Articles | Volume 20, issue 24
https://doi.org/10.5194/acp-20-15835-2020
© Author(s) 2020. 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-20-15835-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
19 Dec 2020
Research article |
| 19 Dec 2020
| 19 Dec 2020
Influence of aerosol copper on HO2 uptake: a novel parameterized equation
Huan Song
State Key Joint Laboratory or Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing, China
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Xiaorui Chen
State Key Joint Laboratory or Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing, China
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
State Key Joint Laboratory or Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing, China
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Qi Zou
State Key Joint Laboratory or Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing, China
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Zhaofeng Tan
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Hendrik Fuchs
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Alfred Wiedensohler
Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany
Daniel R. Moon
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
LISA, Université Paris-Est Créteil, Université de Paris,
Faculté des Sciences et Technologie, 61 avenue du Général de
Gaulle, 94010 Créteil, CEDEX, France
Dwayne E. Heard
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
María-Teresa Baeza-Romero
Universidad de Castilla-La Mancha, Escuela de Ingeniería Industrial
y Aeroespacial de Toledo, 45071 Toledo, Spain
Mei Zheng
State Key Joint Laboratory or Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing, China
Andreas Wahner
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Astrid Kiendler-Scharr
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Yuanhang Zhang
State Key Joint Laboratory or Environmental Simulation and Pollution
Control, College of Environmental Sciences and Engineering, Peking
University, Beijing, China
International Joint Laboratory for Regional Pollution Control, Jülich, Germany
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Junhua Wang, Baozhu Ge, Xueshun Chen, Jie Li, Keding Lu, Yayuan Dong, Lei Kong, Zifa Wang, and Yuanhang Zhang
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Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774, https://doi.org/10.5194/acp-23-4763-2023, https://doi.org/10.5194/acp-23-4763-2023, 2023
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Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
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Tianyu Zhai, Keding Lu, Haichao Wang, Shengrong Lou, Xiaorui Chen, Renzhi Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 2379–2391, https://doi.org/10.5194/acp-23-2379-2023, https://doi.org/10.5194/acp-23-2379-2023, 2023
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Particulate nitrate is a growing issue in air pollution. Based on comprehensive field measurement, we show heavy nitrate pollution in eastern China in summer. OH reacting with NO2 at daytime dominates nitrate formation on clean days, while N2O5 hydrolysis largely enhances and become comparable with that of OH reacting with O2 on polluted days (67.2 % and 30.2 %). Model simulation indicates that VOC : NOx = 2 : 1 is effective in mitigating the O3 and nitrate pollution coordinately.
Adelaide Dinoi, Daniel Gulli, Kay Weinhold, Ivano Ammoscato, Claudia R. Calidonna, Alfred Wiedensohler, and Daniele Contini
Atmos. Chem. Phys., 23, 2167–2181, https://doi.org/10.5194/acp-23-2167-2023, https://doi.org/10.5194/acp-23-2167-2023, 2023
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In this study, particle number size distribution analysis was performed with the purpose of characterizing new particle formation (NPF) events occurring in two areas of southern Italy over 5 years of measurements. The identification of NPF events produced different results in terms of frequency and seasonality. Some of the main variables involved in the process, the local atmospheric conditions in which the events occurred, and the role of the air masses were discussed and compared.
Changmin Cho, Hendrik Fuchs, Andreas Hofzumahaus, Frank Holland, William J. Bloss, Birger Bohn, Hans-Peter Dorn, Marvin Glowania, Thorsten Hohaus, Lu Liu, Paul S. Monks, Doreen Niether, Franz Rohrer, Roberto Sommariva, Zhaofeng Tan, Ralf Tillmann, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Chem. Phys., 23, 2003–2033, https://doi.org/10.5194/acp-23-2003-2023, https://doi.org/10.5194/acp-23-2003-2023, 2023
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With this study, we investigated the processes leading to the formation, destruction, and recycling of radicals for four seasons in a rural environment. Complete knowledge of their chemistry is needed if we are to predict the formation of secondary pollutants from primary emissions. The results highlight a still incomplete understanding of the paths leading to the formation of the OH radical, which has been observed in several other environments as well and needs to be further investigated.
Suding Yang, Xin Li, Limin Zeng, Xuena Yu, Ying Liu, Sihua Lu, Xiaofeng Huang, Dongmei Zhang, Haibin Xu, Shuchen Lin, Hefan Liu, Miao Feng, Danlin Song, Qinwen Tan, Jinhui Cui, Lifan Wang, Ying Chen, Wenjie Wang, Haijiong Sun, Mengdi Song, Liuwei Kong, Yi Liu, Linhui Wei, Xianwu Zhu, and Yuanhang Zhang
Atmos. Meas. Tech., 16, 501–512, https://doi.org/10.5194/amt-16-501-2023, https://doi.org/10.5194/amt-16-501-2023, 2023
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Vertical observation of volatile organic compounds (VOCs) is essential to study the spatial distribution and evolution patterns of VOCs in the planetary boundary layer (PBL). This paper describes multi-channel whole-air sampling equipment onboard an unmanned aerial vehicle (UAV) for near-continuous VOC vertical observation. Vertical profiles of VOCs and trace gases during the evolution of the PBL in south-western China have been successfully obtained by deploying the newly developed UAV system.
Tobias Schuldt, Georgios I. Gkatzelis, Christian Wesolek, Franz Rohrer, Benjamin Winter, Thomas A. J. Kuhlbusch, Astrid Kiendler-Scharr, and Ralf Tillmann
Atmos. Meas. Tech., 16, 373–386, https://doi.org/10.5194/amt-16-373-2023, https://doi.org/10.5194/amt-16-373-2023, 2023
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We report in situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin NT in Germany. We highlight the in-flight evaluation of electrochemical sensors that were installed inside a hatch box located on the bottom of the Zeppelin. Results from this work emphasize the potential of these sensors for other in situ airborne applications, e.g., on board unmanned aerial vehicles (UAVs).
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
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The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities to but also distinct differences from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
Tingting Hu, Yu Lin, Run Liu, Yuepeng Xu, Boguang Wang, Yuanhang Zhang, and Shaw Chen Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-781, https://doi.org/10.5194/acp-2022-781, 2023
Revised manuscript not accepted
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We hypothesize that the cause of the worsening O3 trends in the Beijing-Tianjin-Hebei region, the Yangtze River Delta, and the Pearl River Delta from 2015 to 2020 is attributable to the increased occurrence of meteorological conditions of high solar radiation and positive temperature anomaly under the influence of West Pacific Subtropical High, tropical cyclones as well as mid-high latitude wave activities.
Yuan Wang, Silvia Henning, Laurent Poulain, Chunsong Lu, Frank Stratmann, Yuying Wang, Shengjie Niu, Mira L. Pöhlker, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 15943–15962, https://doi.org/10.5194/acp-22-15943-2022, https://doi.org/10.5194/acp-22-15943-2022, 2022
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Aerosol particle activation affects cloud, precipitation, radiation, and thus the global climate. Its long-term measurements are important but still scarce. In this study, more than 4 years of measurements at a central European station were analyzed. The overall characteristics and seasonal changes of aerosol particle activation are summarized. The power-law fit between particle hygroscopicity factor and diameter was recommended for predicting cloud
condensation nuclei number concentration.
Xiaorui Chen, Haichao Wang, Tianyu Zhai, Chunmeng Li, and Keding Lu
Atmos. Meas. Tech., 15, 7019–7037, https://doi.org/10.5194/amt-15-7019-2022, https://doi.org/10.5194/amt-15-7019-2022, 2022
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N2O5 is an important reservoir of atmospheric nitrogen, on whose interface reaction ambient particles can largely influence the fate of nitrogen oxides and air quality. In this study, we develop an approach to enable the reactions of N2O5 on ambient particles directly in a tube reactor, deriving the reaction rates with high accuracy by means of a chemistry model. Its successful application helps complement the data scarcity and to fill the knowledge gap between laboratory and field results.
Baseerat Romshoo, Mira Pöhlker, Alfred Wiedensohler, Sascha Pfeifer, Jorge Saturno, Andreas Nowak, Krzysztof Ciupek, Paul Quincey, Konstantina Vasilatou, Michaela N. Ess, Maria Gini, Konstantinos Eleftheriadis, Chris Robins, François Gaie-Levrel, and Thomas Müller
Atmos. Meas. Tech., 15, 6965–6989, https://doi.org/10.5194/amt-15-6965-2022, https://doi.org/10.5194/amt-15-6965-2022, 2022
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Black carbon (BC) is often assumed to be spherically shaped, causing uncertainties in its optical properties when modelled. This study investigates different modelling techniques for the optical properties of BC by comparing them to laboratory measurements. We provide experimental support for emphasizing the use of appropriate size representation (polydisperse size method) and morphological representation (aggregate morphology) for optical modelling and parameterization scheme development of BC.
Haichao Wang, Bin Yuan, E Zheng, Xiaoxiao Zhang, Jie Wang, Keding Lu, Chenshuo Ye, Lei Yang, Shan Huang, Weiwei Hu, Suxia Yang, Yuwen Peng, Jipeng Qi, Sihang Wang, Xianjun He, Yubin Chen, Tiange Li, Wenjie Wang, Yibo Huangfu, Xiaobing Li, Mingfu Cai, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 14837–14858, https://doi.org/10.5194/acp-22-14837-2022, https://doi.org/10.5194/acp-22-14837-2022, 2022
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We present intensive field measurement of ClNO2 in the Pearl River Delta in 2019. Large variation in the level, formation, and atmospheric impacts of ClNO2 was found in different air masses. ClNO2 formation was limited by the particulate chloride (Cl−) and aerosol surface area. Our results reveal that Cl− originated from various anthropogenic emissions rather than sea sources and show minor contribution to the O3 pollution and photochemistry.
Zhaofeng Tan, Hendrik Fuchs, Andreas Hofzumahaus, William J. Bloss, Birger Bohn, Changmin Cho, Thorsten Hohaus, Frank Holland, Chandrakiran Lakshmisha, Lu Liu, Paul S. Monks, Anna Novelli, Doreen Niether, Franz Rohrer, Ralf Tillmann, Thalassa S. E. Valkenburg, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Roberto Sommariva
Atmos. Chem. Phys., 22, 13137–13152, https://doi.org/10.5194/acp-22-13137-2022, https://doi.org/10.5194/acp-22-13137-2022, 2022
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During the 2019 JULIAC campaign, ClNO2 was measured at a rural site in Germany in different seasons. The highest ClNO2 level was 1.6 ppbv in September. ClNO2 production was more sensitive to the availability of NO2 than O3. The average ClNO2 production efficiency was up to 18 % in February and September and down to 3 % in December. These numbers are at the high end of the values reported in the literature, indicating the importance of ClNO2 chemistry in rural environments in midwestern Europe.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Xinping Yang, Keding Lu, Xuefei Ma, Yue Gao, Zhaofeng Tan, Haichao Wang, Xiaorui Chen, Xin Li, Xiaofeng Huang, Lingyan He, Mengxue Tang, Bo Zhu, Shiyi Chen, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 12525–12542, https://doi.org/10.5194/acp-22-12525-2022, https://doi.org/10.5194/acp-22-12525-2022, 2022
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We present the OH and HO2 radical observations at the Shenzhen site (Pearl River Delta, China) in the autumn of 2018. The diurnal maxima were 4.5 × 106 cm−3 for OH and 4.2 × 108 cm−3 for HO2 (including an estimated interference of 23 %–28 % from RO2 radicals during the daytime). The OH underestimation was identified again, and it was attributable to the missing OH sources. HO2 heterogeneous uptake, ROx sources and sinks, and the atmospheric oxidation capacity were evaluated as well.
Ruiqi Man, Zhijun Wu, Taomou Zong, Aristeidis Voliotis, Yanting Qiu, Johannes Größ, Dominik van Pinxteren, Limin Zeng, Hartmut Herrmann, Alfred Wiedensohler, and Min Hu
Atmos. Chem. Phys., 22, 12387–12399, https://doi.org/10.5194/acp-22-12387-2022, https://doi.org/10.5194/acp-22-12387-2022, 2022
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Regional and total deposition doses for different age groups were quantified based on explicit hygroscopicity measurements. We found that particle hygroscopic growth led to a reduction (~24 %) in the total dose. The deposition rate of hygroscopic particles was higher in the daytime, while hydrophobic particles exhibited a higher rate at night and during rush hours. The results will deepen the understanding of the impact of hygroscopicity and the mixing state on deposition patterns in the lungs.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, https://doi.org/10.5194/acp-22-11323-2022, 2022
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The oxidation of limonene, a common volatile emitted by trees and chemical products, by NO3, a nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10-30 compounds. Most of the HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted for a major fraction. Their formation can be explained by chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Karine Sartelet, Youngseob Kim, Florian Couvidat, Maik Merkel, Tuukka Petäjä, Jean Sciare, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 8579–8596, https://doi.org/10.5194/acp-22-8579-2022, https://doi.org/10.5194/acp-22-8579-2022, 2022
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A methodology is defined to estimate number emissions from an inventory providing mass emissions. Number concentrations are simulated over Greater Paris using different nucleation parameterisations (binary, ternary involving sulfuric acid and ammonia, and heteromolecular involving sulfuric acid and extremely low-volatility organics, ELVOCs). The comparisons show that ternary nucleation may not be a dominant process for new particle formation in cities, but they stress the role of ELVOCs.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip T. M. Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 22, 8497–8527, https://doi.org/10.5194/acp-22-8497-2022, https://doi.org/10.5194/acp-22-8497-2022, 2022
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This study investigates the radical chemical budget during the limonene oxidation at different atmospheric-relevant NO concentrations in chamber experiments under atmospheric conditions. It is found that the model–measurement discrepancies of HO2 and RO2 are very large at low NO concentrations that are typical for forested environments. Possible additional processes impacting HO2 and RO2 concentrations are discussed.
Ralf Tillmann, Georgios I. Gkatzelis, Franz Rohrer, Benjamin Winter, Christian Wesolek, Tobias Schuldt, Anne C. Lange, Philipp Franke, Elmar Friese, Michael Decker, Robert Wegener, Morten Hundt, Oleg Aseev, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 15, 3827–3842, https://doi.org/10.5194/amt-15-3827-2022, https://doi.org/10.5194/amt-15-3827-2022, 2022
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We report in situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin in Germany. The low costs of commercial flights provide an affordable and efficient method to improve our understanding of changes in emissions in space and time. The experimental setup expands the capabilities of this platform and provides insights into primary and secondary pollution observations and planetary boundary layer dynamics which determine air quality significantly.
Luka Drinovec, Uroš Jagodič, Luka Pirker, Miha Škarabot, Mario Kurtjak, Kristijan Vidović, Luca Ferrero, Bradley Visser, Jannis Röhrbein, Ernest Weingartner, Daniel M. Kalbermatter, Konstantina Vasilatou, Tobias Bühlmann, Celine Pascale, Thomas Müller, Alfred Wiedensohler, and Griša Močnik
Atmos. Meas. Tech., 15, 3805–3825, https://doi.org/10.5194/amt-15-3805-2022, https://doi.org/10.5194/amt-15-3805-2022, 2022
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A new photothermal interferometer (PTAAM-2λ) for artefact-free determination of the aerosol absorption coefficient at two wavelengths is presented. The instrument is calibrated with NO2 and polydisperse nigrosin, resulting in very low uncertainties of the absorption coefficients: 4 % at 532 nm and 6 % at 1064 nm. The instrument’s performance makes the PTAAM-2λ a strong candidate for reference measurements of the aerosol absorption coefficient.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
Xuefei Ma, Zhaofeng Tan, Keding Lu, Xinping Yang, Xiaorui Chen, Haichao Wang, Shiyi Chen, Xin Fang, Shule Li, Xin Li, Jingwei Liu, Ying Liu, Shengrong Lou, Wanyi Qiu, Hongli Wang, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 7005–7028, https://doi.org/10.5194/acp-22-7005-2022, https://doi.org/10.5194/acp-22-7005-2022, 2022
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This paper presents the first OH and HO2 radical observations made in the Yangtze River Delta in China, and strong oxidation capacity is discovered based on direct measurements. The impacts of new OH regeneration mechanisms, monoterpene oxidation, and HO2 uptake processes are examined and discussed. The sources and the factors to sustain such strong oxidation are the key to understanding the ozone pollution formed in this area.
Ajit Ahlawat, Kay Weinhold, Jesus Marval, Paolo Tronville, Ari Leskinen, Mika Komppula, Holger Gerwig, Lars Gerling, Stephan Weber, Rikke Bramming Jørgensen, Thomas Nørregaard Jensen, Marouane Merizak, Ulrich Vogt, Carla Ribalta, Mar Viana, Andre Schmitz, Maria Chiesa, Giacomo Gerosa, Lothar Keck, Markus Pesch, Gerhard Steiner, Thomas Krinke, Torsten Tritscher, Wolfram Birmili, and Alfred Wiedensohler
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-155, https://doi.org/10.5194/amt-2022-155, 2022
Revised manuscript not accepted
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Measurements of ultrafine particles must be done with quality-assured instruments. The performance of portable instruments such as NanoScan SMPS, and GRIMM Mini WRAS spectrometer measuring the particle number size distribution in the range from 10 to 200 nm were investigated. The influence of different aerosol types and maintenance activities on these instruments were explored. The results show that these portable instruments are suitable for mobile UFP measurements for source identification.
Kristina Glojek, Griša Močnik, Honey Dawn C. Alas, Andrea Cuesta-Mosquera, Luka Drinovec, Asta Gregorič, Matej Ogrin, Kay Weinhold, Irena Ježek, Thomas Müller, Martin Rigler, Maja Remškar, Dominik van Pinxteren, Hartmut Herrmann, Martina Ristorini, Maik Merkel, Miha Markelj, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 5577–5601, https://doi.org/10.5194/acp-22-5577-2022, https://doi.org/10.5194/acp-22-5577-2022, 2022
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A pilot study to determine the emissions of wood burning under
real-world laboratoryconditions was conducted. We found that measured black carbon (eBC) and particulate matter (PM) in rural shallow terrain depressions with residential wood burning could be much greater than predicted by models. The exceeding levels are a cause for concern since similar conditions can be expected in numerous hilly and mountainous regions across Europe, where approximately 20 % of the total population lives.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Michael Weger, Holger Baars, Henriette Gebauer, Maik Merkel, Alfred Wiedensohler, and Bernd Heinold
Geosci. Model Dev., 15, 3315–3345, https://doi.org/10.5194/gmd-15-3315-2022, https://doi.org/10.5194/gmd-15-3315-2022, 2022
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Numerical models are an important tool to assess the air quality in cities,
as they can provide near-continouos data in time and space. In this paper,
air pollution for an entire city is simulated at a high spatial resolution of 40 m.
At this spatial scale, the effects of buildings on the atmosphere,
like channeling or blocking of the air flow, are directly represented by diffuse obstacles in the used model CAIRDIO. For model validation, measurements from air-monitoring sites are used.
Xianda Gong, Heike Wex, Thomas Müller, Silvia Henning, Jens Voigtländer, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 22, 5175–5194, https://doi.org/10.5194/acp-22-5175-2022, https://doi.org/10.5194/acp-22-5175-2022, 2022
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We conducted 10 yr measurements to characterize the atmospheric aerosol at Cabo Verde. An unsupervised machine learning algorithm, K-means, was implemented to study the aerosol types. Cloud condensation nuclei number concentrations during dust periods were 2.5 times higher than marine periods. The long-term data sets, together with the aerosol classification, can be used as a basis to improve understanding of annual cycles of aerosol, and aerosol-cloud interactions in the North Atlantic.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J1 Bloss, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-207, https://doi.org/10.5194/acp-2022-207, 2022
Preprint withdrawn
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We measured radicals (OH, HO2, RO2) and OH reactivity at a UK coastal site and compared our observations to the predictions of an MCMv3.3.1 box model. We find variable agreement between measured and modelled radical concentrations and OH reactivity, where the levels of agreement for individual species display strong dependences on NO concentrations. The most substantial disagreement is found for RO2 at high NO (> 1 ppbv), when RO2 levels are underpredicted by a factor of ~10–30.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Xiaorui Chen, Haichao Wang, and Keding Lu
Atmos. Chem. Phys., 22, 3525–3533, https://doi.org/10.5194/acp-22-3525-2022, https://doi.org/10.5194/acp-22-3525-2022, 2022
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We use a complete set of simulations to evaluate whether equilibrium and steady state are appropriate for a chemical system involving several reactive nitrogen-containing species (NO2, NO3, and N2O5) under various conditions. A previously neglected bias for the coefficient applied for interpreting their effects is disclosed, and the relevant ambient factors are examined. We therefore provide a good solution to an accurate representation of nighttime chemistry in high-aerosol areas.
Chaoyang Xue, Can Ye, Jörg Kleffmann, Chenglong Zhang, Valéry Catoire, Fengxia Bao, Abdelwahid Mellouki, Likun Xue, Jianmin Chen, Keding Lu, Yong Zhao, Hengde Liu, Zhaoxin Guo, and Yujing Mu
Atmos. Chem. Phys., 22, 3149–3167, https://doi.org/10.5194/acp-22-3149-2022, https://doi.org/10.5194/acp-22-3149-2022, 2022
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Summertime measurements of nitrous acid (HONO) and related parameters were conducted at the foot and the summit of Mt. Tai (1534 m above sea level). We proposed a rapid vertical air mass exchange between the foot and the summit level, which enhances the role of HONO in the oxidizing capacity of the upper boundary layer. Kinetics for aerosol-derived HONO sources were constrained. HONO formation from different paths was quantified and discussed.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Chaoyang Xue, Can Ye, Jörg Kleffmann, Wenjin Zhang, Xiaowei He, Pengfei Liu, Chenglong Zhang, Xiaoxi Zhao, Chengtang Liu, Zhuobiao Ma, Junfeng Liu, Jinhe Wang, Keding Lu, Valéry Catoire, Abdelwahid Mellouki, and Yujing Mu
Atmos. Chem. Phys., 22, 1035–1057, https://doi.org/10.5194/acp-22-1035-2022, https://doi.org/10.5194/acp-22-1035-2022, 2022
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Nitrous acid (HONO) and related parameters were measured at the foot and the summit of Mt. Tai in the summer of 2018. Based on measurements at the foot station, we utilized a box model to explore the roles of different sources in the HONO budget. We also studied radical chemistry in this high-ozone region.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Sebastian Düsing, Albert Ansmann, Holger Baars, Joel C. Corbin, Cyrielle Denjean, Martin Gysel-Beer, Thomas Müller, Laurent Poulain, Holger Siebert, Gerald Spindler, Thomas Tuch, Birgit Wehner, and Alfred Wiedensohler
Atmos. Chem. Phys., 21, 16745–16773, https://doi.org/10.5194/acp-21-16745-2021, https://doi.org/10.5194/acp-21-16745-2021, 2021
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The work deals with optical properties of aerosol particles in dried and atmospheric states. Based on two measurement campaigns in the rural background of central Europe, different measurement approaches were compared with each other, such as modeling based on Mie theory and direct in situ or remote sensing measurements. Among others, it was shown that the aerosol extinction-to-backscatter ratio is relative humidity dependent, and refinement with respect to the model input parameters is needed.
Diego Aliaga, Victoria A. Sinclair, Marcos Andrade, Paulo Artaxo, Samara Carbone, Evgeny Kadantsev, Paolo Laj, Alfred Wiedensohler, Radovan Krejci, and Federico Bianchi
Atmos. Chem. Phys., 21, 16453–16477, https://doi.org/10.5194/acp-21-16453-2021, https://doi.org/10.5194/acp-21-16453-2021, 2021
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We investigate the origin of air masses sampled at Mount Chacaltaya, Bolivia. Three-quarters of the measured air has not been influenced by the surface in the previous 4 d. However, it is rare that, at any given time, the sampled air has not been influenced at all by the surface, and often the sampled air has multiple origins. The influence of the surface is more prevalent during day than night. Furthermore, during the 6-month study, one-third of the air masses originated from Amazonia.
Zhaofeng Tan, Luisa Hantschke, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Changmin Cho, Hans-Peter Dorn, Xin Li, Anna Novelli, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 16067–16091, https://doi.org/10.5194/acp-21-16067-2021, https://doi.org/10.5194/acp-21-16067-2021, 2021
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The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR. The chemical structure of myrcene is partly similar to isoprene. Therefore, it can be expected that hydrogen shift reactions could play a role as observed for isoprene. In this work, their potential impact on the regeneration efficiency of hydroxyl radicals is investigated.
Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
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Secondary sulfate aerosols are an important component of fine particles in severe air pollution events. We calculated the sulfate formation rates via a state-of-the-art multiphase model constrained to the observed values. We showed that transition metals in urban aerosols contribute significantly to sulfate formation during haze periods and thus play an important role in mitigation strategies and public health measures in megacities worldwide.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Baseerat Romshoo, Thomas Müller, Sascha Pfeifer, Jorge Saturno, Andreas Nowak, Krzysztof Ciupek, Paul Quincey, and Alfred Wiedensohler
Atmos. Chem. Phys., 21, 12989–13010, https://doi.org/10.5194/acp-21-12989-2021, https://doi.org/10.5194/acp-21-12989-2021, 2021
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Modifications in the optical properties of black carbon (BC) due to ageing are presented and quantified in this study using a state-of-the-art description scheme of BC fractal aggregates. It is shown that the relative change in BC radiative forcing can be larger than 50 % as a function of changing fractal dimension and organic content. A comprehensive parameterization scheme for coated BC optical properties is developed with applications for modelling, ambient, and laboratory-based BC studies.
Helmi Uusitalo, Jenni Kontkanen, Ilona Ylivinkka, Ekaterina Ezhova, Anastasiia Demakova, Mikhail Arshinov, Boris Denisovich Belan, Denis Davydov, Nan Ma, Tuukka Petäjä, Alfred Wiedensohler, Markku Kulmala, and Tuomo Nieminen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-530, https://doi.org/10.5194/acp-2021-530, 2021
Publication in ACP not foreseen
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Characteristics of formation of atmospheric aerosol at four boreal forest sites in Finland and Russian Siberia was analyzed. Our results provide information on the governing processes of atmospheric aerosol formation in the boreal forest area, which a substantial part of the continental biosphere. Aerosol formation was occurring less frequently at Siberian than in Finnish sites, which was affected by the lower particle growth rates and higher loss rates in Siberia.
Junhua Wang, Baozhu Ge, Xueshun Chen, Jie Li, Keding Lu, Yayuan Dong, Lei Kong, Zifa Wang, and Yuanhang Zhang
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-259, https://doi.org/10.5194/gmd-2021-259, 2021
Revised manuscript not accepted
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This paper developed a novel quantitative decoupling analysis (QDA) method to quantify the contributions of emission, meteorology, chemical reaction, and their nonlinear interactions on PM2.5 and applied it to a pollution episode in Beijing. This method can provides the researchers and policy makers with valuable information for understanding of key factors to heavy pollution, but also help the modelers to find out the sources of uncertainties among numerical models.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
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We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Luisa Hantschke, Anna Novelli, Birger Bohn, Changmin Cho, David Reimer, Franz Rohrer, Ralf Tillmann, Marvin Glowania, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 12665–12685, https://doi.org/10.5194/acp-21-12665-2021, https://doi.org/10.5194/acp-21-12665-2021, 2021
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The reactions of Δ3-carene with ozone and the hydroxyl radical (OH) and the photolysis and OH reaction of caronaldehyde were investigated in the simulation chamber SAPHIR. Reaction rate constants of these reactions were determined. Caronaldehyde yields of the ozonolysis and OH reaction were determined. The organic nitrate yield of the reaction of Δ3-carene and caronaldehyde-derived peroxy radicals with NO was determined. The ROx budget (ROx = OH+HO2+RO2) was also investigated.
Dimitrios Bousiotis, Francis D. Pope, David C. S. Beddows, Manuel Dall'Osto, Andreas Massling, Jakob Klenø Nøjgaard, Claus Nordstrøm, Jarkko V. Niemi, Harri Portin, Tuukka Petäjä, Noemi Perez, Andrés Alastuey, Xavier Querol, Giorgos Kouvarakis, Nikos Mihalopoulos, Stergios Vratolis, Konstantinos Eleftheriadis, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Thomas Tuch, and Roy M. Harrison
Atmos. Chem. Phys., 21, 11905–11925, https://doi.org/10.5194/acp-21-11905-2021, https://doi.org/10.5194/acp-21-11905-2021, 2021
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Formation of new particles is a key process in the atmosphere. New particle formation events arising from nucleation of gaseous precursors have been analysed in extensive datasets from 13 sites in five European countries in terms of frequency, nucleation rate, and particle growth rate, with several common features and many differences identified. Although nucleation frequencies are lower at roadside sites, nucleation rates and particle growth rates are typically higher.
Markus Hartmann, Xianda Gong, Simonas Kecorius, Manuela van Pinxteren, Teresa Vogl, André Welti, Heike Wex, Sebastian Zeppenfeld, Hartmut Herrmann, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 21, 11613–11636, https://doi.org/10.5194/acp-21-11613-2021, https://doi.org/10.5194/acp-21-11613-2021, 2021
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Ice-nucleating particles (INPs) are not well characterized in the Arctic despite their importance for the Arctic energy budget. Little is known about their nature (mineral or biological) and sources (terrestrial or marine, long-range transport or local). We find indications that, at the beginning of the melt season, a local, biogenic, probably marine source is likely, but significant enrichment of INPs has to take place from the ocean to the aerosol phase.
Kun Qu, Xuesong Wang, Yu Yan, Jin Shen, Teng Xiao, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 11593–11612, https://doi.org/10.5194/acp-21-11593-2021, https://doi.org/10.5194/acp-21-11593-2021, 2021
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Typhoons above the Northwest Pacific frequently lead to severe ambient ozone pollution in the Pearl River Delta, China, in autumn and summer. However, typhoons do not enhance ozone transport, production and accumulation at the same time, and differences also exist between these influences in two seasons. Through systematic comparisons, we revealed the complex interactions between local meteorology and ozone processes, which is essential for understanding the causes of regional ozone pollution.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
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, https://doi.org/10.5194/acp-21-9995-2021, https://doi.org/10.5194/acp-21-9995-2021, 2021
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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.
Simon Rosanka, Rolf Sander, Andreas Wahner, and Domenico Taraborrelli
Geosci. Model Dev., 14, 4103–4115, https://doi.org/10.5194/gmd-14-4103-2021, https://doi.org/10.5194/gmd-14-4103-2021, 2021
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The Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC) is developed and implemented into the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA). JAMOC is an explicit in-cloud oxidation scheme for oxygenated volatile organic compounds (OVOCs), which is suitable for global model applications. Within a box-model study, we show that JAMOC yields reduced gas-phase concentrations of most OVOCs and oxidants, except for nitrogen oxides.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 9909–9930, https://doi.org/10.5194/acp-21-9909-2021, https://doi.org/10.5194/acp-21-9909-2021, 2021
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In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxygenated volatile organic compound (OVOC) oxygenation. Only rudimentary representations of these processes, if any, are currently available in global atmospheric models. By using a comprehensive atmospheric model that includes a complex in-cloud OVOC oxidation scheme, we show that atmospheric oxidants are reduced and models ignoring this process will underpredict clouds as ozone sinks.
Defeng Zhao, Iida Pullinen, Hendrik Fuchs, Stephanie Schrade, Rongrong Wu, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Yindong Guo, Astrid Kiendler-Scharr, Andreas Wahner, Sungah Kang, Luc Vereecken, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 9681–9704, https://doi.org/10.5194/acp-21-9681-2021, https://doi.org/10.5194/acp-21-9681-2021, 2021
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The reaction of isoprene, a biogenic volatile organic compound with the globally largest emission rates, with NO3, an nighttime oxidant influenced heavily by anthropogenic emissions, forms a large number of highly oxygenated organic molecules (HOM). These HOM are formed via one or multiple oxidation steps, followed by autoxidation. Their total yield is much higher than that in the daytime oxidation of isoprene. They may play an important role in nighttime organic aerosol formation and growth.
Marvin Glowania, Franz Rohrer, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech., 14, 4239–4253, https://doi.org/10.5194/amt-14-4239-2021, https://doi.org/10.5194/amt-14-4239-2021, 2021
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Three instruments that use different techniques to measure gaseous formaldehyde concentrations were compared in experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich. The results demonstrated the need to correct the baseline in measurements by instruments that use the Hantzsch reaction or make use of cavity ring-down spectroscopy. After applying corrections, all three methods gave accurate and precise measurements within their specifications.
Chunmeng Li, Haichao Wang, Xiaorui Chen, Tianyu Zhai, Shiyi Chen, Xin Li, Limin Zeng, and Keding Lu
Atmos. Meas. Tech., 14, 4033–4051, https://doi.org/10.5194/amt-14-4033-2021, https://doi.org/10.5194/amt-14-4033-2021, 2021
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We present a feasible instrument for the measurement of NO2, total peroxy nitrates (PNs, RO2NO2), and total alkyl nitrates (ANs, RONO2) in the atmosphere. The instrument samples sequentially from three channels at different temperature settings and then measures spectra using one cavity-enhanced absorption spectrometer. The concentrations are determined by spectral fitting and corrected using the lookup table method conveniently. The instrument will promote the study of PNs and ANs.
Andrea Cuesta-Mosquera, Griša Močnik, Luka Drinovec, Thomas Müller, Sascha Pfeifer, María Cruz Minguillón, Björn Briel, Paul Buckley, Vadimas Dudoitis, Javier Fernández-García, María Fernández-Amado, Joel Ferreira De Brito, Veronique Riffault, Harald Flentje, Eimear Heffernan, Nikolaos Kalivitis, Athina-Cerise Kalogridis, Hannes Keernik, Luminita Marmureanu, Krista Luoma, Angela Marinoni, Michael Pikridas, Gerhard Schauer, Norbert Serfozo, Henri Servomaa, Gloria Titos, Jesús Yus-Díez, Natalia Zioła, and Alfred Wiedensohler
Atmos. Meas. Tech., 14, 3195–3216, https://doi.org/10.5194/amt-14-3195-2021, https://doi.org/10.5194/amt-14-3195-2021, 2021
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Measurements of black carbon must be conducted with instruments operating in quality-checked and assured conditions to generate reliable and comparable data. Here, 23 Aethalometers monitoring black carbon mass concentrations in European networks were characterized and intercompared. The influence of different aerosol sources, maintenance activities, and the filter material on the instrumental variabilities were investigated. Good agreement and in general low deviations were seen.
Claire E. Reeves, Graham P. Mills, Lisa K. Whalley, W. Joe F. Acton, William J. Bloss, Leigh R. Crilley, Sue Grimmond, Dwayne E. Heard, C. Nicholas Hewitt, James R. Hopkins, Simone Kotthaus, Louisa J. Kramer, Roderic L. Jones, James D. Lee, Yanhui Liu, Bin Ouyang, Eloise Slater, Freya Squires, Xinming Wang, Robert Woodward-Massey, and Chunxiang Ye
Atmos. Chem. Phys., 21, 6315–6330, https://doi.org/10.5194/acp-21-6315-2021, https://doi.org/10.5194/acp-21-6315-2021, 2021
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The impact of isoprene on atmospheric chemistry is dependent on how its oxidation products interact with other pollutants, specifically nitrogen oxides. Such interactions can lead to isoprene nitrates. We made measurements of the concentrations of individual isoprene nitrate isomers in Beijing and used a model to test current understanding of their chemistry. We highlight areas of uncertainty in understanding, in particular the chemistry following oxidation of isoprene by the nitrate radical.
Clara Betancourt, Christoph Küppers, Tammarat Piansawan, Uta Sager, Andrea B. Hoyer, Heinz Kaminski, Gerhard Rapp, Astrid C. John, Miriam Küpper, Ulrich Quass, Thomas Kuhlbusch, Jochen Rudolph, Astrid Kiendler-Scharr, and Iulia Gensch
Atmos. Chem. Phys., 21, 5953–5964, https://doi.org/10.5194/acp-21-5953-2021, https://doi.org/10.5194/acp-21-5953-2021, 2021
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For the first time, we included stable isotopes in the Lagrangian particle dispersion model FLEXPART to investigate firewood home heating aerosol. This is an innovative source apportionment methodology since comparison of stable isotope ratio model predictions with observations delivers quantitative understanding of atmospheric processes. The main outcome of this study is that the home heating aerosol in residential areas was not of remote origin.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775, https://doi.org/10.5194/acp-21-5755-2021, https://doi.org/10.5194/acp-21-5755-2021, 2021
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Pontus von Schoenberg, Peter Tunved, Håkan Grahn, Alfred Wiedensohler, Radovan Krejci, and Niklas Brännström
Atmos. Chem. Phys., 21, 5173–5193, https://doi.org/10.5194/acp-21-5173-2021, https://doi.org/10.5194/acp-21-5173-2021, 2021
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In a radiological emergency preparedness system, Lagrangian particle dispersion models are often used to track the dispersion of radioactive material. In this study we have shown the importance of simulating advanced aerosol dynamic processes that are commonly neglected or simplified in these simulations. We show that inclusion of detailed ambient-aerosol dynamics can play a large role in the model result in simulations adopting a more detailed representation of aerosol–cloud interactions.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Mengdi Song, Xin Li, Suding Yang, Xuena Yu, Songxiu Zhou, Yiming Yang, Shiyi Chen, Huabin Dong, Keren Liao, Qi Chen, Keding Lu, Ningning Zhang, Junji Cao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 4939–4958, https://doi.org/10.5194/acp-21-4939-2021, https://doi.org/10.5194/acp-21-4939-2021, 2021
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Due to their lower diffusion capacities and higher conversion capacities, urban areas in Xi’an experienced severe ozone pollution in the summer. In this study, a campaign of comprehensive field observations and VOC grid sampling was conducted in Xi’an from 20 June to 20 July 2019. We found that Xi'an has a strong local emission source of VOCs, and vehicle exhaust was the primary VOC source. In addition, alkenes, aromatics, and oxygenated VOCs played a dominant role in secondary transformations.
Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 3667–3684, https://doi.org/10.5194/acp-21-3667-2021, https://doi.org/10.5194/acp-21-3667-2021, 2021
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We present results from source apportionment analysis on the carbonaceous aerosol particles, including organic aerosol (OA) and equivalent black carbon (eBC), allowing us to distinguish local emissions from long-range transport for OA and eBC sources. By merging online chemical measurements and considering particle number size distribution, the different air masses reaching the sampling place were described and discussed, based on their respective chemical composition and size distribution.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Changmin Cho, Andreas Hofzumahaus, Hendrik Fuchs, Hans-Peter Dorn, Marvin Glowania, Frank Holland, Franz Rohrer, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 14, 1851–1877, https://doi.org/10.5194/amt-14-1851-2021, https://doi.org/10.5194/amt-14-1851-2021, 2021
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This study describes the implementation and characterization of the chemical modulation reactor (CMR) used in the laser-induced fluorescence instrument of the Forschungszentrum Jülich. The CMR allows for interference-free OH radical measurement in ambient air. During a field campaign in a rural environment, the observed interference was mostly below the detection limit of the instrument and fully explained by the known ozone interference.
Dimitrios Bousiotis, James Brean, Francis D. Pope, Manuel Dall'Osto, Xavier Querol, Andrés Alastuey, Noemi Perez, Tuukka Petäjä, Andreas Massling, Jacob Klenø Nøjgaard, Claus Nordstrøm, Giorgos Kouvarakis, Stergios Vratolis, Konstantinos Eleftheriadis, Jarkko V. Niemi, Harri Portin, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Thomas Tuch, and Roy M. Harrison
Atmos. Chem. Phys., 21, 3345–3370, https://doi.org/10.5194/acp-21-3345-2021, https://doi.org/10.5194/acp-21-3345-2021, 2021
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New particle formation events from 16 sites over Europe have been studied, and the influence of meteorological and atmospheric composition variables has been investigated. Some variables, like solar radiation intensity and temperature, have a positive effect on the occurrence of these events, while others have a negative effect, affecting different aspects such as the rate at which particles are formed or grow. This effect varies depending on the site type and magnitude of these variables.
Nikolaos Evangeliou, Stephen M. Platt, Sabine Eckhardt, Cathrine Lund Myhre, Paolo Laj, Lucas Alados-Arboledas, John Backman, Benjamin T. Brem, Markus Fiebig, Harald Flentje, Angela Marinoni, Marco Pandolfi, Jesus Yus-Dìez, Natalia Prats, Jean P. Putaud, Karine Sellegri, Mar Sorribas, Konstantinos Eleftheriadis, Stergios Vratolis, Alfred Wiedensohler, and Andreas Stohl
Atmos. Chem. Phys., 21, 2675–2692, https://doi.org/10.5194/acp-21-2675-2021, https://doi.org/10.5194/acp-21-2675-2021, 2021
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Following the transmission of SARS-CoV-2 to Europe, social distancing rules were introduced to prevent further spread. We investigate the impacts of the European lockdowns on black carbon (BC) emissions by means of in situ observations and inverse modelling. BC emissions declined by 23 kt in Europe during the lockdowns as compared with previous years and by 11 % as compared to the period prior to lockdowns. Residential combustion prevailed in Eastern Europe, as confirmed by remote sensing data.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Liya Ma, Yujiao Zhu, Mei Zheng, Yele Sun, Lei Huang, Xiaohuan Liu, Yang Gao, Yanjie Shen, Huiwang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 21, 183–200, https://doi.org/10.5194/acp-21-183-2021, https://doi.org/10.5194/acp-21-183-2021, 2021
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In this study, we investigate three patterns of new particles growing to CCN (cloud condensation nuclei) size, i.e., one-stage growth and two-stage growth-A and growth-B patterns. Combining the observations of gaseous pollutants and measured or modeled particulate chemical species, the three growth patterns were discussed regarding the spatial heterogeneity, formation of secondary aerosols, and evaporation of semivolatile particulates as was the survival probability of new particles to CCN size.
Wenjie Wang, David D. Parrish, Xin Li, Min Shao, Ying Liu, Ziwei Mo, Sihua Lu, Min Hu, Xin Fang, Yusheng Wu, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15617–15633, https://doi.org/10.5194/acp-20-15617-2020, https://doi.org/10.5194/acp-20-15617-2020, 2020
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During the past decade, China has devoted very substantial resources to improving the environment. These efforts have improved atmospheric particulate matter loading, but ambient ozone levels have continued to increase. In this paper we investigate the causes of the increasing ozone concentrations through analysis of a data set that is, to our knowledge, unique: a 12-year data set including ground-level O3, NOx, and VOC precursors collected at an urban site in Beijing.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Michael Rolletter, Marion Blocquet, Martin Kaminski, Birger Bohn, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Xin Li, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 13701–13719, https://doi.org/10.5194/acp-20-13701-2020, https://doi.org/10.5194/acp-20-13701-2020, 2020
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The photooxidation of pinonaldehyde is investigated in a chamber study under natural sunlight and low NO conditions with and without an added hydroxyl radical (OH) scavenger. The experimentally determined pinonaldehyde photolysis frequency is faster by a factor of 3.5 than currently used parameterizations in atmospheric models. Yields of degradation products are measured in the presence and absence of OH. Measurements are compared to current atmospheric models and a theory-based mechanism.
Yangang Ren, Bastian Stieger, Gerald Spindler, Benoit Grosselin, Abdelwahid Mellouki, Thomas Tuch, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 13069–13089, https://doi.org/10.5194/acp-20-13069-2020, https://doi.org/10.5194/acp-20-13069-2020, 2020
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We present HONO measurements from the TROPOS research site in Melpitz, Germany. Investigations of HONO sources and sinks revealed the nighttime formation by heterogeneous conversion of NO2 to HONO followed by a significant surface deposition at night. The evaporation of dew was identified as the main HONO source in the morning. In the following, dew measurements with a self-made dew collector were performed to estimate the amount of evaporated HONO from dew in the atmospheric HONO distribution.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284, https://doi.org/10.5194/acp-20-12265-2020, https://doi.org/10.5194/acp-20-12265-2020, 2020
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
Ting Lei, Nan Ma, Juan Hong, Thomas Tuch, Xin Wang, Zhibin Wang, Mira Pöhlker, Maofa Ge, Weigang Wang, Eugene Mikhailov, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Alfred Wiedensohler, and Yafang Cheng
Atmos. Meas. Tech., 13, 5551–5567, https://doi.org/10.5194/amt-13-5551-2020, https://doi.org/10.5194/amt-13-5551-2020, 2020
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We present the design of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. We further introduce comprehensive methods for system calibration and validation of the performance of the system. We then study the size dependence of the deliquescence and the efflorescence of aerosol nanoparticles for sizes down to 6 nm.
Jost Heintzenberg, Wolfram Birmili, Bryan Hellack, Gerald Spindler, Thomas Tuch, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 10967–10984, https://doi.org/10.5194/acp-20-10967-2020, https://doi.org/10.5194/acp-20-10967-2020, 2020
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A total of 10 years of hourly aerosol and gas data at four rural German stations have been combined with hourly back trajectories to the stations and inventories of the European Emissions Database for Global Atmospheric Research (EDGAR), yielding emission maps and trends over Germany for PM10, particle number concentrations, and equivalent black carbon (eBC). The maps reflect aerosol emissions modified with atmospheric processes during transport between sources and receptor sites.
Laurent Poulain, Gerald Spindler, Achim Grüner, Thomas Tuch, Bastian Stieger, Dominik van Pinxteren, Jean-Eudes Petit, Olivier Favez, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Meas. Tech., 13, 4973–4994, https://doi.org/10.5194/amt-13-4973-2020, https://doi.org/10.5194/amt-13-4973-2020, 2020
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The stability and the comparability between ACSM and collocated filter sampling and MPSS measurements was investigated in order to examine the instruments robustness for year-long measurements. Specific attention was paid to the influence of the upper size cutoff diameter to better understand how it might affect the data validation. Recommendations are provided for better on-site quality assurance and quality control of the ACSM, which would be useful for either long-term or intensive campaigns.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
Yang Chen, Jing Cai, Zhichao Wang, Chao Peng, Xiaojiang Yao, Mi Tian, Yiqun Han, Guangming Shi, Zongbo Shi, Yue Liu, Xi Yang, Mei Zheng, Tong Zhu, Kebin He, Qiang Zhang, and Fumo Yang
Atmos. Chem. Phys., 20, 9231–9247, https://doi.org/10.5194/acp-20-9231-2020, https://doi.org/10.5194/acp-20-9231-2020, 2020
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Patterns of particle transport, accumulation, and evolution in both urban and rural areas of Beijing are investigated. The two sites shared 17 common particle types in different stages of atmospheric processing.
Yang Chen, Guangming Shi, Jing Cai, Zongbo Shi, Zhichao Wang, Xiaojiang Yao, Mi Tian, Chao Peng, Yiqun Han, Tong Zhu, Yue Liu, Xi Yang, Mei Zheng, Fumo Yang, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 20, 9249–9263, https://doi.org/10.5194/acp-20-9249-2020, https://doi.org/10.5194/acp-20-9249-2020, 2020
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Individual particles were observed in two field studies during winter 2016 in the urban and rural areas of Beijing. An online single-particle chemical composition analysis was used as a tracing system to investigate the impact of heating activities and the formation of haze events. During the pollution events, a pattern of transport and accumulation was found with evidence of single particles. The transport from Pinggu to Peking University was significant but PKU to PG occurred occasionally.
Martine Collaud Coen, Elisabeth Andrews, Andrés Alastuey, Todor Petkov Arsov, John Backman, Benjamin T. Brem, Nicolas Bukowiecki, Cédric Couret, Konstantinos Eleftheriadis, Harald Flentje, Markus Fiebig, Martin Gysel-Beer, Jenny L. Hand, András Hoffer, Rakesh Hooda, Christoph Hueglin, Warren Joubert, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Casper Labuschagne, Neng-Huei Lin, Yong Lin, Cathrine Lund Myhre, Krista Luoma, Hassan Lyamani, Angela Marinoni, Olga L. Mayol-Bracero, Nikos Mihalopoulos, Marco Pandolfi, Natalia Prats, Anthony J. Prenni, Jean-Philippe Putaud, Ludwig Ries, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Patrick Sheridan, James Patrick Sherman, Junying Sun, Gloria Titos, Elvis Torres, Thomas Tuch, Rolf Weller, Alfred Wiedensohler, Paul Zieger, and Paolo Laj
Atmos. Chem. Phys., 20, 8867–8908, https://doi.org/10.5194/acp-20-8867-2020, https://doi.org/10.5194/acp-20-8867-2020, 2020
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Long-term trends of aerosol radiative properties (52 stations) prove that aerosol load has significantly decreased over the last 20 years. Scattering trends are negative in Europe (EU) and North America (NA), not ss in Asia, and show a mix of positive and negative trends at polar stations. Absorption has mainly negative trends. The single scattering albedo has positive trends in Asia and eastern EU and negative in western EU and NA, leading to a global positive median trend of 0.02 % per year.
Andreas Petzold, Patrick Neis, Mihal Rütimann, Susanne Rohs, Florian Berkes, Herman G. J. Smit, Martina Krämer, Nicole Spelten, Peter Spichtinger, Philippe Nédélec, and Andreas Wahner
Atmos. Chem. Phys., 20, 8157–8179, https://doi.org/10.5194/acp-20-8157-2020, https://doi.org/10.5194/acp-20-8157-2020, 2020
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The first analysis of 15 years of global-scale water vapour and relative humidity observations by passenger aircraft in the MOZAIC and IAGOS programmes resolves detailed features of water vapour and ice-supersaturated air in the mid-latitude tropopause. Key results provide in-depth insight into seasonal and regional variability and chemical signatures of ice-supersaturated air masses, including trend analyses, and show a close link to cirrus clouds and their highly important effects on climate.
Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di Liu, Zongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 20, 7531–7552, https://doi.org/10.5194/acp-20-7531-2020, https://doi.org/10.5194/acp-20-7531-2020, 2020
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Using the chemical composition of offline filter samples, we report that a large share of oxidized organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates showed a strong correlation with the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate in heterogeneous reactions and further demonstrates that iSOA formation is controlled by anthropogenic emissions.
Jingyi Li, Haowen Zhang, Qi Ying, Zhijun Wu, Yanli Zhang, Xinming Wang, Xinghua Li, Yele Sun, Min Hu, Yuanhang Zhang, and Jianlin Hu
Atmos. Chem. Phys., 20, 7291–7306, https://doi.org/10.5194/acp-20-7291-2020, https://doi.org/10.5194/acp-20-7291-2020, 2020
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Large gaps still exist in modeled and observed secondary organic aerosol (SOA) mass loading and properties. Here we investigated the impacts of water partitioning into organic aerosol and nonideality of the organic–water mixture on SOA over eastern China using a regional 3D model. SOA is increased more significantly in humid and hot environments. Increases in SOA further cause an enhancement of the cooling effects of aerosols. It is crucial to consider the above processes in modeling SOA.
Jia Sun, Wolfram Birmili, Markus Hermann, Thomas Tuch, Kay Weinhold, Maik Merkel, Fabian Rasch, Thomas Müller, Alexander Schladitz, Susanne Bastian, Gunter Löschau, Josef Cyrys, Jianwei Gu, Harald Flentje, Björn Briel, Christoph Asbach, Heinz Kaminski, Ludwig Ries, Ralf Sohmer, Holger Gerwig, Klaus Wirtz, Frank Meinhardt, Andreas Schwerin, Olaf Bath, Nan Ma, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 7049–7068, https://doi.org/10.5194/acp-20-7049-2020, https://doi.org/10.5194/acp-20-7049-2020, 2020
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To evaluate the effectiveness of emission mitigation policies, we evaluated the trends of the size-resolved particle number concentrations and equivalent black carbon mass concentration at 16 observational sites for various environments in Germany (2009–2018). Overall, significant decrease trends are found for most of the parameters and sites. This study suggests that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales such as in Germany.
Robert Woodward-Massey, Eloise J. Slater, Jake Alen, Trevor Ingham, Danny R. Cryer, Leanne M. Stimpson, Chunxiang Ye, Paul W. Seakins, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Meas. Tech., 13, 3119–3146, https://doi.org/10.5194/amt-13-3119-2020, https://doi.org/10.5194/amt-13-3119-2020, 2020
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The OH radical is known as nature’s detergent, removing most trace gases from the atmosphere. Hence, an accurate measurement of its concentration is very important. We present measurements of OH in several field locations using a laser-based fluorescence method equipped with an OH scavenger. By determining the background signal in two different ways, we show that the instrument does not suffer any significant interferences that could result in an overestimation of OH concentrations.
Lavinia Onel, Alexander Brennan, Michele Gianella, James Hooper, Nicole Ng, Gus Hancock, Lisa Whalley, Paul W. Seakins, Grant A. D. Ritchie, and Dwayne E. Heard
Atmos. Meas. Tech., 13, 2441–2456, https://doi.org/10.5194/amt-13-2441-2020, https://doi.org/10.5194/amt-13-2441-2020, 2020
Sascha Pfeifer, Thomas Müller, Andrew Freedman, and Alfred Wiedensohler
Atmos. Meas. Tech., 13, 2161–2167, https://doi.org/10.5194/amt-13-2161-2020, https://doi.org/10.5194/amt-13-2161-2020, 2020
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The effect of the baseline drift on the resulting extinction values of three CAPS PMex monitors with different wavelengths was analysed for an urban background station. A significant baseline drift was observed, which leads to characteristic measurement artefacts for particle extinction. Two alternative methods for recalculating the baseline are shown. With these methods the extinction artefacts are diminished and the effective scattering of the resulting extinction values is reduced.
Chuan Yu, Zhe Wang, Men Xia, Xiao Fu, Weihao Wang, Yee Jun Tham, Tianshu Chen, Penggang Zheng, Hongyong Li, Ye Shan, Xinfeng Wang, Likun Xue, Yan Zhou, Dingli Yue, Yubo Ou, Jian Gao, Keding Lu, Steven S. Brown, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 20, 4367–4378, https://doi.org/10.5194/acp-20-4367-2020, https://doi.org/10.5194/acp-20-4367-2020, 2020
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This study provides a holistic picture of N2O5 heterogeneous uptake on ambient aerosols and the influencing factors under various climatic and chemical conditions in China, and it proposes an observation-based empirical parameterization. The empirical parameterization can be used in air quality models to improve the prediction of PM2.5 and photochemical pollution in China and similar polluted regions of the world.
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
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Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
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, https://doi.org/10.5194/acp-20-2161-2020, https://doi.org/10.5194/acp-20-2161-2020, 2020
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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.
Marco Paglione, Stefania Gilardoni, Matteo Rinaldi, Stefano Decesari, Nicola Zanca, Silvia Sandrini, Lara Giulianelli, Dimitri Bacco, Silvia Ferrari, Vanes Poluzzi, Fabiana Scotto, Arianna Trentini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Francesco Canonaco, André S. H. Prévôt, Paola Massoli, Claudio Carbone, Maria Cristina Facchini, and Sandro Fuzzi
Atmos. Chem. Phys., 20, 1233–1254, https://doi.org/10.5194/acp-20-1233-2020, https://doi.org/10.5194/acp-20-1233-2020, 2020
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Our multi-year observational study regarding organic aerosol (OA) in the Po Valley indicates that more than half of OA is of secondary origin (SOA) through all the year and at both urban and rural sites. Within the SOA, the measurements show the importance of biomass burning (BB) aging products during cold seasons and indicate aqueous-phase processing of BB emissions as a fundamental driver of SOA formation in wintertime, with important consequences for air quality policy at the global level.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Aurélien Chauvigné, Diego Aliaga, Karine Sellegri, Nadège Montoux, Radovan Krejci, Griša Močnik, Isabel Moreno, Thomas Müller, Marco Pandolfi, Fernando Velarde, Kay Weinhold, Patrick Ginot, Alfred Wiedensohler, Marcos Andrade, and Paolo Laj
Atmos. Chem. Phys., 19, 14805–14824, https://doi.org/10.5194/acp-19-14805-2019, https://doi.org/10.5194/acp-19-14805-2019, 2019
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The study presents for the first time the analysis of aerosol optical properties at the unique high-altitude station of Chacaltaya, Bolivia. Ideally located, the station allows us to better understand influences of urban areas and the Amazon Forest on tropospheric properties. An emerging method is applied to characterize aerosol origins and permits us to illustrate evidence of natural and anthropogenic influences.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Simonas Kecorius, Teresa Vogl, Pauli Paasonen, Janne Lampilahti, Daniel Rothenberg, Heike Wex, Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Silvia Henning, Xianda Gong, Andre Welti, Markku Kulmala, Frank Stratmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 19, 14339–14364, https://doi.org/10.5194/acp-19-14339-2019, https://doi.org/10.5194/acp-19-14339-2019, 2019
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Arctic sea-ice retreat, atmospheric new particle formation (NPF), and aerosol–cloud interaction may all be linked via a positive feedback mechanism. Understanding the sources of cloud condensation nuclei (CCN) is an important piece in the Arctic amplification puzzle. We show that Arctic newly formed particles do not have to grow beyond the Aitken mode to act as CCN. This is important, because NPF occurrence in the Arctic is expected to increase, making it a significant contributor to CCN budget.
Min Cui, Cheng Li, Yingjun Chen, Fan Zhang, Jun Li, Bin Jiang, Yangzhi Mo, Jia Li, Caiqing Yan, Mei Zheng, Zhiyong Xie, Gan Zhang, and Junyu Zheng
Atmos. Chem. Phys., 19, 13945–13956, https://doi.org/10.5194/acp-19-13945-2019, https://doi.org/10.5194/acp-19-13945-2019, 2019
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Refined source apportionment is urgently needed but hard to achieve due to a lack of specific biomarkers. Recently, Fourier transform ion cyclotron resonance mass spectrometry has been used to analyse the probable chemical structure of polar organic matter emitted from off-road engines. We found more condensed aromatic rings in S-containing compounds for HFO-fueled vessels, while more abundant aliphatic chains were observed in emissions from diesel equipment.
Sebastian Düsing, Birgit Wehner, Thomas Müller, Almond Stöcker, and Alfred Wiedensohler
Atmos. Meas. Tech., 12, 5879–5895, https://doi.org/10.5194/amt-12-5879-2019, https://doi.org/10.5194/amt-12-5879-2019, 2019
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This study examines the effect of changes in relative humidity on measurements made by two different filter-based absorption photometers. Different filter loads, loading materials, and filter types are considered. It was found that both instruments react opposingly and with different magnitudes. One of the devices showed a variation in the dependence on the loading material. For each of the two devices, a correction approach is provided. Recommendations based on the findings are given.
Michael Rolletter, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 19, 11635–11649, https://doi.org/10.5194/acp-19-11635-2019, https://doi.org/10.5194/acp-19-11635-2019, 2019
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Here we present a study of the photooxidation of alpha-pinene, the most abundant monoterpene, by hydroxyl radicals (OH) conducted in the simulation chamber SAPHIR under low NOx and atmospheric alpha-pinene concentrations. Yields of the main degradation products acetone, formaldehyde, and pinonaldehyde were determined and the HOx (OH + HO2) radical budget was investigated. Measurements were used to test current atmospheric models and a theory-based mechanism.
Honey Dawn C. Alas, Kay Weinhold, Francesca Costabile, Antonio Di Ianni, Thomas Müller, Sascha Pfeifer, Luca Di Liberto, Jay R. Turner, and Alfred Wiedensohler
Atmos. Meas. Tech., 12, 4697–4712, https://doi.org/10.5194/amt-12-4697-2019, https://doi.org/10.5194/amt-12-4697-2019, 2019
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Traffic-related air pollutants are highly variable in space. To determine their spatial distribution in relation to human exposure, portable black carbon and PM2.5 mass concentration sensors aboard mobile platforms can be used. High-spatial-resolution data can help improve exposure estimates. The quality of these data becomes increasingly important. This study provides a detailed methodology on how to achieve highly quality assured data from the abovementioned mobile measurements.
Xianda Gong, Heike Wex, Thomas Müller, Alfred Wiedensohler, Kristina Höhler, Konrad Kandler, Nan Ma, Barbara Dietel, Thea Schiebel, Ottmar Möhler, and Frank Stratmann
Atmos. Chem. Phys., 19, 10883–10900, https://doi.org/10.5194/acp-19-10883-2019, https://doi.org/10.5194/acp-19-10883-2019, 2019
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For the diverse aerosol on Cyprus, we found the following: new particle formation can be a source of cloud condensation nuclei. Particle hygroscopicity showed that particles ~<100 nm contained mostly organic material, while larger ones were more hygroscopic. Two separate methods obtained similar concentrations of ice-nucleating particles (INP), with mostly no evidence of a local origin. Different parameterizations overestimated INP concentration in this rather polluted region.
Jingwei Liu, Xin Li, Yiming Yang, Haichao Wang, Yusheng Wu, Xuewei Lu, Mindong Chen, Jianlin Hu, Xiaobo Fan, Limin Zeng, and Yuanhang Zhang
Atmos. Meas. Tech., 12, 4439–4453, https://doi.org/10.5194/amt-12-4439-2019, https://doi.org/10.5194/amt-12-4439-2019, 2019
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Incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) has been proven to be a reliable method for measuring glyoxal and methylglyoxal in the atmosphere. However, the commonly overlying strong spectral absorption of nitrogen dioxide hampers the accurate and sensitive resolve of the weak absorption features of glyoxal and methylglyoxal. Here, we report a custom-built IBBCEAS system that could overcome this problem by quantitatively removing nitrogen dioxide from the sample air.
Michael Hollaway, Oliver Wild, Ting Yang, Yele Sun, Weiqi Xu, Conghui Xie, Lisa Whalley, Eloise Slater, Dwayne Heard, and Dantong Liu
Atmos. Chem. Phys., 19, 9699–9714, https://doi.org/10.5194/acp-19-9699-2019, https://doi.org/10.5194/acp-19-9699-2019, 2019
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This study, for the first time, uses combinations of aerosol and lidar data to drive an offline photolysis scheme. Absorbing species are shown to have the greatest impact on photolysis rate constants in the winter and scattering aerosol are shown to dominate responses in the summer. During haze episodes, aerosols are shown to produce a greater impact than cloud cover. The findings demonstrate the potential photochemical impacts of haze pollution in a highly polluted urban environment.
Run Liu, Lu Mao, Shaw Chen Liu, Yuanhang Zhang, Hong Liao, Huopo Chen, and Yuhang Wang
Atmos. Chem. Phys., 19, 8563–8568, https://doi.org/10.5194/acp-19-8563-2019, https://doi.org/10.5194/acp-19-8563-2019, 2019
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The recent paper by Shen et al. (2018; referred to hereafter as SHEN) made a sweeping statement on the winter haze pollution in Beijing by claiming an
Insignificant effect of climate change on winter haze in Beijing. We argue that the paper contains three serious flaws. Any one of the three flaws can nullify the claim of SHEN.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Zhaofeng Tan, Keding Lu, Andreas Hofzumahaus, Hendrik Fuchs, Birger Bohn, Frank Holland, Yuhan Liu, Franz Rohrer, Min Shao, Kang Sun, Yusheng Wu, Limin Zeng, Yinsong Zhang, Qi Zou, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 7129–7150, https://doi.org/10.5194/acp-19-7129-2019, https://doi.org/10.5194/acp-19-7129-2019, 2019
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Atmospheric OH, HO2, and RO2 radicals; OH reactivity; and trace gases measured in the Pearl River Delta in autumn 2014 are used for radical budget analyses. The RO2 budget suggests that unexplained OH reactivity is due to unmeasured volatile organic compounds. The OH budget points to a missing OH source and that of RO2 to a missing RO2 sink at low NO. This could indicate a common, unknown process that converts RO2 to OH without the involvement of NO, which would reduce ozone production by 30 %.
Yue Liu, Mei Zheng, Mingyuan Yu, Xuhui Cai, Huiyun Du, Jie Li, Tian Zhou, Caiqing Yan, Xuesong Wang, Zongbo Shi, Roy M. Harrison, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 19, 6595–6609, https://doi.org/10.5194/acp-19-6595-2019, https://doi.org/10.5194/acp-19-6595-2019, 2019
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This study is part of the UK–China APHH campaign. To identify both source types and source regions at the same time, this study developed a combined method including receptor model, footprint model, and air quality model for the first time to investigate sources of PM2.5 during haze episodes in Beijing. It is an expansion of the application of the receptor model and is helpful for formulating effective control strategies to improve air quality in this region.
Zhenying Xu, Mingxu Liu, Minsi Zhang, Yu Song, Shuxiao Wang, Lin Zhang, Tingting Xu, Tiantian Wang, Caiqing Yan, Tian Zhou, Yele Sun, Yuepeng Pan, Min Hu, Mei Zheng, and Tong Zhu
Atmos. Chem. Phys., 19, 5605–5613, https://doi.org/10.5194/acp-19-5605-2019, https://doi.org/10.5194/acp-19-5605-2019, 2019
Zhaofeng Tan, Keding Lu, Meiqing Jiang, Rong Su, Hongli Wang, Shengrong Lou, Qingyan Fu, Chongzhi Zhai, Qinwen Tan, Dingli Yue, Duohong Chen, Zhanshan Wang, Shaodong Xie, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 3493–3513, https://doi.org/10.5194/acp-19-3493-2019, https://doi.org/10.5194/acp-19-3493-2019, 2019
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We evaluated the atmospheric oxidation capacity (AOC) in four Chinese megacities during photochemically polluted seasons. The chemical production of ozone and particle nitrate was diagnosed through a box model, which can be attributed to daytime radical chemistry. Our work highlights that the formation of both ozone and fine particles is largely driven by the atmospheric radical chemistry in China. Consequently, we suggest future pollution mitigation strategies should consider the role of AOC.
Sascha R. Albrecht, Anna Novelli, Andreas Hofzumahaus, Sungah Kang, Yare Baker, Thomas Mentel, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech., 12, 891–902, https://doi.org/10.5194/amt-12-891-2019, https://doi.org/10.5194/amt-12-891-2019, 2019
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Within this study we demonstrate reliable measurement of hydroperoxy (HO2) radicals via chemical ionisation mass spectrometry. HO2 is detected as an ion cluster with bromide ions, which allows a selective detection. This direct and sensitive measurement provides reliable data of HO2 radical concentrations in the atmosphere as demonstrated in the first application in simulation chamber experiments.
Shan Huang, Zhijun Wu, Laurent Poulain, Manuela van Pinxteren, Maik Merkel, Denise Assmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 18, 18043–18062, https://doi.org/10.5194/acp-18-18043-2018, https://doi.org/10.5194/acp-18-18043-2018, 2018
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The Atlantic aerosols are characterized based on high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements during four open-ocean cruises. This unique data set provides the latitudinal distribution of source contributions of organic aerosols (OAs) over the Atlantic Ocean, showing that marine sources could control the OA formation over the South Atlantic, while strong continental influence was found near Africa and Europe.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
Daocheng Gong, Hao Wang, Shenyang Zhang, Yu Wang, Shaw Chen Liu, Hai Guo, Min Shao, Congrong He, Duohong Chen, Lingyan He, Lei Zhou, Lidia Morawska, Yuanhang Zhang, and Boguang Wang
Atmos. Chem. Phys., 18, 14417–14432, https://doi.org/10.5194/acp-18-14417-2018, https://doi.org/10.5194/acp-18-14417-2018, 2018
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The complex air pollution in the air-polluted Pearl River Delta (PRD) region in southern China has significantly elevated the background atmospheric oxidative capacity of the adjacent forests and subsequently lowered the levels of important biogenic volatile organic compounds, such as isoprene, which probably affect the regional air quality and ecological environment in the long term.
Yee Jun Tham, Zhe Wang, Qinyi Li, Weihao Wang, Xinfeng Wang, Keding Lu, Nan Ma, Chao Yan, Simonas Kecorius, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 18, 13155–13171, https://doi.org/10.5194/acp-18-13155-2018, https://doi.org/10.5194/acp-18-13155-2018, 2018
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This study addresses the limited understanding of heterogeneous N2O5 uptake and ClNO2 production in the polluted environment of China. The results showed that N2O5 uptake and ClNO2 yield cannot be well explained by previous parameterizations and were largely influenced by factors like aerosol water content and biomass burning emission. Our findings illuminate the need to realistically parameterize these heterogeneous processes for better simulation of photochemical and haze pollution in China.
Michael Le Breton, Åsa M. Hallquist, Ravi Kant Pathak, David Simpson, Yujue Wang, John Johansson, Jing Zheng, Yudong Yang, Dongjie Shang, Haichao Wang, Qianyun Liu, Chak Chan, Tao Wang, Thomas J. Bannan, Michael Priestley, Carl J. Percival, Dudley E. Shallcross, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 13013–13030, https://doi.org/10.5194/acp-18-13013-2018, https://doi.org/10.5194/acp-18-13013-2018, 2018
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We apply state-of-the-art chemical characterization to determine the chloride radical production in Beijing via measurement of inorganic halogens at a semi-rural site. The high concentration of inorganic halogens, namely nitryl chloride, enables the production of chlorinated volatile organic compounds which are measured in both the gas and particle phases simultaneously. This enables the secondary production of aerosols via chlorine oxidation to be directly observed in ambient air.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Zhaofeng Tan, Franz Rohrer, Keding Lu, Xuefei Ma, Birger Bohn, Sebastian Broch, Huabin Dong, Hendrik Fuchs, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Yuhan Liu, Anna Novelli, Min Shao, Haichao Wang, Yusheng Wu, Limin Zeng, Min Hu, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 12391–12411, https://doi.org/10.5194/acp-18-12391-2018, https://doi.org/10.5194/acp-18-12391-2018, 2018
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We present the first wintertime OH, HO2, and RO2 measurements in Beijing, China. OH concentrations are nearly 2-fold larger than those observed in foreign cities during wintertime. The high OH and large OH reactivities indicate photochemical processes can be effective even during wintertime. A box model largely underestimated HO2 and RO2 concentrations during pollution episodes correlated with high NOx, indicating a deficit current chemistry in the high NOx regime.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Xiao-Feng Huang, Bei-Bing Zou, Ling-Yan He, Min Hu, André S. H. Prévôt, and Yuan-Hang Zhang
Atmos. Chem. Phys., 18, 11563–11580, https://doi.org/10.5194/acp-18-11563-2018, https://doi.org/10.5194/acp-18-11563-2018, 2018
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A novel multilinear engine (ME-2) model was applied to the PM2.5 dataset observed in the Pearl River Delta (PRD) of China in 2015 and identified the sources of secondary sulfate (21 %), vehicle emissions (14 %), industrial emissions (13 %), secondary nitrate (11 %), biomass burning (11 %), secondary organic aerosol (7 %), coal burning (6 %), fugitive dust (5 %), ship emissions (3 %) and aged sea salt (2 %). The central PRD area was clearly identified as the key emission area in the PRD.
Anna Novelli, Martin Kaminski, Michael Rolletter, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Frank Holland, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 18, 11409–11422, https://doi.org/10.5194/acp-18-11409-2018, https://doi.org/10.5194/acp-18-11409-2018, 2018
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The impact of photooxidation of 2-methyl-3-butene-2-ol (MBO) on the concentration of radical species was studied in the atmospheric simulation chamber SAPHIR. MBO is a volatile organic compound mainly emitted by ponderosa and lodgepole pines which are very abundant in forests in the central-west USA. A very good agreement between measured and modelled radical concentrations and products from the oxidation of MBO was observed in an environment with NO of ~ 200 pptv.
Jun Duan, Min Qin, Bin Ouyang, Wu Fang, Xin Li, Keding Lu, Ke Tang, Shuaixi Liang, Fanhao Meng, Zhaokun Hu, Pinhua Xie, Wenqing Liu, and Rolf Häsler
Atmos. Meas. Tech., 11, 4531–4543, https://doi.org/10.5194/amt-11-4531-2018, https://doi.org/10.5194/amt-11-4531-2018, 2018
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We report a custom-built instrument for simultaneous unambiguous measurements of HONO and NO2 based on incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS). The current IBBCEAS instrument has made significant improvements in terms of efficient sampling as well as resistance against vibration; temperature change and the measurement precisions (2σ) for HONO are about 180 and 340 ppt in 30 s, respectively. The field inter-comparison and the mobile measurements are present.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Angela Benedetti, Jeffrey S. Reid, Peter Knippertz, John H. Marsham, Francesca Di Giuseppe, Samuel Rémy, Sara Basart, Olivier Boucher, Ian M. Brooks, Laurent Menut, Lucia Mona, Paolo Laj, Gelsomina Pappalardo, Alfred Wiedensohler, Alexander Baklanov, Malcolm Brooks, Peter R. Colarco, Emilio Cuevas, Arlindo da Silva, Jeronimo Escribano, Johannes Flemming, Nicolas Huneeus, Oriol Jorba, Stelios Kazadzis, Stefan Kinne, Thomas Popp, Patricia K. Quinn, Thomas T. Sekiyama, Taichu Tanaka, and Enric Terradellas
Atmos. Chem. Phys., 18, 10615–10643, https://doi.org/10.5194/acp-18-10615-2018, https://doi.org/10.5194/acp-18-10615-2018, 2018
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Numerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation authorities, solar energy plant managers, climate service providers, and health professionals. This paper describes the advances in the field and sets out requirements for observations for the sustainability of these activities.
Haichao Wang, Keding Lu, Xiaorui Chen, Qindan Zhu, Zhijun Wu, Yusheng Wu, and Kang Sun
Atmos. Chem. Phys., 18, 10483–10495, https://doi.org/10.5194/acp-18-10483-2018, https://doi.org/10.5194/acp-18-10483-2018, 2018
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The vertical measurement of NOx and O3 was carried out on a movable carriage on a tower during a winter heavy-haze episode in urban Beijing, China. We found that pNO3- formation via N2O5 uptake was significant at high altitudes (e.g., > 150 m), which was supported by the lower total oxidant
(NO2 + O3) level at high altitudes than at ground level. This study highlights the fact that pNO3- formation via N2O5 uptake may be an important source of pNO3- in the urban airshed during wintertime.
Michael Le Breton, Yujue Wang, Åsa M. Hallquist, Ravi Kant Pathak, Jing Zheng, Yudong Yang, Dongjie Shang, Marianne Glasius, Thomas J. Bannan, Qianyun Liu, Chak K. Chan, Carl J. Percival, Wenfei Zhu, Shengrong Lou, David Topping, Yuchen Wang, Jianzhen Yu, Keding Lu, Song Guo, Min Hu, and Mattias Hallquist
Atmos. Chem. Phys., 18, 10355–10371, https://doi.org/10.5194/acp-18-10355-2018, https://doi.org/10.5194/acp-18-10355-2018, 2018
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This paper utilizes a chemical ionisation mass spectrometer measuring gas and particle-phase organosulfates (OS) simultaneously during a field campaign in Beijing, China, and highlights how high time frequency online measurements enable a detailed analysis of dominant production mechanisms. We find that high aerosol acidity, organic precursor concentration and relative humidity promote the production of OS. The thermogram desorption reveals the potential for semi-volatile gas-phase OS.
Haichao Wang, Keding Lu, Song Guo, Zhijun Wu, Dongjie Shang, Zhaofeng Tan, Yujue Wang, Michael Le Breton, Shengrong Lou, Mingjin Tang, Yusheng Wu, Wenfei Zhu, Jing Zheng, Limin Zeng, Mattias Hallquist, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 9705–9721, https://doi.org/10.5194/acp-18-9705-2018, https://doi.org/10.5194/acp-18-9705-2018, 2018
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N2O5, ClNO2, and particulate nitrate were measured simultaneously in Beijing, China, in 2016. The elevated N2O5 uptake coefficient and ClNO2 yield were determined, which suggest fast N2O5 uptake in Beijing. We highlight that the NO3 oxidation in nocturnal VOC degradation is efficient, with fast formation of organic nitrates. More studies are needed to investigate NO3–N2O5 chemistry and its contribution to secondary organic aerosol formation.
Florian Berkes, Norbert Houben, Ulrich Bundke, Harald Franke, Hans-Werner Pätz, Franz Rohrer, Andreas Wahner, and Andreas Petzold
Atmos. Meas. Tech., 11, 3737–3757, https://doi.org/10.5194/amt-11-3737-2018, https://doi.org/10.5194/amt-11-3737-2018, 2018
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The need for in situ nitrogen oxide measurements on a global scale is crucial to improve the chemistry in global chemistry models and evaluate satellite retrievals. Here we present the characterization of the new IAGOS NOx instrument installed on passenger aircraft, which will provide statistical robust measurements from the surface up to 13 km.
Hendrik Fuchs, Sascha Albrecht, Ismail–Hakki Acir, Birger Bohn, Martin Breitenlechner, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Martin Kaminski, Frank N. Keutsch, Anna Novelli, David Reimer, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, Alexander Zaytsev, Astrid Kiendler-Scharr, and Andreas Wahner
Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, https://doi.org/10.5194/acp-18-8001-2018, 2018
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The photooxidation of methyl vinyl ketone MVK, one of the most important products of isoprene that is emitted by plants, was investigated in the atmospheric simulation chamber SAPHIR for conditions found in forested areas. The comparison of measured trace gas time series with model calculations shows a gap in the understanding of radical chemistry in the MVK oxidation scheme. The possibility of unimolecular isomerization reactions were investigated by means of quantum-chemical calculations.
Marco Pandolfi, Lucas Alados-Arboledas, Andrés Alastuey, Marcos Andrade, Christo Angelov, Begoña Artiñano, John Backman, Urs Baltensperger, Paolo Bonasoni, Nicolas Bukowiecki, Martine Collaud Coen, Sébastien Conil, Esther Coz, Vincent Crenn, Vadimas Dudoitis, Marina Ealo, Kostas Eleftheriadis, Olivier Favez, Prodromos Fetfatzis, Markus Fiebig, Harald Flentje, Patrick Ginot, Martin Gysel, Bas Henzing, Andras Hoffer, Adela Holubova Smejkalova, Ivo Kalapov, Nikos Kalivitis, Giorgos Kouvarakis, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Chris Lunder, Krista Luoma, Hassan Lyamani, Angela Marinoni, Nikos Mihalopoulos, Marcel Moerman, José Nicolas, Colin O'Dowd, Tuukka Petäjä, Jean-Eudes Petit, Jean Marc Pichon, Nina Prokopciuk, Jean-Philippe Putaud, Sergio Rodríguez, Jean Sciare, Karine Sellegri, Erik Swietlicki, Gloria Titos, Thomas Tuch, Peter Tunved, Vidmantas Ulevicius, Aditya Vaishya, Milan Vana, Aki Virkkula, Stergios Vratolis, Ernest Weingartner, Alfred Wiedensohler, and Paolo Laj
Atmos. Chem. Phys., 18, 7877–7911, https://doi.org/10.5194/acp-18-7877-2018, https://doi.org/10.5194/acp-18-7877-2018, 2018
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This investigation presents the variability in near-surface in situ aerosol particle light-scattering measurements obtained over the past decade at 28 measuring atmospheric observatories which are part of the ACTRIS Research Infrastructure, and most of them belong to the GAW network. This paper provides a comprehensive picture of the spatial and temporal variability of aerosol particles optical properties in Europe.
Mingjin Wang, Tong Zhu, Defeng Zhao, Florian Rubach, Andreas Wahner, Astrid Kiendler-Scharr, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 7345–7359, https://doi.org/10.5194/acp-18-7345-2018, https://doi.org/10.5194/acp-18-7345-2018, 2018
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Organic coatings modify hygroscopicity and CCN activation of mineral dust perticles. Small amounts of oleic acid coating (volume fraction (vf) ≤ 4.1 %) decreased the CCN activity of CaCO3 particles, while more oleic acid coating (vf ≥ 14.8 %) increased the CCN activity of CaCO3 particles, while malonic acid coating (vf = 0.4−42 %) even in smallest amounts increased the CCN activity of CaCO3 particles. Our laboratory results should also hold under conditions of the atmosphere.
Silvia Bucci, Paolo Cristofanelli, Stefano Decesari, Angela Marinoni, Silvia Sandrini, Johannes Größ, Alfred Wiedensohler, Chiara F. Di Marco, Eiko Nemitz, Francesco Cairo, Luca Di Liberto, and Federico Fierli
Atmos. Chem. Phys., 18, 5371–5389, https://doi.org/10.5194/acp-18-5371-2018, https://doi.org/10.5194/acp-18-5371-2018, 2018
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This paper analyses some of the processes affecting PM levels over the Po Valley, one of the most polluted regions of Europe, during the 2012 summer campaigns. Under conditions of air transport from the Sahara, data show that desert dust can rapidly penetrate into the lower atmosphere, directly affecting the PM concentration at the ground. Processes of particles growth in high relative humidity and uplift of local soil particles, potentially affecting PM level, are also analysed.
Liwei Wang, Xinfeng Wang, Rongrong Gu, Hao Wang, Lan Yao, Liang Wen, Fanping Zhu, Weihao Wang, Likun Xue, Lingxiao Yang, Keding Lu, Jianmin Chen, Tao Wang, Yuanghang Zhang, and Wenxing Wang
Atmos. Chem. Phys., 18, 4349–4359, https://doi.org/10.5194/acp-18-4349-2018, https://doi.org/10.5194/acp-18-4349-2018, 2018
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This study presents concentrations, variation characteristics, sources and secondary formations of nitrated phenols, a major component of brown carbon, in typical seasons at four sites in northern China. The results highlight the strong influences and contributions of anthropogenic activities, in particular coal combustion and the aging processes, to the atmospheric nitrated phenols in this region.
Jacob T. Shaw, Richard T. Lidster, Danny R. Cryer, Noelia Ramirez, Fiona C. Whiting, Graham A. Boustead, Lisa K. Whalley, Trevor Ingham, Andrew R. Rickard, Rachel E. Dunmore, Dwayne E. Heard, Ally C. Lewis, Lucy J. Carpenter, Jacqui F. Hamilton, and Terry J. Dillon
Atmos. Chem. Phys., 18, 4039–4054, https://doi.org/10.5194/acp-18-4039-2018, https://doi.org/10.5194/acp-18-4039-2018, 2018
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The lifetime of a chemical in the atmosphere is largely governed by the rate of its reaction with the hydroxyl radical (OH). Measurements of rates for many of the thousands of identified volatile organic compounds (VOCs) have yet to be determined experimentally. We have developed a new technique for the rapid determination of gas-phase rate coefficients for the simultaneous reactions between multiple VOCs and OH. The method is tasted across a range of scenarios and is used to derive new values.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Lisa K. Whalley, Daniel Stone, Rachel Dunmore, Jacqueline Hamilton, James R. Hopkins, James D. Lee, Alastair C. Lewis, Paul Williams, Jörg Kleffmann, Sebastian Laufs, Robert Woodward-Massey, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, https://doi.org/10.5194/acp-18-2547-2018, 2018
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This paper presents the first radical observations made in London and subsequent model comparisons. This work highlights that there are uncertainties in the degradation mechanism of complex biogenic and diesel-related VOC species under low-NOx conditions and under high-NOx conditions there is a missing source of RO2 radicals. The impact of these model uncertainties on in situ ozone production as a function of NOx is discussed.
Johannes Größ, Amar Hamed, André Sonntag, Gerald Spindler, Hanna Elina Manninen, Tuomo Nieminen, Markku Kulmala, Urmas Hõrrak, Christian Plass-Dülmer, Alfred Wiedensohler, and Wolfram Birmili
Atmos. Chem. Phys., 18, 1835–1861, https://doi.org/10.5194/acp-18-1835-2018, https://doi.org/10.5194/acp-18-1835-2018, 2018
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This paper revisits the atmospheric new particle formation (NPF) process in the polluted troposphere. Novel aspects include a new NPF classification, which aims at more objectivity, and a long-term analysis of neutral cluster and air ion spectrometer data. Intense NPF events were associated with enhanced sulfur dioxide concentrations and solar radiation, while no significant relationships were observed with the condensation sink, surface-measured turbulence parameters, or ammonia.
Defeng Zhao, Sebastian H. Schmitt, Mingjin Wang, Ismail-Hakki Acir, Ralf Tillmann, Zhaofeng Tan, Anna Novelli, Hendrik Fuchs, Iida Pullinen, Robert Wegener, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 1611–1628, https://doi.org/10.5194/acp-18-1611-2018, https://doi.org/10.5194/acp-18-1611-2018, 2018
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Air pollutants emitted by human activities such as NOx and SO2 can influence the abundance of secondary organic aerosol (SOA) from biogenic volatile organic compounds (VOCs). We found that NOx suppressed new particle formation and SOA mass formation. When both SO2 and NOx are present, the suppressing effect of NOx on SOA mass formation was counteracted by SO2. High NOx changed SOA chemical composition, forming more organic nitrate, because NOx changed radical chemistry during VOC oxidation.
Sebastian Düsing, Birgit Wehner, Patric Seifert, Albert Ansmann, Holger Baars, Florian Ditas, Silvia Henning, Nan Ma, Laurent Poulain, Holger Siebert, Alfred Wiedensohler, and Andreas Macke
Atmos. Chem. Phys., 18, 1263–1290, https://doi.org/10.5194/acp-18-1263-2018, https://doi.org/10.5194/acp-18-1263-2018, 2018
Ying Chen, Ralf Wolke, Liang Ran, Wolfram Birmili, Gerald Spindler, Wolfram Schröder, Hang Su, Yafang Cheng, Ina Tegen, and Alfred Wiedensohler
Atmos. Chem. Phys., 18, 673–689, https://doi.org/10.5194/acp-18-673-2018, https://doi.org/10.5194/acp-18-673-2018, 2018
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The heterogeneous hydrolysis of N2O5 on particle surfaces is crucial for the nitrogen cycle in the atmosphere. The reaction rate is determined by meteorological and particle properties, but its parameterization in previous 3-D modelling studies did not comprehensively consider these parameters. We propose a parameterization to take these into account and improve nitrate prediction; we report that the organic coating suppression on the N2O5 reaction is not as important as expected in the EU.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
Lavinia Onel, Alexander Brennan, Michele Gianella, Grace Ronnie, Ana Lawry Aguila, Gus Hancock, Lisa Whalley, Paul W. Seakins, Grant A. D. Ritchie, and Dwayne E. Heard
Atmos. Meas. Tech., 10, 4877–4894, https://doi.org/10.5194/amt-10-4877-2017, https://doi.org/10.5194/amt-10-4877-2017, 2017
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Hydroperoxy (HO2) radicals are key intermediates participating in a rapid chemical cycling at the centre of the tropospheric oxidation. Fluorescence assay by gas expansion (FAGE) technique is the most commonly used for the HO2 measurements in the atmosphere. However, FAGE is an indirect technique, requiring calibration. This work finds a good agreement between the indirect FAGE method and the direct cavity ring-down spectroscopy method and hence validates FAGE and the FAGE calibration method.
Lavinia Onel, Alexander Brennan, Paul W. Seakins, Lisa Whalley, and Dwayne E. Heard
Atmos. Meas. Tech., 10, 3985–4000, https://doi.org/10.5194/amt-10-3985-2017, https://doi.org/10.5194/amt-10-3985-2017, 2017
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Methyl peroxy (CH3O2) radicals are the most abundant organic peroxy radical species and are critical intermediates in rapid chemical cycling at the heart of tropospheric oxidation. Despite their importance, at present CH3O2 radicals are not specifically measured in the atmosphere by any direct or indirect method. This work presents a new method for the selective and sensitive detection of CH3O2 radicals and its use for the measurement of CH3O2 in the atmospheric simulation chamber HIRAC.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Florian Berkes, Patrick Neis, Martin G. Schultz, Ulrich Bundke, Susanne Rohs, Herman G. J. Smit, Andreas Wahner, Paul Konopka, Damien Boulanger, Philippe Nédélec, Valerie Thouret, and Andreas Petzold
Atmos. Chem. Phys., 17, 12495–12508, https://doi.org/10.5194/acp-17-12495-2017, https://doi.org/10.5194/acp-17-12495-2017, 2017
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This study highlights the importance of independent global measurements with high and long-term accuracy to quantify long-term changes, especially in the UTLS region, and to help identify inconsistencies between different data sets of observations and models. Here we investigated temperature trends over different regions within a climate-sensitive area of the atmosphere and demonstrated the value of the IAGOS temperature observations as an anchor point for the evaluation of reanalyses.
Mingjin Tang, Xin Huang, Keding Lu, Maofa Ge, Yongjie Li, Peng Cheng, Tong Zhu, Aijun Ding, Yuanhang Zhang, Sasho Gligorovski, Wei Song, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 17, 11727–11777, https://doi.org/10.5194/acp-17-11727-2017, https://doi.org/10.5194/acp-17-11727-2017, 2017
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We provide a comprehensive and critical review of laboratory studies of heterogeneous uptake of OH, NO3, O3, and their directly related species by mineral dust particles. The atmospheric importance of heterogeneous uptake as sinks for these species is also assessed. In addition, we have outlined major open questions and challenges in this field and discussed research strategies to address them.
Matthew J. Gunsch, Rachel M. Kirpes, Katheryn R. Kolesar, Tate E. Barrett, Swarup China, Rebecca J. Sheesley, Alexander Laskin, Alfred Wiedensohler, Thomas Tuch, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 10879–10892, https://doi.org/10.5194/acp-17-10879-2017, https://doi.org/10.5194/acp-17-10879-2017, 2017
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Arctic sea ice loss is leading to increasing petroleum extraction and shipping. It is necessary to identify emissions from these activities for improved Arctic air quality and climate assessment. Atmospheric particles were measured from August to September 2015 in Utqiaġvik, AK. For periods influenced by Prudhoe Bay, significant influence associated with combustion emissions was observed, compared to fresh sea spray influence during Arctic Ocean periods.
Yujiao Zhu, Caiqing Yan, Renyi Zhang, Zifa Wang, Mei Zheng, Huiwang Gao, Yang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 17, 9469–9484, https://doi.org/10.5194/acp-17-9469-2017, https://doi.org/10.5194/acp-17-9469-2017, 2017
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This study reports the distinct effects of street canyons on new particle formation (NPF) under warm or cold ambient temperature conditions because of on-road vehicle emissions; i.e., stronger condensation sinks are responsible for the reduced NPF in the springtime, but efficient nucleation and partitioning of gaseous species contribute to the enhanced NPF in the wintertime. The oxidization of biogenic organics is suggested to play an important role in growing new particles.
Cheng Wu, Iida Pullinen, Stefanie Andres, Astrid Kiendler-Scharr, Einhard Kleist, Andreas Wahner, Jürgen Wildt, and Thomas F. Mentel
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-260, https://doi.org/10.5194/bg-2017-260, 2017
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Biogenic volatile organic compounds are important for atmospheric chemistry. We showed by 13CO2 labelling experiments that biosynthesis is not restricted to the presence of light. In particular sesquiterpenes exhibit substantial de novo emissions in darkness with the carbon being delivered from alternative carbon sources. Our findings are of importance for future emissions under conditions of climate change as the response of de novo emissions to stresses differs from that of pool emissions.
Yudong Yang, Min Shao, Stephan Keßel, Yue Li, Keding Lu, Sihua Lu, Jonathan Williams, Yuanhang Zhang, Liming Zeng, Anke C. Nölscher, Yusheng Wu, Xuemei Wang, and Junyu Zheng
Atmos. Chem. Phys., 17, 7127–7142, https://doi.org/10.5194/acp-17-7127-2017, https://doi.org/10.5194/acp-17-7127-2017, 2017
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Total OH reactivity is an important parameter to evaluate understanding of atmospheric chemistry, especially the VOC contribution to air pollution. Measured by comparative reactivity methods, total OH reactivity in Beijing and Heshan revealed significant differences between measured and calculated results, such as missing reactivity, which were related to unmeasured primary or secondary species. This missing reactivity would introduce a 21–30 % underestimation for ozone production efficiency.
Martin Kaminski, Hendrik Fuchs, Ismail-Hakki Acir, Birger Bohn, Theo Brauers, Hans-Peter Dorn, Rolf Häseler, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, and Andreas Wahner
Atmos. Chem. Phys., 17, 6631–6650, https://doi.org/10.5194/acp-17-6631-2017, https://doi.org/10.5194/acp-17-6631-2017, 2017
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Monoterpenes emitted by trees are among the volatile organic compounds with the highest global emission rates. The atmospheric degradation of the monoterpene β-pinene was investigated in the atmosphere simulation chamber SAPHIR in Jülich under low NOx and atmospheric β-pinene concentrations. While the budget of OH was balanced, both OH and HO2 concentrations were underestimated in the simulation results. These observations suggest the existence of unaccounted sources of HO2.
Kgaugelo Euphinia Chiloane, Johan Paul Beukes, Pieter Gideon van Zyl, Petra Maritz, Ville Vakkari, Miroslav Josipovic, Andrew Derick Venter, Kerneels Jaars, Petri Tiitta, Markku Kulmala, Alfred Wiedensohler, Catherine Liousse, Gabisile Vuyisile Mkhatshwa, Avishkar Ramandh, and Lauri Laakso
Atmos. Chem. Phys., 17, 6177–6196, https://doi.org/10.5194/acp-17-6177-2017, https://doi.org/10.5194/acp-17-6177-2017, 2017
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This paper presents atmospheric black carbon (BC) data collected in South Africa (SA). In general, BC level were higher than in the developed world. At one site, five sources were identified, with household combustion as well as savannah and grassland fires the most significant sources during winter and spring, while coal-fired power stations, pyrometallurgical smelters and traffic contributed year round.
Haichao Wang, Jun Chen, and Keding Lu
Atmos. Meas. Tech., 10, 1465–1479, https://doi.org/10.5194/amt-10-1465-2017, https://doi.org/10.5194/amt-10-1465-2017, 2017
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A new incoherent broadband cavity-enhanced absorption spectrometer for ambient NO3 and N2O5 detection is developed. This new instrument is featured with a mechanically aligned non-adjustable optical mounting system. Fast setup and stable running of this N2O5 spectrometer were successfully achieved during recent field campaigns in China due to this new feature. In addition, a dynamic reference spectrum is used for the CEAS type of instrument by NO titration for the first time.
Yuxuan Zhang, Hang Su, Simonas Kecorius, Zhibin Wang, Min Hu, Tong Zhu, Kebin He, Alfred Wiedensohler, Qiang Zhang, and Yafang Cheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-222, https://doi.org/10.5194/acp-2017-222, 2017
Revised manuscript not accepted
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The light absorption of black carbon (BC) strongly depends on their mixing state. By now, the BC mixing state in the atmosphere is still unclear. In this work, we have investigated the comprehensive characterization of BC mixing state at a polluted regional background site of the North China Plain (NCP) based on in site measurements. we found that BC aerosols of the NCP were fully aged, suggesting a strong optical and climate effect of BC on the regional scale in northern China.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Clémence Rose, Karine Sellegri, Isabel Moreno, Fernando Velarde, Michel Ramonet, Kay Weinhold, Radovan Krejci, Marcos Andrade, Alfred Wiedensohler, Patrick Ginot, and Paolo Laj
Atmos. Chem. Phys., 17, 1529–1541, https://doi.org/10.5194/acp-17-1529-2017, https://doi.org/10.5194/acp-17-1529-2017, 2017
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Using an indirect method based on particle size distribution measurements, we show that new particle formation (NPF) is responsible for a large contribution to the cloud condensation nuclei concentration at the highest observatory in the world (Bolivia, 5240 m a.s.l.) as expected from some global model predictions. We also provide unique results related to the influence of the boundary layer on the NPF process, showing direct evidence for the important NPF frequency in the free troposphere.
Shurui Chen, Liang Xu, Yinxiao Zhang, Bing Chen, Xinfeng Wang, Xiaoye Zhang, Mei Zheng, Jianmin Chen, Wenxing Wang, Yele Sun, Pingqing Fu, Zifa Wang, and Weijun Li
Atmos. Chem. Phys., 17, 1259–1270, https://doi.org/10.5194/acp-17-1259-2017, https://doi.org/10.5194/acp-17-1259-2017, 2017
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Many studies have focused on the unusually severe hazes instead of the more frequent light and moderate hazes (22–63 %) in winter in the North China Plain (NCP). The morphology, mixing state, and size of organic aerosols in the L & M hazes were characterized. We conclude that the direct emissions from residential coal stoves without any pollution controls in rural and urban outskirts contribute large amounts of primary OM particles to the regional L & M hazes in winter in the NCP.
Zhaofeng Tan, Hendrik Fuchs, Keding Lu, Andreas Hofzumahaus, Birger Bohn, Sebastian Broch, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinsong Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 663–690, https://doi.org/10.5194/acp-17-663-2017, https://doi.org/10.5194/acp-17-663-2017, 2017
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In this study, we performed accurate OH measurements as well as selective HO2 and RO2 measurements at a rural site in North China Plain with state-of-the-art instruments newly developed. We confirmed the previous discovery on the enhancement of the OH in low NOx with which little O3 production was associated, and we found a missing RO2 source in high NOx which promoted higher O3 production. Our results are of vital importance for ozone abatement strategies currently under discussion for China.
Hendrik Fuchs, Zhaofeng Tan, Keding Lu, Birger Bohn, Sebastian Broch, Steven S. Brown, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Kyung-Eun Min, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinson Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 645–661, https://doi.org/10.5194/acp-17-645-2017, https://doi.org/10.5194/acp-17-645-2017, 2017
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OH reactivity was measured during a 1-month long campaign at a rural site in the North China Plain in 2014. OH reactivity measurements are compared to calculations using OH reactant measurements. Good agreement is found indicating that all important OH reactants were measured. In addition, the chemical OH budget is analyzed. In contrast to previous campaigns in China in 2006, no significant imbalance between OH production and destruction is found.
Yee Jun Tham, Zhe Wang, Qinyi Li, Hui Yun, Weihao Wang, Xinfeng Wang, Likun Xue, Keding Lu, Nan Ma, Birger Bohn, Xin Li, Simonas Kecorius, Johannes Größ, Min Shao, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 16, 14959–14977, https://doi.org/10.5194/acp-16-14959-2016, https://doi.org/10.5194/acp-16-14959-2016, 2016
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This work addresses the unclear global significance of chlorine activation processes in the troposphere. The first high-quality measurement data set of ClNO2 in northern China revealed strong ClNO2 production in the residual layers, and demonstrated its significant effects on radical budget and ozone production. Our findings imply the widespread effects of ClNO2 over the polluted regions of northern China, which may increase photochemical and haze pollution.
Wei Hu, Min Hu, Wei-Wei Hu, Hongya Niu, Jing Zheng, Yusheng Wu, Wentai Chen, Chen Chen, Lingyu Li, Min Shao, Shaodong Xie, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 13213–13230, https://doi.org/10.5194/acp-16-13213-2016, https://doi.org/10.5194/acp-16-13213-2016, 2016
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An Aerodyne high-resolution time-of-flight AMS was deployed at a suburban site in the Sichuan Basin, southwestern China, under high emission intensity, and unique geographical and adverse meteorological conditions. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. The contributions of BBOA and BC to PM1 were high in primary emission episodes, highlighting the critical influence of biomass burning.
Hang Su, Yafang Cheng, Nan Ma, Zhibin Wang, Xiaoxiang Wang, Mira L. Pöhlker, Björn Nillius, Alfred Wiedensohler, and Ulrich Pöschl
Atmos. Meas. Tech., 9, 5183–5192, https://doi.org/10.5194/amt-9-5183-2016, https://doi.org/10.5194/amt-9-5183-2016, 2016
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In cloud condensation nuclei (CCN) measurements, the supersaturation scan is often time-consuming and limits the temporal resolution of CCN measurements. Here we present a new concept, termed the broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned, resulting in fast measurements of CCN activity.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Óscar Gálvez, M. Teresa Baeza-Romero, Mikel Sanz, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 16, 12703–12713, https://doi.org/10.5194/acp-16-12703-2016, https://doi.org/10.5194/acp-16-12703-2016, 2016
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Reactive iodine species play a key role in the oxidation capacity of the polar troposphere, although sources and mechanisms are poorly understood. In this paper, the photolysis of frozen iodate salt has been studied, confirming that under near-UV–Vis radiation iodate is photolysed. Incorporating this result into an Antarctic atmospheric model, we have shown that it could increase the atmospheric IO levels and could constitute a pathway for the release of active iodine to the polar atmosphere
Ying Chen, Yafang Cheng, Nan Ma, Ralf Wolke, Stephan Nordmann, Stephanie Schüttauf, Liang Ran, Birgit Wehner, Wolfram Birmili, Hugo A. C. Denier van der Gon, Qing Mu, Stefan Barthel, Gerald Spindler, Bastian Stieger, Konrad Müller, Guang-Jie Zheng, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 12081–12097, https://doi.org/10.5194/acp-16-12081-2016, https://doi.org/10.5194/acp-16-12081-2016, 2016
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Sea salt aerosol (SSA) is important for primary and secondary aerosols on a global scale. During 10–20 September 2013, the SSA mass concentration was overestimated by a factor of 8–20 over central Europe by WRF-Chem model, stem from the uncertainty of its emission scheme. This could facilitate the coarse-mode nitrate formation (~ 140 % but inhibit the fine-mode nitrate formation (~−20 %). A special long-range transport mechanism could broaden this influence of SSA to a larger downwind region.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Quynh T. Nguyen, Marianne Glasius, Lise L. Sørensen, Bjarne Jensen, Henrik Skov, Wolfram Birmili, Alfred Wiedensohler, Adam Kristensson, Jacob K. Nøjgaard, and Andreas Massling
Atmos. Chem. Phys., 16, 11319–11336, https://doi.org/10.5194/acp-16-11319-2016, https://doi.org/10.5194/acp-16-11319-2016, 2016
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Aerosol particles strongly influence climate change as they can absorb or reflect solar radiation. This work investigates aerosol particles in the remote northern Arctic. "Newly born" particles are small, then they "age" and grow in size due to different mechanisms. The results showed that during the polar night and especially Arctic spring, particles were likely transported from longer distances and were aged. During summer, "younger" particles are observed, which might be linked to ozone.
Mehrnaz Sarrafzadeh, Jürgen Wildt, Iida Pullinen, Monika Springer, Einhard Kleist, Ralf Tillmann, Sebastian H. Schmitt, Cheng Wu, Thomas F. Mentel, Defeng Zhao, Donald R. Hastie, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 16, 11237–11248, https://doi.org/10.5194/acp-16-11237-2016, https://doi.org/10.5194/acp-16-11237-2016, 2016
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We investigated NOx impacts on the formation of secondary organic aerosol (SOA) mass from b-pinene and we could reveal two different mechanisms of impacts. One of them was the impact of NOx on OH that could explain increasing SOA yield with increasing NOx at low NOx conditions. The other was the suppression of new particle formation limiting the condensational sink for the SOA precursors. This effect could explain a substantial fraction of the decrease of SOA yield observed at high NOx.
Yin Wang, Zhongming Chen, Qinqin Wu, Hao Liang, Liubin Huang, Huan Li, Keding Lu, Yusheng Wu, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 10985–11000, https://doi.org/10.5194/acp-16-10985-2016, https://doi.org/10.5194/acp-16-10985-2016, 2016
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Comparison of modeled and measured peroxide concentrations at a rural site in the summer North China Plain demonstrated an underestimation during biomass burning events and an overestimation on haze days, which were related to the direct production of peroxides from biomass burning and the heterogeneous uptake of peroxides by aerosols, respectively. Our findings are of great significance for comprehensively understanding the chemical budget of atmospheric peroxides in detail.
Wolfram Birmili, Kay Weinhold, Fabian Rasch, André Sonntag, Jia Sun, Maik Merkel, Alfred Wiedensohler, Susanne Bastian, Alexander Schladitz, Gunter Löschau, Josef Cyrys, Mike Pitz, Jianwei Gu, Thomas Kusch, Harald Flentje, Ulrich Quass, Heinz Kaminski, Thomas A. J. Kuhlbusch, Frank Meinhardt, Andreas Schwerin, Olaf Bath, Ludwig Ries, Holger Gerwig, Klaus Wirtz, and Markus Fiebig
Earth Syst. Sci. Data, 8, 355–382, https://doi.org/10.5194/essd-8-355-2016, https://doi.org/10.5194/essd-8-355-2016, 2016
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The German Ultrafine Aerosol Network (GUAN) provides new continuous data on tropospheric aerosol particles including number size distributions and black carbon. The data are equally relevant for atmospheric studies related to both climate-related and health-related issues. The published data underwent uniform measures of quality assurance and control. The data are available free of charge at the World Data Center for Aerosols EBAS data repository.
Birger Bohn, Dwayne E. Heard, Nikolaos Mihalopoulos, Christian Plass-Dülmer, Rainer Schmitt, and Lisa K. Whalley
Atmos. Meas. Tech., 9, 3455–3466, https://doi.org/10.5194/amt-9-3455-2016, https://doi.org/10.5194/amt-9-3455-2016, 2016
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Filter radiometers are instruments that quantify the rate of formation of excited oxygen atoms from photolysis of ozone in the atmosphere. The excited oxygen atoms are important for the atmospheric self-cleaning ability. The radiometers were characterised by measurements of their spectral response. Together with field comparisons with a reference instrument, the characterisations improved the performance. That will help to better understand atmospheric photochemistry in future research.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
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, https://doi.org/10.5194/acp-16-8593-2016, https://doi.org/10.5194/acp-16-8593-2016, 2016
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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.
Daniel Stone, Lisa K. Whalley, Trevor Ingham, Peter M. Edwards, Danny R. Cryer, Charlotte A. Brumby, Paul W. Seakins, and Dwayne E. Heard
Atmos. Meas. Tech., 9, 2827–2844, https://doi.org/10.5194/amt-9-2827-2016, https://doi.org/10.5194/amt-9-2827-2016, 2016
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OH reactivity is the total pseudo-first-order loss rate coefficient describing the removal of OH radicals to all sinks in the atmosphere. Measurements of ambient OH reactivity can be used to discover the extent to which measured OH sinks contribute to the total OH loss rate. In this work, we describe the design and characterisation of an instrument to measure OH reactivity using laser flash photolysis coupled to laser-induced fluorescence (LFP-LIF) spectroscopy.
Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108, https://doi.org/10.5194/acp-16-8095-2016, https://doi.org/10.5194/acp-16-8095-2016, 2016
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This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
Bernadette Rosati, Martin Gysel, Florian Rubach, Thomas F. Mentel, Brigitta Goger, Laurent Poulain, Patrick Schlag, Pasi Miettinen, Aki Pajunoja, Annele Virtanen, Henk Klein Baltink, J. S. Bas Henzing, Johannes Größ, Gian Paolo Gobbi, Alfred Wiedensohler, Astrid Kiendler-Scharr, Stefano Decesari, Maria Cristina Facchini, Ernest Weingartner, and Urs Baltensperger
Atmos. Chem. Phys., 16, 7295–7315, https://doi.org/10.5194/acp-16-7295-2016, https://doi.org/10.5194/acp-16-7295-2016, 2016
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This study presents PEGASOS project data from field campaigns in the Po Valley, Italy and the Netherlands. Vertical profiles of aerosol hygroscopicity and chemical composition were investigated with airborne measurements on board a Zeppelin NT airship. A special focus was on the evolution of different mixing layers within the PBL as a function of daytime. A closure study showed that variations in aerosol hygroscopicity can well be explained by the variations in chemical composition.
Markus Hermann, Andreas Weigelt, Denise Assmann, Sascha Pfeifer, Thomas Müller, Thomas Conrath, Jens Voigtländer, Jost Heintzenberg, Alfred Wiedensohler, Bengt G. Martinsson, Terry Deshler, Carl A. M. Brenninkmeijer, and Andreas Zahn
Atmos. Meas. Tech., 9, 2179–2194, https://doi.org/10.5194/amt-9-2179-2016, https://doi.org/10.5194/amt-9-2179-2016, 2016
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Aerosol particles are an important component of the Earth's atmosphere. Here we describe the composition and characterization of a new optical particle size spectrometer (OPSS) for aircraft-borne measurements of the aerosol particle size distribution (how many particles there are with a certain size) in the 140–1050 nm size range. The OPSS was characterized throughout concerning its measurement capabilities (response, pressure dependence, coincidence) and validated versus balloon measurement.
Yuxuan Zhang, Qiang Zhang, Yafang Cheng, Hang Su, Simonas Kecorius, Zhibin Wang, Zhijun Wu, Min Hu, Tong Zhu, Alfred Wiedensohler, and Kebin He
Atmos. Meas. Tech., 9, 1833–1843, https://doi.org/10.5194/amt-9-1833-2016, https://doi.org/10.5194/amt-9-1833-2016, 2016
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We develop a novel method in this work for in situ measurements of the morphology and effective density of ambient In-BC cores using a volatility tandem differential mobility analyzer and a single-particle soot photometer. We find that In-BC cores hardly transform the morphology of BC into a void-free sphere. Taking the morphology and density of ambient In-BC cores into account, our work provides a new insight into the enhancement of light absorption for In-BC particles in the atmosphere.
Bernadette Rosati, Erik Herrmann, Silvia Bucci, Federico Fierli, Francesco Cairo, Martin Gysel, Ralf Tillmann, Johannes Größ, Gian Paolo Gobbi, Luca Di Liberto, Guido Di Donfrancesco, Alfred Wiedensohler, Ernest Weingartner, Annele Virtanen, Thomas F. Mentel, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4539–4554, https://doi.org/10.5194/acp-16-4539-2016, https://doi.org/10.5194/acp-16-4539-2016, 2016
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We present vertical profiles of aerosol optical properties, which were explored within the planetary boundary layer in a case study in 2012 in the Po Valley region. A comparison of in situ measurements recorded aboard a Zeppelin NT and ground-based remote-sensing data was performed yielding good agreement. Additionally, the role of ambient relative humidity for the aerosol particles' optical properties was investigated.
Hendrik Fuchs, Zhaofeng Tan, Andreas Hofzumahaus, Sebastian Broch, Hans-Peter Dorn, Frank Holland, Christopher Künstler, Sebastian Gomm, Franz Rohrer, Stephanie Schrade, Ralf Tillmann, and Andreas Wahner
Atmos. Meas. Tech., 9, 1431–1447, https://doi.org/10.5194/amt-9-1431-2016, https://doi.org/10.5194/amt-9-1431-2016, 2016
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The hydroxyl radical is the key reactant that controls the chemical transformation of pollutants in the atmosphere. Observations of nighttime radicals concentrations were larger than predicted by models in field campaigns in forested and urban environments. Here, we investigated, if measurements could have been affected by artifacts. No significant interferences were found for atmospheric concentrations of reactants in ozonolysis experiments, but small artificats from nitrate radicals.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
T. Hohaus, U. Kuhn, S. Andres, M. Kaminski, F. Rohrer, R. Tillmann, A. Wahner, R. Wegener, Z. Yu, and A. Kiendler-Scharr
Atmos. Meas. Tech., 9, 1247–1259, https://doi.org/10.5194/amt-9-1247-2016, https://doi.org/10.5194/amt-9-1247-2016, 2016
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As an extension of the atmosphere simulation chamber SAPHIR, an environmentally-controlled dynamic (flow-through) plant chamber under SAPHIR (SAPHIR-PLUS) was developed. This facility allows for feeding a natural blend of biogenic trace gases into SAPHIR. PLUS is utilized to characterize the atmospheric chemistry of natural trace gas mixtures at close to ambient concentration levels. In this study, the results of the initial characterization experiments are presented in detail.
Andrea Ghirardo, Junfei Xie, Xunhua Zheng, Yuesi Wang, Rüdiger Grote, Katja Block, Jürgen Wildt, Thomas Mentel, Astrid Kiendler-Scharr, Mattias Hallquist, Klaus Butterbach-Bahl, and Jörg-Peter Schnitzler
Atmos. Chem. Phys., 16, 2901–2920, https://doi.org/10.5194/acp-16-2901-2016, https://doi.org/10.5194/acp-16-2901-2016, 2016
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Trees can impact urban air quality. Large emissions of plant volatiles are emitted in Beijing as a stress response to the urban polluted environment, but their impacts on secondary particulate matter remain relatively low compared to those originated from anthropogenic activities. The present study highlights the importance of including stress-induced compounds when studying plant volatile emissions.
J. D. Lee, L. K. Whalley, D. E. Heard, D. Stone, R. E. Dunmore, J. F. Hamilton, D. E. Young, J. D. Allan, S. Laufs, and J. Kleffmann
Atmos. Chem. Phys., 16, 2747–2764, https://doi.org/10.5194/acp-16-2747-2016, https://doi.org/10.5194/acp-16-2747-2016, 2016
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This paper presents field measurements of HONO and a range of other gas phase and particulate species from an urban background site in London. The measured daytime HONO cannot be reproduced with a simple box model and thus a significant daytime missing source of HONO is present. We show that this missing source could be responsible for 40 % of the OH radical source and 57 % of the OH initiation; hence its potential importance for atmospheric oxidation and ozone production.
Thomas B. Kristensen, Thomas Müller, Konrad Kandler, Nathalie Benker, Markus Hartmann, Joseph M. Prospero, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 16, 2675–2688, https://doi.org/10.5194/acp-16-2675-2016, https://doi.org/10.5194/acp-16-2675-2016, 2016
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We have investigated the cloud condensation nuclei (CCN) properties in the trade wind marine boundary layer of the western North Atlantic during the dust season. Little is known about the CCN influencing cloud optical properties in that region. High mass concentrations of mineral dust were observed, but the number concentrations of mineral dust and sea salt were not high enough to influence CCN properties, and the CCN were likely to be dominated by a mixture of sulfates and organic species.
Lisa K. Whalley, Daniel Stone, Brian Bandy, Rachel Dunmore, Jacqueline F. Hamilton, James Hopkins, James D. Lee, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, https://doi.org/10.5194/acp-16-2109-2016, 2016
M. Dal Maso, L. Liao, J. Wildt, A. Kiendler-Scharr, E. Kleist, R. Tillmann, M. Sipilä, J. Hakala, K. Lehtipalo, M. Ehn, V.-M. Kerminen, M. Kulmala, D. Worsnop, and T. Mentel
Atmos. Chem. Phys., 16, 1955–1970, https://doi.org/10.5194/acp-16-1955-2016, https://doi.org/10.5194/acp-16-1955-2016, 2016
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In this paper, we present the first direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We found that the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength, and that the formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid.
Ying Chen, Ya-Fang Cheng, Stephan Nordmann, Wolfram Birmili, Hugo A. C. Denier van der Gon, Nan Ma, Ralf Wolke, Birgit Wehner, Jia Sun, Gerald Spindler, Qing Mu, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 1823–1835, https://doi.org/10.5194/acp-16-1823-2016, https://doi.org/10.5194/acp-16-1823-2016, 2016
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We evaluated the EC point sources in Germany with high-resolution simulation by WRF-Chem, and find out that point sources contribute too much EC in the coarse mode aerosol mass. The area emissions in Eastern Europe and Russia also allocate too much EC emission in coarse mode in the EUCAARI EC emission inventory. Because of the shorter life time of coarse mode EC, about 20–40 % less EC can be transported to Melpitz from Eastern Europe. Size segregation information is important for EC inventories.
K.-E. Min, R. A. Washenfelder, W. P. Dubé, A. O. Langford, P. M. Edwards, K. J. Zarzana, J. Stutz, K. Lu, F. Rohrer, Y. Zhang, and S. S. Brown
Atmos. Meas. Tech., 9, 423–440, https://doi.org/10.5194/amt-9-423-2016, https://doi.org/10.5194/amt-9-423-2016, 2016
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We have developed a two-channel broadband cavity enhanced absorption spectrometer for field measurements of glyoxal, methylglyoxal, nitrous acid, nitrogen dioxide, and water. We have successfully deployed this instrument during two aircraft and two ground-based field campaigns. The demonstrated precision (2σ) for retrievals of CHOCHO, HONO, and NO2 are 34, 350, and 80 parts per trillion (pptv) in 5 s, with accuracy of 5.8, 9.0 and 5.0 %.
Z. J. Wu, J. Zheng, D. J. Shang, Z. F. Du, Y. S. Wu, L. M. Zeng, A. Wiedensohler, and M. Hu
Atmos. Chem. Phys., 16, 1123–1138, https://doi.org/10.5194/acp-16-1123-2016, https://doi.org/10.5194/acp-16-1123-2016, 2016
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Most pre-existing measurements lack a linkage between particle hygroscopicity and chemical composition with a high time resolution in China. Our work provided a general overview of particle hygroscopicity and its closure with chemical composition on the basis of HTDMA and AMS measurements. An increase in particle hygroscopicity with increasing air pollution level was found, as well as a quick transformation from external mixtures to internal mixtures for pre-existing particles during NPF events.
D. F. Zhao, A. Buchholz, B. Kortner, P. Schlag, F. Rubach, H. Fuchs, A. Kiendler-Scharr, R. Tillmann, A. Wahner, Å. K. Watne, M. Hallquist, J. M. Flores, Y. Rudich, K. Kristensen, A. M. K. Hansen, M. Glasius, I. Kourtchev, M. Kalberer, and Th. F. Mentel
Atmos. Chem. Phys., 16, 1105–1121, https://doi.org/10.5194/acp-16-1105-2016, https://doi.org/10.5194/acp-16-1105-2016, 2016
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This study investigated the cloud droplet activation behavior and hygroscopic growth of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Cloud droplet activation behaviors of different types of SOA were similar. In contrast, the hygroscopicity of ASOA was higher than BSOA and ABSOA. ASOA components enhanced the hygroscopicity of the ABSOA. Yet this enhancement cannot be described by a linear mixing of pure SOA systems.
V. N. Dos Santos, E. Herrmann, H. E. Manninen, T. Hussein, J. Hakala, T. Nieminen, P. P. Aalto, M. Merkel, A. Wiedensohler, M. Kulmala, T. Petäjä, and K. Hämeri
Atmos. Chem. Phys., 15, 13717–13737, https://doi.org/10.5194/acp-15-13717-2015, https://doi.org/10.5194/acp-15-13717-2015, 2015
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Atmospheric charged particles, i.e. air ions, contribute to secondary aerosol formation and have an effect on global climate as potential cloud condensation nuclei. We aimed to evaluate air ion concentrations and characteristics during new particle formation (NPF) events in the megacity Paris, France. We analyzed frequency and seasonal v