, Zhe Wang, Anran Zhang, Chuanfeng Zhao, Min Hu, Dongjie Shang, Lizi Tang, Ru-Jin Huang, Yele Sun, and Fang Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1483, https://doi.org/10.5194/egusphere-2025-1483, 2025
Preprint archived
Short summary
Short summary
In this study, a new framework of cloud condensation nuclei (CCN) prediction in polluted region has been developed and it achieves well prediction of hourly-to-yearly scale across North China Plain. The study reveals a significant long-term decreasing trend of CCN concentration at typical supersaturations due to a rapid reduction in aerosol concentrations from 2014 to 2018. This improvement of our new model would be helpful to aerosols climate effect assessment in models.
Xiao-Bing Li, Bin Yuan, Yibo Huangfu, Suxia Yang, Xin Song, Jipeng Qi, Xianjun He, Sihang Wang, Yubin Chen, Qing Yang, Yongxin Song, Yuwen Peng, Guiqian Tang, Jian Gao, Dasa Gu, and Min Shao
Atmos. Chem. Phys., 25, 2459–2472, https://doi.org/10.5194/acp-25-2459-2025, https://doi.org/10.5194/acp-25-2459-2025, 2025
Short summary
Short summary
Online vertical gradient measurements of volatile organic compounds (VOCs), ozone, and NOx were conducted based on a 325 m tall tower in urban Beijing. Vertical changes in the concentrations, compositions, key drivers, and environmental impacts of VOCs were analyzed in this study. We find that VOC species display differentiated vertical variation patterns and distinct roles in contributing to photochemical ozone formation with increasing height in the urban planetary boundary layer.
Ye Kuang, Jiangchuan Tao, Hanbing Xu, Li Liu, Pengfei Liu, Wanyun Xu, Weiqi Xu, Yele Sun, and Chunsheng Zhao
Atmos. Chem. Phys., 25, 1163–1174, https://doi.org/10.5194/acp-25-1163-2025, https://doi.org/10.5194/acp-25-1163-2025, 2025
Short summary
Short summary
This study presents a novel optical framework to measure supersaturation, a fundamental parameter in cloud physics, by observing the scattering properties of particles that have or have not grown into cloud droplets. The technique offers high-resolution measurements, capturing essential fluctuations in supersaturation necessary for understanding cloud physics.
Zilu Zhang, Libo Zhou, and Meigen Zhang
Atmos. Chem. Phys., 25, 1–25, https://doi.org/10.5194/acp-25-1-2025, https://doi.org/10.5194/acp-25-1-2025, 2025
Short summary
Short summary
By integrating the SNICAR model with Polar-WRF, we find that 50 ng g−1 black carbon (BC) deposition decreases snow albedo, increasing radiative forcing (RF) by 1–4 W m−2, especially in Greenland, Baffin Island, and eastern Siberia. The impact is strongly linked to BC mass, with deep snowpacks showing greater sensitivity. Snowmelt and land–atmosphere interactions are crucial. High-resolution modelling is necessary to better understand these effects on Arctic climate change.
Hongyi Li, Ting Yang, Lars Nerger, Dawei Zhang, Di Zhang, Guigang Tang, Haibo Wang, Yele Sun, Pingqing Fu, Hang Su, and Zifa Wang
Geosci. Model Dev., 17, 8495–8519, https://doi.org/10.5194/gmd-17-8495-2024, https://doi.org/10.5194/gmd-17-8495-2024, 2024
Short summary
Short summary
To accurately characterize the spatiotemporal distribution of particulate matter <2.5 µm chemical components, we developed the Nested Air Quality Prediction Model System with the Parallel Data Assimilation Framework (NAQPMS-PDAF) v2.0 for chemical components with non-Gaussian and nonlinear properties. NAQPMS-PDAF v2.0 has better computing efficiency, excels when used with a small ensemble size, and can significantly improve the simulation performance of chemical components.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
Atmos. Chem. Phys., 24, 9387–9399, https://doi.org/10.5194/acp-24-9387-2024, https://doi.org/10.5194/acp-24-9387-2024, 2024
Short summary
Short summary
We deployed an advanced aerosol–fog sampling system at a rural site in the North China Plain to investigate impacts of aerosol hygroscopic growth and activation on the physicochemical properties of submicron aerosols. Observed results highlighted remarkably different aqueous processing of primary and secondary submicron aerosol components under distinct ambient relative humidity (RH) conditions and that RH levels significantly impact aerosol sampling through the aerosol swelling effect.
Jiangchuan Tao, Biao Luo, Weiqi Xu, Gang Zhao, Hanbin Xu, Biao Xue, Miaomiao Zhai, Wanyun Xu, Huarong Zhao, Sanxue Ren, Guangsheng Zhou, Li Liu, Ye Kuang, and Yele Sun
Atmos. Chem. Phys., 24, 9131–9154, https://doi.org/10.5194/acp-24-9131-2024, https://doi.org/10.5194/acp-24-9131-2024, 2024
Short summary
Short summary
Using simultaneous measurements of DMA–CCNC, H(/V)TDMA, and DMA–SP2, impacts of primary emissions and secondary aerosol formations on changes in aerosol physicochemical properties were comprehensively investigated. It was found that intercomparisons among aerosol mixing-state parameters derived from different techniques can help us gain more insight into aerosol physical properties which, in turn, will aid the investigation of emission characteristics and secondary aerosol formation pathways.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
Short summary
Short summary
We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
Short summary
Short summary
We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
Short summary
Short summary
Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Xinlei Ge, Yele Sun, Justin Trousdell, Mindong Chen, and Qi Zhang
Atmos. Meas. Tech., 17, 423–439, https://doi.org/10.5194/amt-17-423-2024, https://doi.org/10.5194/amt-17-423-2024, 2024
Short summary
Short summary
This study aims to enhance the application of the Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) in characterizing organic nitrogen (ON) species within aerosol particles and droplets. A thorough analysis was conducted on 75 ON standards that represent a diverse spectrum of ambient ON types. The results underscore the capacity of the HR-AMS in examining the concentration and chemistry of atmospheric ON compounds, thereby offering insights into their sources and environmental impacts.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
Short summary
Short summary
Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Aodong Du, Jiaxing Sun, Hang Liu, Weiqi Xu, Wei Zhou, Yuting Zhang, Lei Li, Xubing Du, Yan Li, Xiaole Pan, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 23, 13597–13611, https://doi.org/10.5194/acp-23-13597-2023, https://doi.org/10.5194/acp-23-13597-2023, 2023
Short summary
Short summary
We characterized the impacts of emission controls on particle mixing state and density during the Beijing Olympic Winter Games using a SPAMS in tandem with a DMA and an AAC. OC and sulfate-containing particles increased, while those from primary emissions decreased. The effective particle densities increased and varied largely for different particles, highlighting the impacts of aging and formation processes on the changes of particle density and mixing state.
Tao Wang, Hang Liu, Jie Li, Shuai Wang, Youngseob Kim, Yele Sun, Wenyi Yang, Huiyun Du, Zhe Wang, and Zifa Wang
Geosci. Model Dev., 16, 5585–5599, https://doi.org/10.5194/gmd-16-5585-2023, https://doi.org/10.5194/gmd-16-5585-2023, 2023
Short summary
Short summary
This paper developed a two-way coupled module in a new version of a regional urban–street network model, IAQMS-street v2.0, in which the mass flux from streets to background is considered. Test cases are defined to evaluate the performance of IAQMS-street v2.0 in Beijing by comparing it with that simulated by IAQMS-street v1.0 and a regional model. The contribution of local emissions and the influence of on-road vehicle control measures on air quality are evaluated by using IAQMS-street v2.0.
Yong Zhang, Jie Tian, Qiyuan Wang, Lu Qi, Manousos Ioannis Manousakas, Yuemei Han, Weikang Ran, Yele Sun, Huikun Liu, Renjian Zhang, Yunfei Wu, Tianqu Cui, Kaspar Rudolf Daellenbach, Jay Gates Slowik, André S. H. Prévôt, and Junji Cao
Atmos. Chem. Phys., 23, 9455–9471, https://doi.org/10.5194/acp-23-9455-2023, https://doi.org/10.5194/acp-23-9455-2023, 2023
Short summary
Short summary
PM2.5 pollution still frequently occurs in northern China during winter, and it is necessary to figure out the causes of air pollution based on intensive real-time measurement. The findings elaborate the chemical characteristics and source contributions of PM2.5 in three pilot cities, reveal potential formation mechanisms of secondary aerosols, and highlight the importance of controlling biomass burning and inhibiting generation of secondary aerosol for air quality improvement.
Hang Liu, Xiaole Pan, Shandong Lei, Yuting Zhang, Aodong Du, Weijie Yao, Guiqian Tang, Tao Wang, Jinyuan Xin, Jie Li, Yele Sun, Junji Cao, and Zifa Wang
Atmos. Chem. Phys., 23, 7225–7239, https://doi.org/10.5194/acp-23-7225-2023, https://doi.org/10.5194/acp-23-7225-2023, 2023
Short summary
Short summary
We provide the average vertical profiles of black carbon (BC) concentration, size distribution and coating thickness at different times of the day in an urban area based on 112 vertical profiles. In addition, it is found that BC in the residual layer generally has a thicker coating, higher absorption enhancement and hygroscopicity than on the surface. Such aged BC could enter into the boundary layer and influence the BC properties in the early morning.
Xingxia Kou, Zhen Peng, Meigen Zhang, Fei Hu, Xiao Han, Ziming Li, and Lili Lei
Atmos. Chem. Phys., 23, 6719–6741, https://doi.org/10.5194/acp-23-6719-2023, https://doi.org/10.5194/acp-23-6719-2023, 2023
Short summary
Short summary
A CMAQ EnSRF-based regional inversion system was extended to resolve satellite retrievals into biogenic source–sink changes. The size of the assimilated biosphere sink in China inferred from GOSAT was −0.47 Pg C yr−1. The biosphere flux at the provincial scale was re-estimated following the refined description in the regional inversion.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
Short summary
Short summary
A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
Short summary
Short summary
The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
Short summary
Short summary
Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Shujun Zhong, Shuang Chen, Junjun Deng, Yanbing Fan, Qiang Zhang, Qiaorong Xie, Yulin Qi, Wei Hu, Libin Wu, Xiaodong Li, Chandra Mouli Pavuluri, Jialei Zhu, Xin Wang, Di Liu, Xiaole Pan, Yele Sun, Zifa Wang, Yisheng Xu, Haijie Tong, Hang Su, Yafang Cheng, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 2061–2077, https://doi.org/10.5194/acp-23-2061-2023, https://doi.org/10.5194/acp-23-2061-2023, 2023
Short summary
Short summary
This study investigated the role of the secondary organic aerosol (SOA) loading on the molecular composition of wintertime urban aerosols by ultrahigh-resolution mass spectrometry. Results demonstrate that the SOA loading is an important factor associated with the oxidation degree, nitrate group content, and chemodiversity of nitrooxy–organosulfates. Our study also found that the hydrolysis of nitrooxy–organosulfates is a possible pathway for the formation of organosulfates.
Yuying Wang, Rong Hu, Qiuyan Wang, Zhanqing Li, Maureen Cribb, Yele Sun, Xiaorui Song, Yi Shang, Yixuan Wu, Xin Huang, and Yuxiang Wang
Atmos. Chem. Phys., 22, 14133–14146, https://doi.org/10.5194/acp-22-14133-2022, https://doi.org/10.5194/acp-22-14133-2022, 2022
Short summary
Short summary
The mixing state of size-resolved soot particles and their influencing factors were investigated. The results suggest anthropogenic emissions and aging processes have diverse impacts on the mixing state of soot particles in different modes. Considering that the mixing state of soot particles is crucial to model aerosol absorption, this finding is important to study particle growth and the warming effect of black carbon aerosols.
Futing Wang, Ting Yang, Zifa Wang, Haibo Wang, Xi Chen, Yele Sun, Jianjun Li, Guigang Tang, and Wenxuan Chai
Atmos. Meas. Tech., 15, 6127–6144, https://doi.org/10.5194/amt-15-6127-2022, https://doi.org/10.5194/amt-15-6127-2022, 2022
Short summary
Short summary
We develop a new algorithm to get the vertical mass concentration profiles of fine aerosol components based on the synergy of ground-based remote sensing for the first time. The comparisons with in situ observations and chemistry transport models validate the performance of the algorithm. Uncertainties caused by input parameters are also assessed in this paper. We expected that the algorithm can provide a new idea for lidar inversion and promote the development of aerosol component profiles.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
Short summary
Short summary
Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
Short summary
Short summary
This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Zhiqiang Zhang, Yele Sun, Chun Chen, Bo You, Aodong Du, Weiqi Xu, Yan Li, Zhijie Li, Lu Lei, Wei Zhou, Jiaxing Sun, Yanmei Qiu, Lianfang Wei, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 10409–10423, https://doi.org/10.5194/acp-22-10409-2022, https://doi.org/10.5194/acp-22-10409-2022, 2022
Short summary
Short summary
We present a comprehensive characterization of water-soluble organic aerosol and the first mass spectral characterization of water-insoluble organic aerosol in the cold season in Beijing by integrating online and offline aerosol mass spectrometer measurements. WSOA comprised dominantly secondary OA and showed large changes during the transition season from autumn to winter. WIOA was characterized by prominent hydrocarbon ions series, low oxidation states, and significant day–night differences.
Jiaxing Sun, Yele Sun, Conghui Xie, Weiqi Xu, Chun Chen, Zhe Wang, Lei Li, Xubing Du, Fugui Huang, Yan Li, Zhijie Li, Xiaole Pan, Nan Ma, Wanyun Xu, Pingqing Fu, and Zifa Wang
Atmos. Chem. Phys., 22, 7619–7630, https://doi.org/10.5194/acp-22-7619-2022, https://doi.org/10.5194/acp-22-7619-2022, 2022
Short summary
Short summary
We analyzed the chemical composition and mixing state of BC-containing particles at urban and rural sites in winter in the North China Plain and evaluated their impact on light absorption enhancement. BC was dominantly mixed with organic carbon, nitrate, and sulfate, and the mixing state evolved significantly as a function of relative humidity (RH) at both sites. The absorption enhancement depended strongly on coated secondary inorganic aerosol and was up to ~1.3–1.4 during aging processes.
Junjun Deng, Hao Ma, Xinfeng Wang, Shujun Zhong, Zhimin Zhang, Jialei Zhu, Yanbing Fan, Wei Hu, Libin Wu, Xiaodong Li, Lujie Ren, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 22, 6449–6470, https://doi.org/10.5194/acp-22-6449-2022, https://doi.org/10.5194/acp-22-6449-2022, 2022
Short summary
Short summary
Light-absorbing brown carbon (BrC) plays an important role in climate change and atmospheric chemistry. Here we investigated the seasonal and diurnal variations in water-soluble BrC in PM2.5 in the megacity Tianjin in coastal China. Results of the source apportionments from the combination with organic molecular compositions and optical properties of water-soluble BrC reveal a large contribution from primary bioaerosol particles to BrC in the urban atmosphere.
Jingnan Shi, Juan Hong, Nan Ma, Qingwei Luo, Yao He, Hanbing Xu, Haobo Tan, Qiaoqiao Wang, Jiangchuan Tao, Yaqing Zhou, Shuang Han, Long Peng, Linhong Xie, Guangsheng Zhou, Wanyun Xu, Yele Sun, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 4599–4613, https://doi.org/10.5194/acp-22-4599-2022, https://doi.org/10.5194/acp-22-4599-2022, 2022
Short summary
Short summary
In this study, we investigated the hygroscopicity of submicron aerosols at a rural site in the North China Plain during the winter of 2018, using a HTDMA and a CV-ToF-ACSM. We observed differences in aerosol hygroscopicity during two distinct episodes with different primary emissions and secondary aerosol formation processes. These results provide an improved understanding of the complex influence of sources and aerosol evolution processes on their hygroscopicity.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
Short summary
Short summary
This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Jiaxing Sun, Zhe Wang, Wei Zhou, Conghui Xie, Cheng Wu, Chun Chen, Tingting Han, Qingqing Wang, Zhijie Li, Jie Li, Pingqing Fu, Zifa Wang, and Yele Sun
Atmos. Chem. Phys., 22, 561–575, https://doi.org/10.5194/acp-22-561-2022, https://doi.org/10.5194/acp-22-561-2022, 2022
Short summary
Short summary
We analyzed 9-year measurements of BC and aerosol optical properties from 2012 to 2020 in Beijing, China. Our results showed large reductions in BC and light extinction coefficient due to the Clean Air Action Plan. As a response, both SSA and mass extinction efficiency (MEE) showed considerable increases, demonstrating a future challenge in visibility improvement. The primary and secondary BrC was also separated and quantified, and the changes in radiative forcing of BC and BrC were estimated.
Yuting Zhang, Hang Liu, Shandong Lei, Wanyun Xu, Yu Tian, Weijie Yao, Xiaoyong Liu, Qi Liao, Jie Li, Chun Chen, Yele Sun, Pingqing Fu, Jinyuan Xin, Junji Cao, Xiaole Pan, and Zifa Wang
Atmos. Chem. Phys., 21, 17631–17648, https://doi.org/10.5194/acp-21-17631-2021, https://doi.org/10.5194/acp-21-17631-2021, 2021
Short summary
Short summary
In this study, the authors used a single-particle soot photometer (SP2) to characterize the particle size, mixing state, and optical properties of black carbon aerosols in rural areas of the North China Plain in winter. Relatively warm and high-RH environments (RH > 50 %, −4° < T < 4 °) were more favorable to rBC aging than dry and cold environments (RH < 60 %, T < −8°). The paper emphasizes the importance of meteorological parameters in the mixing state of black carbon.
Quan Liu, Dantong Liu, Yangzhou Wu, Kai Bi, Wenkang Gao, Ping Tian, Delong Zhao, Siyuan Li, Chenjie Yu, Guiqian Tang, Yunfei Wu, Kang Hu, Shuo Ding, Qian Gao, Fei Wang, Shaofei Kong, Hui He, Mengyu Huang, and Deping Ding
Atmos. Chem. Phys., 21, 14749–14760, https://doi.org/10.5194/acp-21-14749-2021, https://doi.org/10.5194/acp-21-14749-2021, 2021
Short summary
Short summary
Through simultaneous online measurements of detailed aerosol compositions at both surface and surface-influenced mountain sites, the evolution of aerosol composition during daytime vertical transport was investigated. The results show that, from surface to the top of the planetary boundary layer, the oxidation state of organic aerosol had been significantly enhanced due to evaporation and further oxidation of these evaporated gases.
Sihui Jiang, Fang Zhang, Jingye Ren, Lu Chen, Xing Yan, Jieyao Liu, Yele Sun, and Zhanqing Li
Atmos. Chem. Phys., 21, 14293–14308, https://doi.org/10.5194/acp-21-14293-2021, https://doi.org/10.5194/acp-21-14293-2021, 2021
Short summary
Short summary
New particle formation (NPF) can be a large source of CCN and affect weather and climate. Here we show that the NPF contributes largely to cloud droplet number concentration (Nd) but is suppressed at high particle number concentrations in Beijing due to water vapor competition. We also reveal a considerable impact of primary sources on the evaluation in the urban atmosphere. Our study has great significance for assessing NPF-associated effects on climate in polluted regions.
Hong Ren, Wei Hu, Lianfang Wei, Siyao Yue, Jian Zhao, Linjie Li, Libin Wu, Wanyu Zhao, Lujie Ren, Mingjie Kang, Qiaorong Xie, Sihui Su, Xiaole Pan, Zifa Wang, Yele Sun, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 21, 12949–12963, https://doi.org/10.5194/acp-21-12949-2021, https://doi.org/10.5194/acp-21-12949-2021, 2021
Short summary
Short summary
This study presents vertical profiles of biogenic and anthropogenic secondary organic aerosols (SOAs) in the urban boundary layer based on a 325 m tower in Beijing in late summer. The increases in the isoprene and toluene SOAs with height were found to be more related to regional transport, whereas the decrease in those from monoterpenes and sesquiterpene were more subject to local emissions. Such complicated vertical distributions of SOA should be considered in future modeling work.
Yang Yang, Minqiang Zhou, Ting Wang, Bo Yao, Pengfei Han, Denghui Ji, Wei Zhou, Yele Sun, Gengchen Wang, and Pucai Wang
Atmos. Chem. Phys., 21, 11741–11757, https://doi.org/10.5194/acp-21-11741-2021, https://doi.org/10.5194/acp-21-11741-2021, 2021
Short summary
Short summary
This study introduces the in situ CO2 measurement system installed in Beijing (urban), Xianghe (suburban), and Xinglong (rural) in North China for the first time. The spatial and temporal variations in CO2 mole fractions at the three sites between June 2018 and April 2020 are discussed on both seasonal and diurnal scales.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
Short summary
Short summary
This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Ying Wei, Xueshun Chen, Huansheng Chen, Yele Sun, Wenyi Yang, Huiyun Du, Qizhong Wu, Dan Chen, Xiujuan Zhao, Jie Li, and Zifa Wang
Geosci. Model Dev., 14, 4411–4428, https://doi.org/10.5194/gmd-14-4411-2021, https://doi.org/10.5194/gmd-14-4411-2021, 2021
Short summary
Short summary
The sub-grid particle formation (SGPF) in plumes plays an important role in air pollution and climate. We coupled an SGPF scheme to a chemical transport model with an aerosol microphysics module and applied it to investigate the SGPF impact over China. The scheme clearly improved the model performance in simulating aerosol components and particle number at typical sites influenced by point sources. The results indicate the significant effects of SGPF on aerosol particles in industrial areas.
Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
Atmos. Chem. Phys., 21, 9343–9366, https://doi.org/10.5194/acp-21-9343-2021, https://doi.org/10.5194/acp-21-9343-2021, 2021
Short summary
Short summary
Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Zhaobin Sun, Xiujuan Zhao, Ziming Li, Guiqian Tang, and Shiguang Miao
Atmos. Chem. Phys., 21, 8863–8882, https://doi.org/10.5194/acp-21-8863-2021, https://doi.org/10.5194/acp-21-8863-2021, 2021
Short summary
Short summary
Different weather types will shape significantly different structures of the pollution boundary layer. The findings of this study allow us to understand the inherent difference among heavy pollution boundary layers; in addition, they reveal the formation mechanism of haze pollution from an integrated synoptic-scale and boundary layer structure perspective.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
Short summary
Short summary
This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
Short summary
Short summary
Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Jiangchuan Tao, Ye Kuang, Nan Ma, Juan Hong, Yele Sun, Wanyun Xu, Yanyan Zhang, Yao He, Qingwei Luo, Linhong Xie, Hang Su, and Yafang Cheng
Atmos. Chem. Phys., 21, 7409–7427, https://doi.org/10.5194/acp-21-7409-2021, https://doi.org/10.5194/acp-21-7409-2021, 2021
Short summary
Short summary
The mechanism of secondary aerosol (SA) formation can be affected by relative humidity (RH) and has different influences on the particle CCN activity under different RH conditions. In the North China Plain, we find different responses of CCN activity and enhancements of CCN number concentration to SA formation under different RH conditions. In addition, variations of aerosol mixing state due to SA formation contribute some of the largest uncertainties in predicting CCN number concentration.
Jingsha Xu, Di Liu, Xuefang Wu, Tuan V. Vu, Yanli Zhang, Pingqing Fu, Yele Sun, Weiqi Xu, Bo Zheng, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 7321–7341, https://doi.org/10.5194/acp-21-7321-2021, https://doi.org/10.5194/acp-21-7321-2021, 2021
Short summary
Short summary
Source apportionment of fine aerosols in an urban site of Beijing used a chemical mass balance (CMB) model. Seven primary sources (industrial/residential coal burning, biomass burning, gasoline/diesel vehicles, cooking and vegetative detritus) explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. CMB was found to resolve more primary OA sources than AMS-PMF, but the latter apportioned more secondary OA sources.
Cited articles
Benkovitz, C. M., Scholtz, M. T., Pacyna, J., Tarrason, L., Dignon, J.,
Voldner, E. C., Spiro, P. A., Logan, J. A., and Graedel, T. E.: Global
gridded inventories of anthropogenic emissions of sulfur and nitrogen, J.
Geophys. Res.-Atmos., 101, 29239–29253, https://doi.org/10.1029/96jd00126, 1996.
Boylan, J. W. and Russell, A. G.: PM and light extinction model performance
metrics, goals, and criteria for three-dimensional air quality models, Atmos.
Environ., 40, 4946–4959, https://doi.org/10.1016/j.atmonsenv.2005.09.087,
2006.
Byun, D. and Schere, K. L.: Review of the governing equations,
computational algorithms, and other components of the models-3 Community
Multiscale Air Quality (CMAQ) modeling system, Appl. Mech. Rev., 59, 51–77,
https://doi.org/10.1115/1.2128636, 2006.
Carlton, A. G., Turpin, B. J., Lim, H. J., Altieri, K. E., and Seitzinger,
S.: Link between isoprene and secondary organic aerosol (SOA): Pyruvic acid
oxidation yields low volatility organic acids in clouds, Geophys. Res. Lett.,
33, 272–288, 2006.
Carlton, A. G., Turpin, B. J., Altieri, K. E., Seitzinger, S. P., Mathur,
R., Roselle, S. J., and Weber, R. J.: CMAQ Model Performance Enhanced When
In-Cloud Secondary Organic Aerosol is Included: Comparisons of Organic Carbon
Predictions with Measurements, Environ. Sci. Technol., 42, 8798–8802,
https://doi.org/10.1021/es801192n, 2008.
Carlton, A. G., Bhave, P. V., Napelenok, S. L., Edney, E. D., Sarwar, G.,
Pinder, R. W., Pouliot, G. A., and Houyoux, M.: Model Representation of
Secondary Organic Aerosol in CMAQv4.7, Environ. Sci. Technol., 44,
8553–8560, https://doi.org/10.1021/es100636q, 2010.
Carter, W. P. L.: Implementation of the SAPRC-99 Chemical Mechanism into the
Models-3 Framework Report to the US Environmental Protection Agency, Research
Triangle Park, NC, 2000.
Chandra, B. P. and Sinha, V.: Contribution of post-harvest agricultural
paddy residue fires in the NW Indo-Gangetic Plain to ambient carcinogenic
benzenoids, toxic isocyanic acid and carbon monoxide, Environ. Int., 88,
187–197, https://doi.org/10.1016/j.envint.2015.12.025, 2016.
Corrigan, A. L., Hanley, S. W., and De Haan, D. O.: Uptake of glyoxal by
organic and inorganic aerosol, Environ. Sci. Technol., 42, 4428–4433,
https://doi.org/10.1021/es7032394, 2008.
Cotton, W. R., Pielke, R. A., Walko, R. L., Liston, G. E., Tremback, C. J.,
Jiang, H., McAnelly, R. L., Harrington, J. Y., Nicholls, M. E., Carrio, G.
G., and McFadden, J. P.: RAMS 2001: Current status and future directions,
Meteorol. Atmos. Phys., 82, 5–29, https://doi.org/10.1007/s00703-001-0584-9, 2003.
Curry, L. A., Tsui, W. G., and McNeill, V. F.: Technical note: Updated
parameterization of the reactive uptake of glyoxal and methylglyoxal by
atmospheric aerosols and cloud droplets, Atmos. Chem. Phys., 18, 9823–9830,
https://doi.org/10.5194/acp-18-9823-2018, 2018.
de Gouw, J. A., Middlebrook, A. M., Warneke, C., Goldan, P. D., Kuster, W.
C., Roberts, J. M., Fehsenfeld, F. C., Worsnop, D. R., Canagaratna, M. R.,
Pszenny, A. A. P., Keene, W. C., Marchewka, M., Bertman, S. B., and Bates, T.
S.: Budget of organic carbon in a polluted atmosphere: Results from the New
England Air Quality Study in 2002, J. Geophys. Res.-Atmos., 110,
D16305, https://doi.org/10.1029/2004jd005623, 2005.
De Haan, D. O., Jimenez, N. G., de Loera, A., Cazaunau, M., Gratien, A.,
Pangui, E., and Doussin, J.-F.: Methylglyoxal Uptake Coefficients on Aqueous
Aerosol Surfaces, J. Phys. Chem. A, 122, 4854–4860,
https://doi.org/10.1021/acs.jpca.8b00533, 2018.
Dentener, F. J. and Crutzen, P. J.: Reaction of N2O5 on tropospheric
aerosols – impact on the global distributions of NOx, O3,
and OH, J. Geophys. Res.-Atmos., 98, 7149–7163, https://doi.org/10.1029/92jd02979, 1993.
Emery, C., Tai, E., and Yarwood, G.: Enhanced meteorological modeling and
performance evaluation for two Texas ozone episodes, In: Prepared for the
Texas Natural Resource Conservation Commission, ENVIRON International
Corporation, Novato, CA, USA, 2001.
Emmons, L. K., Walters, S., Hess, P. G., Lamarque, J.-F., Pfister, G. G.,
Fillmore, D., Granier, C., Guenther, A., Kinnison, D., Laepple, T., Orlando,
J., Tie, X., Tyndall, G., Wiedinmyer, C., Baughcum, S. L., and Kloster, S.:
Description and evaluation of the Model for Ozone and Related chemical
Tracers, version 4 (MOZART-4), Geosci. Model Dev., 3, 43–67,
https://doi.org/10.5194/gmd-3-43-2010, 2010.
Ervens, B. and Volkamer, R.: Glyoxal processing by aerosol multiphase
chemistry: towards a kinetic modeling framework of secondary organic aerosol
formation in aqueous particles, Atmos. Chem. Phys., 10, 8219–8244,
https://doi.org/10.5194/acp-10-8219-2010, 2010.
Ervens, B., Feingold, G., Frost, G. J., and Kreidenweis, S. M.: A modeling
study of aqueous production of dicarboxylic acids: 1. Chemical pathways and
speciated organic mass production, J. Geophys. Res.-Atmos., 109, D15205,
https://doi.org/10.1029/2003JD004387, 2004.
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol
formation in cloud droplets and aqueous particles (aqSOA): a review of
laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102,
https://doi.org/10.5194/acp-11-11069-2011, 2011.
Ervens, B., Sorooshian, A., Lim, Y. B., and Turpin, B. J.: Key parameters
controlling OH-initiated formation of secondary organic aerosol in the
aqueous phase (aqSOA), J. Geophys. Res.-Atmos., 119, 3997–4016,
https://doi.org/10.1002/2013jd021021, 2014.
Farina, S. C., Adams, P. J., and Pandis, S. N.: Modeling global secondary
organic aerosol formation and processing with the volatility basis set:
Implications for anthropogenic secondary organic aerosol, J. Geophys.
Res.-Atmos., 115, D09202, https://doi.org/10.1029/2009jd013046, 2010.
Feng, T., Bei, N., Huang, R.-J., Cao, J., Zhang, Q., Zhou, W., Tie, X., Liu,
S., Zhang, T., Su, X., Lei, W., Molina, L. T., and Li, G.: Summertime ozone
formation in Xi'an and surrounding areas, China, Atmos. Chem. Phys., 16,
4323–4342, https://doi.org/10.5194/acp-16-4323-2016, 2016.
Foley, K. M., Roselle, S. J., Appel, K. W., Bhave, P. V., Pleim, J. E., Otte,
T. L., Mathur, R., Sarwar, G., Young, J. O., Gilliam, R. C., Nolte, C. G.,
Kelly, J. T., Gilliland, A. B., and Bash, J. O.: Incremental testing of the
Community Multiscale Air Quality (CMAQ) modeling system version 4.7, Geosci.
Model Dev., 3, 205–226, https://doi.org/10.5194/gmd-3-205-2010, 2010.
Fu, T.-M., Jacob, D. J., Wittrock, F., Burrows, J. P., Vrekoussis, M., and
Henze, D. K.: Global budgets of atmospheric glyoxal and methylglyoxal, and
implications for formation of secondary organic aerosols, J. Geophys.
Res.-Atmos., 113, D15303, https://doi.org/10.1029/2007jd009505, 2008.
Fu, T. M., Jacob, D. J., and Heald, C. L.: Aqueous-phase reactive uptake of
dicarbonyls as a source of organic aerosol over eastern North America, Atmos.
Environ., 43, 1814–1822, 2009.
Galloway, M. M., Chhabra, P. S., Chan, A. W. H., Surratt, J. D., Flagan, R.
C., Seinfeld, J. H., and Keutsch, F. N.: Glyoxal uptake on ammonium sulphate
seed aerosol: reaction products and reversibility of uptake under dark and
irradiated conditions, Atmos. Chem. Phys., 9, 3331–3345,
https://doi.org/10.5194/acp-9-3331-2009, 2009.
Gao, M., Carmichael, G. R., Wang, Y., Saide, P. E., Yu, M., Xin, J., Liu, Z.,
and Wang, Z.: Modeling study of the 2010 regional haze event in the North
China Plain, Atmos. Chem. Phys., 16, 1673–1691,
https://doi.org/10.5194/acp-16-1673-2016, 2016.
Goldstein, A. H. and Galbally, I. E.: Known and unexplored organic
constituents in the earth's atmosphere, Environ. Sci. Technol., 41,
1514–1521, https://doi.org/10.1021/es072476p, 2007.
Gong, S. L.: A parameterization of sea-salt aerosol source function for sub-
and super-micron particles, Global Biogeochem. Cy., 17, 1097,
https://doi.org/10.1029/2003gb002079, 2003.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T.,
Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols
from Nature version 2.1 (MEGAN2.1): an extended and updated framework for
modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492,
https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Han, Z., Xie, Z., Wang, G., Zhang, R., and Tao, J.: Modeling organic
aerosols over east China using a volatility basis-set approach with aging
mechanism in a regional air quality model, Atmos. Environ., 124, 186–198,
https://doi.org/10.1016/j.atmosenv.2015.05.045, 2016.
Han, Z. W., Ueda, H., Matsuda, K., Zhang, R. J., Arao, K., Kanai, Y., and
Hasome, H.: Model study on particle size segregation and deposition during
Asian dust events in March 2002, J. Geophys. Res.-Atmos., 109, D19205,
https://doi.org/10.1029/2004jd004920, 2004.
Harrison, R. M. and Yin, J. X.: Particulate matter in the atmosphere: which
particle properties are important for its effects on health?, Sci. Total
Environ., 249, 85–101, https://doi.org/10.1016/s0048-9697(99)00513-6, 2000.
Heald, C. L., Jacob, D. J., Park, R. J., Russell, L. M., Huebert, B. J.,
Seinfeld, J. H., Liao, H., and Weber, R. J.: A large organic aerosol source
in the free troposphere missing from current models, Geophys. Res. Lett., 32,
L18809, https://doi.org/10.1029/2005gl023831, 2005.
Hu, J., Wang, P., Ying, Q., Zhang, H., Chen, J., Ge, X., Li, X., Jiang, J.,
Wang, S., Zhang, J., Zhao, Y., and Zhang, Y.: Modeling biogenic and
anthropogenic secondary organic aerosol in China, Atmos. Chem. Phys., 17,
77–92, https://doi.org/10.5194/acp-17-77-2017, 2017.
Intergovernmental Panel on Climate Change (IPCC): The Physical Science Basis
of Climate Change: Changes in Atmospheric Constituents and in Radiative
Forcing, Cambridge University Press, New York, 26–27, 2007.
Jacob, D. J.: Heterogeneous chemistry and tropospheric ozone, Atmos.
Environ., 34, 2131–2159, https://doi.org/10.1016/s1352-2310(99)00462-8, 2000.
Jiang, F., Liu, Q., Huang, X., Wang, T., Zhuang, B., and Xie, M.: Regional
modeling of secondary organic aerosol over China using WRF/Chem, J. Aerosol
Sci., 43, 57–73, https://doi.org/10.1016/j.jaerosci.2011.09.003, 2012.
Jo, D. S., Park, R. J., Kim, M. J., and Spracklen, D. V.: Effects of
chemical aging on global secondary organic aerosol using the volatility basis
set approach, Atmos. Environ., 81, 230–244,
https://doi.org/10.1016/j.atmosenv.2013.08.055, 2013.
Juda-Rezler, K., Reizer, M., Huszar, P., Krueger, B. C., Zanis, P., Syrakov,
D., Katragkou, E., Trapp, W., Melas, D., Chervenkov, H., Tegoulias, I., and
Halenka, T.: Modelling the effects of climate change on air quality over
Central and Eastern Europe: concept, evaluation and projections, Clim. Res.,
53, 179–203, https://doi.org/10.3354/cr01072, 2012.
Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A.
S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and
Baltensperger, U.: Identification of polymers as major components of
atmospheric organic aerosols, Science, 303, 1659–1662,
https://doi.org/10.1126/science.1092185, 2004.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J.,
Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J.,
Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat,
G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E.,
Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate
modelling: a review, Atmos. Chem. Phys., 5, 1053–1123,
https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C., and Seinfeld, J. H.:
Secondary organic aerosol formation from isoprene photooxidation under
high-NOx conditions, Geophys. Res. Lett., 32, L18808, https://doi.org/10.1029/2005gl023637,
2005.
Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C., and Seinfeld, J. H.:
Secondary organic aerosol formation from isoprene photooxidation, Environ.
Sci. Technol., 40, 1869–1877, https://doi.org/10.1021/es0524301, 2006.
Kurokawa, J., Ohara, T., Morikawa, T., Hanayama, S., Janssens-Maenhout, G.,
Fukui, T., Kawashima, K., and Akimoto, H.: Emissions of air pollutants and
greenhouse gases over Asian regions during 2000–2008: Regional Emission
inventory in ASia (REAS) version 2, Atmos. Chem. Phys., 13, 11019–11058,
https://doi.org/10.5194/acp-13-11019-2013, 2013.
Lal, V., Khalizov, A. F., Lin, Y., Galvan, M. D., Connell, B. T., and Zhang,
R.: Heterogeneous reactions of epoxides in acidic media, J. Phys. Chem. A,
116, 6078–6090, https://doi.org/10.1021/jp2112704, 2012.
Lane, T. E., Donahue, N. M., and Pandis, S. N.: Simulating secondary organic
aerosol formation using the volatility basis-set approach in a chemical
transport model, Atmos. Environ., 42, 7439–7451,
https://doi.org/10.1016/j.atmosenv.2008.06.026, 2008.
Li, J., Mao, J., Min, K.-E., Washenfelder, R. A., Brown, S. S., Kaiser, J.,
Keutsch, F. N., Volkamer, R., Wolfe, G. M., Hanisco, T. F., Pollack, I. B.,
Ryerson, T. B., Graus, M., Gilman, J. B., Lerner, B. M., Warneke, C., de
Gouw, J. A., Middlebrook, A. M., Liao, J., Welti, A., Henderson, B. H.,
McNeill, V. F., Hall, S. R., Ullmann, K., Donner, L. J., Paulot, F., and
Horowitz, L. W.: Observational constraints on glyoxal production from
isoprene oxidation and its contribution to organic aerosol over the Southeast
United States, J. Geophys. Res.-Atmos., 121, 9849–9861,
https://doi.org/10.1002/2016jd025331, 2016.
Li, J., Zhang, M., Wu, F., Sun, Y., and Tang, G.: Assessment of the impacts
of aromatic VOC emissions and yields of SOA on SOA concentrations with the
air quality model RAMS-CMAQ, Atmos. Environ., 158, 105–115,
https://doi.org/10.1016/j.atmosenv.2017.03.035, 2017.
Li, J., Zhang, M., Tang, G., Wu, F., Alvarado, L. M. A., Vrekoussis, M.,
Richter, A., and Burrows, J. P.: Investigating missing sources of glyoxal
over China using a regional air quality model (RAMS-CMAQ), J. Environ. Sci.,
71, 108–118, https://doi.org/10.1016/j.jes.2018.04.021, 2018.
Li, L., Chen, C. H., Huang, C., Huang, H. Y., Zhang, G. F., Wang, Y. J.,
Wang, H. L., Lou, S. R., Qiao, L. P., Zhou, M., Chen, M. H., Chen, Y. R.,
Streets, D. G., Fu, J. S., and Jang, C. J.: Process analysis of regional
ozone formation over the Yangtze River Delta, China using the Community
Multi-scale Air Quality modeling system, Atmos. Chem. Phys., 12,
10971–10987, https://doi.org/10.5194/acp-12-10971-2012, 2012.
Li, M., Zhang, Q., Kurokawa, J.-I., Woo, J.-H., He, K., Lu, Z., Ohara, T.,
Song, Y., Streets, D. G., Carmichael, G. R., Cheng, Y., Hong, C., Huo, H.,
Jiang, X., Kang, S., Liu, F., Su, H., and Zheng, B.: MIX: a mosaic Asian
anthropogenic emission inventory under the international collaboration
framework of the MICS-Asia and HTAP, Atmos. Chem. Phys., 17, 935–963,
https://doi.org/10.5194/acp-17-935-2017, 2017.
Li, N., Fu, T.-M., Cao, J., Lee, S., Huang, X.-F., He, L.-Y., Ho, K.-F., Fu,
J. S., and Lam, Y.-F.: Sources of secondary organic aerosols in the Pearl
River Delta region in fall: Contributions from the aqueous reactive uptake of
dicarbonyls, Atmos. Environ., 76, 200–207,
https://doi.org/10.1016/j.atmosenv.2012.12.005, 2013.
Liggio, J., Li, S. M., and Mclaren, R.: Reactive uptake of glyoxal by
particulate matter, J. Geophys. Res., 110, 257–266, 2005.
Lim, Y. B. and Ziemann, P. J.: Products and mechanism of secondary organic
aerosol formation from reactions of n-alkanes with OH radicals in the
presence of NOx, Environ. Sci. Technol., 39, 9229–9236,
https://doi.org/10.1021/es051447g, 2005.
Lim, Y. B., Tan, Y., Perri, M. J., Seitzinger, S. P., and Turpin, B. J.:
Aqueous chemistry and its role in secondary organic aerosol (SOA) formation,
Atmos. Chem. Phys., 10, 10521–10539,
https://doi.org/10.5194/acp-10-10521-2010, 2010.
Lin, G., Penner, J. E., Sillman, S., Taraborrelli, D., and Lelieveld, J.:
Global modeling of SOA formation from dicarbonyls, epoxides, organic nitrates
and peroxides, Atmos. Chem. Phys., 12, 4743–4774,
https://doi.org/10.5194/acp-12-4743-2012, 2012.
Lin, G., Sillman, S., Penner, J. E., and Ito, A.: Global modeling of SOA: the
use of different mechanisms for aqueous-phase formation, Atmos. Chem. Phys.,
14, 5451–5475, https://doi.org/10.5194/acp-14-5451-2014, 2014.
Lin, J., An, J., Qu, Y., Chen, Y., Li, Y., Tang, Y., Wang, F., and Xiang,
W.: Local and distant source contributions to secondary organic aerosol in
the Beijing urban area in summer, Atmos. Environ., 124, 176–185,
https://doi.org/10.1016/j.atmosenv.2015.08.098, 2016.
Lin, Y.-H., Zhang, H., Pye, H. O. T., Zhang, Z., Marth, W. J., Park, S.,
Arashiro, M., Cui, T., Budisulistiorini, H., Sexton, K. G., Vizuete, W., Xie,
Y., Luecken, D. J., Piletic, I. R., Edney, E. O., Bartolotti, L. J., Gold,
A., and Surratt, J. D.: Epoxide as a precursor to secondary organic aerosol
formation from isoprene photooxidation in the presence of nitrogen oxides, P.
Natl. Acad. Sci. USA, 110, 6718–6723, https://doi.org/10.1073/pnas.1221150110, 2013.
Liu, Z., Wang, Y., Vrekoussis, M., Richter, A., Wittrock, F., Burrows, J.
P., Shao, M., Chang, C.-C., Liu, S.-C., Wang, H., and Chen, C.: Exploring the
missing source of glyoxal (CHOCHO) over China, Geophys. Res. Lett., 39,
L10812, https://doi.org/10.1029/2012gl051645, 2012.
Loeffler, K. W., Koehler, C. A., Paul, N. M., and De Haan, D. O.: Oligomer
formation in evaporating aqueous glyoxal and methyl glyoxal solutions,
Environ. Sci. Technol., 40, 6318–6323, https://doi.org/10.1021/es060810w, 2006.
Morris, R. E., McNally, D. E., Tesche, T. W., Tonnesen, G., Boylan, J. W.,
and Brewer, P.: Preliminary evaluation of the community multiscale air,
quality model for 2002 over the southeastern United States, J. Air Waste
Manage., 55, 1694–1708, https://doi.org/10.1080/10473289.2005.10464765, 2005.
Morris, R. E., Koo, B., Guenther, A., Yarwood, G., McNally, D., Tesche, T.
W., Tonnesen, G., Boylan, J., and Brewer, P.: Model sensitivity evaluation
for organic carbon using two multi-pollutant air quality models that simulate
regional haze in the southeastern United States, Atmos. Environ., 40,
4960–4972, https://doi.org/10.1016/j.atmonsenv.2005.09.088, 2006.
Murphy, B. N. and Pandis, S. N.: Simulating the Formation of Semivolatile
Primary and Secondary Organic Aerosol in a Regional Chemical Transport Model,
Environ. Sci. Technol., 43, 4722–4728, https://doi.org/10.1021/es803168a, 2009.
Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M.,
Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber,
R. J.: Single-particle mass spectrometry of tropospheric aerosol particles,
J. Geophys. Res.-Atmos., 111, D23S32, https://doi.org/10.1029/2006jd007340, 2006.
Myriokefalitakis, S., Vrekoussis, M., Tsigaridis, K., Wittrock, F., Richter,
A., Brühl, C., Volkamer, R., Burrows, J. P., and Kanakidou, M.: The
influence of natural and anthropogenic secondary sources on the glyoxal
global distribution, Atmos. Chem. Phys., 8, 4965–4981,
https://doi.org/10.5194/acp-8-4965-2008, 2008.
Ng, N. L., Kroll, J. H., Chan, A. W. H., Chhabra, P. S., Flagan, R. C., and
Seinfeld, J. H.: Secondary organic aerosol formation from m-xylene,
toluene, and benzene, Atmos. Chem. Phys., 7, 3909–3922,
https://doi.org/10.5194/acp-7-3909-2007, 2007.
Perry, R. H. and Green, D.: Perry's Chemical Engineers Handbook,
McGraw-Hill, New York, 2–370, 1999.
Pöschl, U.: Atmospheric aerosols: Composition, transformation, climate and
health effects, Angew. Chem. Int. Edit., 44, 7520–7540,
https://doi.org/10.1002/anie.200501122, 2005.
Randerson, J. T., van der Werf, G. R., Giglio, L., Collatz, G. J., and Kasibhatla,
P. S.: Global fire emissions database, version 4 (GFEDv4), Data set available
at: http://daac.ornl.gov/ (last access: 16 April 2019),
from Oak Ridge National Laboratory Distributed Active Archive Center, Oak
Ridge, Tennessee, USA, https://doi.org/10.3334/ORNLDAAC/1293, 2015.
Roberts, M. C., Andreae, M. O., Zhou, J. C., and Artaxo, P.: Cloud
condensation nuclei in the Amazon Basin: “Marine” conditions over a
continent?, Geophys. Res. Lett., 28, 2807–2810, 2001.
Shrivastava, M. K., Lane, T. E., Donahue, N. M., Pandis, S. N., and
Robinson, A. L.: Effects of gas particle partitioning and aging of primary
emissions on urban and regional organic aerosol concentrations, J. Geophys.
Res.-Atmos., 113, D18301, https://doi.org/10.1029/2007jd009735, 2008.
Stavrakou, T., Mueller, J. F., De Smedt, I., Van Roozendael, M., Kanakidou,
M., Vrekoussis, M., Wittrock, F., Richter, A., and Burrows, J. P.: The
continental source of glyoxal estimated by the synergistic use of spaceborne
measurements and inverse modelling, Atmos. Chem. Phys., 9, 8431–8446,
https://doi.org/10.5194/acp-9-8431-2009, 2009.
Stavrakou, T., Peeters, J., and Müller, J.-F.: Improved global modelling of
HOx recycling in isoprene oxidation: evaluation against the GABRIEL
and INTEX-A aircraft campaign measurements, Atmos. Chem. Phys., 10,
9863–9878, https://doi.org/10.5194/acp-10-9863-2010, 2010.
Sun, J., Wu, F., Hu, B., Tang, G., Zhang, J., and Wang, Y.: VOC
characteristics, emissions and contributions to SOA formation during hazy
episodes, Atmos. Environ., 141, 560–570, https://doi.org/10.1016/j.atmosenv.2016.06.060,
2016.
Surratt, J. D., Lewandowski, M., Offenberg, J. H., Jaoui, M., Kleindienst,
T. E., Edney, E. O., and Seinfeld, J. H.: Effect of acidity on secondary
organic aerosol formation from isoprene, Environ. Sci. Technol., 41,
5363–5369, https://doi.org/10.1021/es0704176, 2007.
Tsigaridis, K., Daskalakis, N., Kanakidou, M., Adams, P. J., Artaxo, P.,
Bahadur, R., Balkanski, Y., Bauer, S. E., Bellouin, N., Benedetti, A.,
Bergman, T., Berntsen, T. K., Beukes, J. P., Bian, H., Carslaw, K. S., Chin,
M., Curci, G., Diehl, T., Easter, R. C., Ghan, S. J., Gong, S. L., Hodzic,
A., Hoyle, C. R., Iversen, T., Jathar, S., Jimenez, J. L., Kaiser, J. W.,
Kirkevåg, A., Koch, D., Kokkola, H., Lee, Y. H., Lin, G., Liu, X., Luo,
G., Ma, X., Mann, G. W., Mihalopoulos, N., Morcrette, J.-J., Müller,
J.-F., Myhre, G., Myriokefalitakis, S., Ng, N. L., O'Donnell, D., Penner, J.
E., Pozzoli, L., Pringle, K. J., Russell, L. M., Schulz, M., Sciare, J.,
Seland, Ø., Shindell, D. T., Sillman, S., Skeie, R. B., Spracklen, D.,
Stavrakou, T., Steenrod, S. D., Takemura, T., Tiitta, P., Tilmes, S., Tost,
H., van Noije, T., van Zyl, P. G., von Salzen, K., Yu, F., Wang, Z., Wang,
Z., Zaveri, R. A., Zhang, H., Zhang, K., Zhang, Q., and Zhang, X.: The
AeroCom evaluation and intercomparison of organic aerosol in global models,
Atmos. Chem. Phys., 14, 10845–10895,
https://doi.org/10.5194/acp-14-10845-2014, 2014.
Volkamer, R., Jimenez, J. L., San Martini, F., Dzepina, K., Zhang, Q.,
Salcedo, D., Molina, L. T., Worsnop, D. R., and Molina, M. J.: Secondary
organic aerosol formation from anthropogenic air pollution: Rapid and higher
than expected, Geophys. Res. Lett., 33, L17811, https://doi.org/10.1029/2006gl026899,
2006.
Wang, F., An, J., Li, Y., Tang, Y., Lin, J., Qu, Y., Chen, Y., Zhang, B.,
and Zhai, J.: Impacts of uncertainty in AVOC emissions on the summer
ROx budget and ozone production rate in the three most
rapidly-developing economic growth regions of China, Adv. Atmos. Sci., 31,
1331–1342, https://doi.org/10.1007/s00376-014-3251-z, 2014.
Warneck, P.: In-cloud chemistry opens pathway to the formation of oxalic
acid in the marine atmosphere, Atmos. Environ., 37, 2423–2427,
https://doi.org/10.1016/s1352-2310(03)00136-5, 2003.
Willmott, C. J.: On the validation of models, Phys. Geogr., 2,
184–194, https://doi.org/10.1080/02723646.1981.10642213, 1981.
Woo, J. L. and McNeill, V. F.: simpleGAMMA v1.0 – a reduced model of
secondary organic aerosol formation in the aqueous aerosol phase (aaSOA),
Geosci. Model Dev., 8, 1821–1829, https://doi.org/10.5194/gmd-8-1821-2015,
2015.
Wu, F., Yu, Y., Sun, J., Zhang, J., Wang, J., Tang, G., and Wang, Y.:
Characteristics, source apportionment and reactivity of ambient volatile
organic compounds at Dinghu Mountain in Guangdong Province, China, Sci. Total
Environ., 548, 347–359, https://doi.org/10.1016/j.scitotenv.2015.11.069,
2016.
Xu, W., Han, T., Du, W., Wang, Q., Chen, C., Zhao, J., Zhang, Y., Li, J.,
Fu, P., Wang, Z., Worsnop, D. R., and Sun, Y.: Effects of Aqueous-Phase and
Photochemical Processing on Secondary Organic Aerosol Formation and Evolution
in Beijing, China, Environ. Sci. Technol., 51, 762–770,
https://doi.org/10.1021/acs.est.6b04498, 2017.
Xu, W. Q., Sun, Y. L., Chen, C., Du, W., Han, T. T., Wang, Q. Q., Fu, P. Q.,
Wang, Z. F., Zhao, X. J., Zhou, L. B., Ji, D. S., Wang, P. C., and Worsnop,
D. R.: Aerosol composition, oxidation properties, and sources in Beijing:
results from the 2014 Asia-Pacific Economic Cooperation summit study, Atmos.
Chem. Phys., 15, 13681–13698, https://doi.org/10.5194/acp-15-13681-2015,
2015.
Ying, Q., Li, J., and Kota, S. H.: Significant Contributions of Isoprene to
Summertime Secondary Organic Aerosol in Eastern United States, Environ. Sci.
Technol., 49, 7834–7842, https://doi.org/10.1021/acs.est.5b02514, 2015.
Yu, S., Mathur, R., Schere, K., Kang, D., Pleim, J., Young, J., Tong, D.,
Pouliot, G., McKeen, S. A., and Rao, S. T.: Evaluation of real-time
PM2.5 forecasts and process analysis for PM2.5 formation over the
eastern United States using the Eta-CMAQ forecast model during the 2004
ICARTT study, J. Geophys. Res.-Atmos., 113, D06204, https://doi.org/10.1029/2007jd009226,
2008.
Zhang, H. and Ying, Q.: Secondary organic aerosol from polycyclic aromatic
hydrocarbons in Southeast Texas, Atmos. Environ., 55, 279–287,
https://doi.org/10.1016/j.atmosenv.2012.03.043, 2012.
Zhang, H. and Ying, Q.: Secondary organic aerosol formation and source
apportionment in Southeast Texas, Atmos. Environ., 45, 3217–3227,
https://doi.org/10.1016/j.atmosenv.2011.03.046, 2011.
Zhang, H., Li, J., Ying, Q., Yu, J. Z., Wu, D., Cheng, Y., He, K., and
Jiang, J.: Source apportionment of PM2.5 nitrate and sulfate in China
using a source-oriented chemical transport model, Atmos. Environ., 62,
228–242, https://doi.org/10.1016/j.atmosenv.2012.08.014, 2012.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H.,
Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L.,
Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch,
T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N.,
Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian,
K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J.,
Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and
dominance of oxygenated species in organic aerosols in
anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res.
Lett., 34, L13801, https://doi.org/10.1029/2007gl029979, 2007.
Short summary
There are large uncertainties in the sources of secondary organic aerosol (SOA). Simulations of SOA concentrations in China with aqueous SOA formation pathway updated and glyoxal simulation improved reveal that dicarbonyl-derived SOA (AAQ) can explain a significant fraction of the unaccounted SOA sources. The mean AAQ can contribute 60.6 % and 64.5 % to the total concentration of SOA in summer and fall, respectively.
There are large uncertainties in the sources of secondary organic aerosol (SOA). Simulations of...
Altmetrics
Final-revised paper
Preprint