Articles | Volume 14, issue 23
Research article 15 Dec 2014
Research article | 15 Dec 2014
Emission of iodine-containing volatiles by selected microalgae species
U. R. Thorenz et al.
No articles found.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455,Short summary
We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886,Short summary
We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104,Short summary
Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Bo Galle, Santiago Arellano, Nicole Bobrowski, Vladimir Conde, Tobias P. Fischer, Gustav Gerdes, Alexandra Gutmann, Thorsten Hoffmann, Ima Itikarai, Tomas Krejci, Emma J. Liu, Kila Mulina, Scott Nowicki, Tom Richardson, Julian Rüdiger, Kieran Wood, and Jiazhi Xu
Atmos. Meas. Tech., 14, 4255–4277,Short summary
Measurements of volcanic gases are important for geophysical research, risk assessment and environmental impact studies. Some gases, like SO2 and BrO, may be studied from the ground at a safe distance using remote sensing techniques. Many other gases require in situ access to the gas plume. Here, a drone may be an attractive alternative. This paper describes a drone specially adapted for volcanic gas studies and demonstrates its use in a field campaign at Manam volcano in Papua New Guinea.
Wei Xu, Kirsten N. Fossum, Jurgita Ovadnevaite, Chunshui Lin, Ru-Jin Huang, Colin O'Dowd, and Darius Ceburnis
Atmos. Chem. Phys., 21, 8655–8675,Short summary
Cloud condensation nuclei (CCN) are an important topic in atmospheric studies, especially for evaluating the climate impact of aerosol. Here in this study, CCN closure is studied by using chemical composition based on an aerosol mass spectrometer (AMS) and hygroscopicity growth measurements based on a humidified tandem differential mobility analyzer (HTDMA) at the Mace Head atmospheric research station.
Chao Peng, Patricia N. Razafindrambinina, Kotiba A. Malek, Lanxiadi Chen, Weigang Wang, Ru-Jin Huang, Yuqing Zhang, Xiang Ding, Maofa Ge, Xinming Wang, Akua A. Asa-Awuku, and Mingjin Tang
Atmos. Chem. Phys., 21, 7135–7148,Short summary
Organosulfates are important constituents in tropospheric aerosol particles, but their hygroscopic properties and cloud condensation nuclei activities are not well understood. In our work, three complementary techniques were employed to investigate the interactions of 11 organosulfates with water vapor under sub- and supersaturated conditions.
Inken Heidke, Adam Hartland, Denis Scholz, Andrew Pearson, John Hellstrom, Sebastian F. M. Breitenbach, and Thorsten Hoffmann
Biogeosciences, 18, 2289–2300,Short summary
We analyzed lignin oxidation products (LOPs) in leaf litter and different soil horizons as well as dripwater and flowstone samples from four different cave sites from different vegetation zones in New Zealand using liquid chromatography coupled to mass spectrometry. We test whether the original source-dependent LOP signal of the overlying vegetation is preserved and can be recovered from flowstone samples and investigate how the signal is altered by the transport from the soil to the cave.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697,Short summary
We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys. Discuss.,
Revised manuscript has not been submitted
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393,Short summary
We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943,Short summary
Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730,Short summary
We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Haiyan Ni, Ru-Jin Huang, Max M. Cosijn, Lu Yang, Jie Guo, Junji Cao, and Ulrike Dusek
Atmos. Chem. Phys., 20, 16041–16053,Short summary
We investigated sources of carbonaceous aerosols in Beijing and Xi'an during severe winter haze. Elemental carbon (EC) was dominated by vehicle emissions in Xi’an and coal burning in Beijing. Organic carbon (OC) increment during haze days was driven by the increase in primary and secondary OC (SOC). SOC was more from fossil sources in Beijing than Xi’an, especially during haze days. In Xi’an, no strong day–night differences in EC or OC sources suggest a large accumulation of particles.
Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903,
Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, and Thorsten Hoffmann
Atmos. Meas. Tech. Discuss.,
Revised manuscript accepted for AMTShort summary
Motivated by the special interest in bromine chemistry in volcanic plumes, the study presented here describes a new method for the quantitative collection of gaseous hydrogen bromide in gas diffusion denuders. The hydrogen bromide reacted during sampling with appropriate epoxides applied to the denuder walls. The denuder sampling assembly was successfully deployed in the volcanic plume of Masaya volcano, Nicaragua.
Marcel Weloe and Thorsten Hoffmann
Atmos. Meas. Tech., 13, 5725–5738,Short summary
Aerosol mass spectrometers (AMSs) are frequently applied in atmospheric aerosol research in connection with climate, environmental or health-related projects. The paper describes a new real-time technique for the measurement of organic peroxides, which play an important role in new particle formation and as
reactive oxygen speciesin aerosol–health-related aspects of atmospheric aerosols.
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,Short summary
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.
Chunshui Lin, Darius Ceburnis, Wei Xu, Eimear Heffernan, Stig Hellebust, John Gallagher, Ru-Jin Huang, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 20, 10513–10529,Short summary
Chemical composition and sources of submicron aerosols (PM1) were simultaneously investigated at a kerbside site in the Dublin city center and at a residential site in suburban Dublin (~5 km apart) during both a nonheating and a heating period in 2018. This study highlights the temporal and spatial variability of sources within the Dublin city center and the need for additional aerosol characterization studies to improve targeted mitigation solutions for a greater impact on urban air quality.
Ru-Jin Huang, Yao He, Jing Duan, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Weiwei Hu, Chunshui Lin, Haiyan Ni, Wenting Dai, Junji Cao, Yunfei Wu, Renjian Zhang, Wei Xu, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin D. O'Dowd
Atmos. Chem. Phys., 20, 9101–9114,Short summary
We systematically compared the submicron particle (PM1) processes in haze days with low and high relative humidity (RH) in wintertime Beijing. Nitrate had similar daytime growth rates in low-RH and high-RH pollution. OOA had a higher growth rate in low-RH pollution than in high-RH pollution. Sulfate had a decreasing trend in low-RH pollution, while it increased significantly in high-RH pollution. This distinction may be explained by the different processes affected by meteorological conditions.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472,Short summary
This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
Wei Yuan, Ru-Jin Huang, Lu Yang, Jie Guo, Ziyi Chen, Jing Duan, Ting Wang, Haiyan Ni, Yongming Han, Yongjie Li, Qi Chen, Yang Chen, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 20, 5129–5144,Short summary
We characterized light-absorbing properties, chromophore composition and sources of brown carbon (BrC) in Xi'an; identified three groups of light-absorbing organics; and quantified their contribution to overall BrC absorption. Our results showed that vehicle emissions and secondary formation are major sources of BrC in spring, coal combustion and vehicle emissions are major sources in fall, biomass burning and coal combustion become major sources in winter, and secondary BrC dominates in summer.
Stefano Decesari, Marco Paglione, Matteo Rinaldi, Manuel Dall'Osto, Rafel Simó, Nicola Zanca, Francesca Volpi, Maria Cristina Facchini, Thorsten Hoffmann, Sven Götz, Christopher Johannes Kampf, Colin O'Dowd, Darius Ceburnis, Jurgita Ovadnevaite, and Emilio Tagliavini
Atmos. Chem. Phys., 20, 4193–4207,Short summary
Atmospheric aerosols in Antarctica contribute to regulate the delicate budget of cloud formation and precipitations. Besides the well-known biogenic production of sulfur-containing aerosol components such as methanesulfonate (MSA), the assessment of biological sources of organic particles in Antarctica remains an active area of research. Here we present the results of aerosol organic characterization during a research cruise performed in the Weddell Sea and in the Southern Ocean in Jan–Feb 2015.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807,Short summary
We characterized secondary aerosol formation in Beijing. Our results showed that relative humidity (RH) and Ox have opposite effects on sulfate and nitrate formation in summer and winter. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC). Meanwhile, the dependence of less-oxidized OOA (LO-OOA) and the mass ratio of LO-OOA to MO-OOA in Ox both degraded when RH > 60 %, suggesting that RH or ALWC may also affect LO-OOA formation.
Wei Xu, Jurgita Ovadnevaite, Kirsten N. Fossum, Chunshui Lin, Ru-Jin Huang, Colin O'Dowd, and Darius Ceburnis
Atmos. Chem. Phys., 20, 3777–3791,Short summary
A humidified tandem differential mobility analyser (HTDMA) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were simultaneously deployed during winter at Mace Head observatory to characterise the hygroscopicity of marine aerosols and their link to chemical composition. Good agreement was generally found between measured and estimated growth factors. A significant degree of external mixing was found in all air masses manifesting primary and secondary sources.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Jie Guo, Haoyue Deng, and Ulrike Dusek
Atmos. Chem. Phys., 19, 15609–15628,Short summary
We present a 1-year source apportionment record of carbonaceous aerosols in Xi'an, China. Biomass burning strongly increases in winter, while seasonal changes of coal and liquid fossil fuel combustion are moderate. We find strong evidence for fossil secondary OC formation during the warm period that is further enhanced in stagnant, polluted conditions due to longer atmospheric residence times. At the same time we find that water-insoluble (primary) fossil is lost due to photochemical processing.
Jun Zhou, Miriam Elser, Ru-Jin Huang, Manuel Krapf, Roman Fröhlich, Deepika Bhattu, Giulia Stefenelli, Peter Zotter, Emily A. Bruns, Simone M. Pieber, Haiyan Ni, Qiyuan Wang, Yichen Wang, Yaqing Zhou, Chunying Chen, Mao Xiao, Jay G. Slowik, Samuel Brown, Laure-Estelle Cassagnes, Kaspar R. Daellenbach, Thomas Nussbaumer, Marianne Geiser, André S. H. Prévôt, Imad El-Haddad, Junji Cao, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 19, 14703–14720,Short summary
Reactive oxygen species (ROS) are believed to contribute to the adverse health effects of aerosols. We measured particle-bound ROS (PB-ROS) with an online instrument in two distinct environments, i.e., Beijing (China) and Bern (Switzerland). In both cities these exogenic ROS are predominantly related to secondary organic aerosol (SOA). PB-ROS content in SOA from various anthropogenic emission sources tested in the laboratory was comparable to that in the ambient measurements.
Chunshui Lin, Darius Ceburnis, Ru-Jin Huang, Wei Xu, Teresa Spohn, Damien Martin, Paul Buckley, John Wenger, Stig Hellebust, Matteo Rinaldi, Maria Cristina Facchini, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 19, 14091–14106,Short summary
To gain insight into the spatial and chemical variation in submicron aerosol, a nationwide characterization of wintertime PM1 was performed at four representative sites across Ireland. This nationwide source apportionment study highlights the large contribution of residential solid fuel burning to urban air pollution and has significant implications for aerosol regional-transport models.
Meng Wang, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Chunshui Lin, Haiyan Ni, Jing Duan, Ting Wang, Yang Chen, Yongjie Li, Qi Chen, Imad El Haddad, and Thorsten Hoffmann
Atmos. Meas. Tech., 12, 4779–4789,Short summary
The analytical performances of SE-GC-MS and TD-GC-MS for the determination of n-alkanes, PAHs and hopanes were evaluated and compared. The two methods show a good agreement with a high correlation efficient (R2 > 0.98) and a slope close to unity. The concentrations of n-alkanes, PAHs and hopanes are found to be much higher in Beijing than those in Chengdu, Shanghai and Guangzhou, most likely due to emissions from coal combustion for wintertime heating in Beijing.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Haoyue Deng, Anita Aerts-Bijma, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 19, 10405–10422,Short summary
We apply radiocarbon source apportionment of more volatile organic carbon (mvOC) to winter aerosol samples from six Chinese cities. We find a consistently larger contribution of fossil sources to mvOC than to secondary or total organic carbon. Fossil mvOC concentrations are strongly correlated with primary fossil OC but not with secondary fossil OC. The variability in nonfossil mvOC seems to be related to both primary and secondary biomass burning sources.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334,Short summary
We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Yunfei Wu, Yunjie Xia, Rujin Huang, Zhaoze Deng, Ping Tian, Xiangao Xia, and Renjian Zhang
Atmos. Meas. Tech., 12, 4347–4359,Short summary
The morphology and effective density of externally mixed black carbon (extBC) aerosols were studied using a tandem technique coupling a DMA with a SP2. The study extended the mass–mobility relationship to large extBC with a mobility diameter larger than 350 nm, a size range seldom included in previous tandem measurements of BC aggregates. On this basis, quantities such as the mass–mobility scaling exponent were revealed for extBC in urban Beijing.
Kun Li, Junling Li, Shengrui Tong, Weigang Wang, Ru-Jin Huang, and Maofa Ge
Atmos. Chem. Phys., 19, 8021–8036,Short summary
Wintertime volatile organic compounds (VOCs) in suburban and urban Beijing were measured. Urban VOC concentrations were much higher than suburban ones, but the emission features were similar. The photochemical processes were more active in the urban site, resulting in the high daytime formation of oxygenated VOCs. In addition, human activities during holidays can largely influence the VOC levels. These results are helpful in better understanding the atmospheric chemistry of VOCs in Beijing.
Inken Heidke, Denis Scholz, and Thorsten Hoffmann
Clim. Past, 15, 1025–1037,Short summary
This is the first quantitative study of lignin biomarkers in stalagmites and cave drip water. Lignin is only produced by higher plants; therefore, its analysis can be used to reconstruct the vegetation of the past. We compared our lignin results with stable isotope and trace element records from the same samples and found correlations or similarities with P, Ba, U and Mg concentrations as well as δ13C values. These results can help to better interpret other vegetation proxies.
Yang Chen, Mi Tian, Ru-Jin Huang, Guangming Shi, Huanbo Wang, Chao Peng, Junji Cao, Qiyuan Wang, Shumin Zhang, Dongmei Guo, Leiming Zhang, and Fumo Yang
Atmos. Chem. Phys., 19, 3245–3255,Short summary
Amine-containing particles were characterized in an urban area of Chongqing during both summer and winter using a single-particle aerosol mass spectrometer (SPAMS). Amines were observed to internally mix with elemental carbon (EC), organic carbon (OC), sulfate, and nitrate. Diethylamine (DEA) was the most abundant in both number and peak area among amine-containing particles. Vegetation and traffic were the primary sources of particulate amines.
Li Xing, Jiarui Wu, Miriam Elser, Shengrui Tong, Suixin Liu, Xia Li, Lang Liu, Junji Cao, Jiamao Zhou, Imad El-Haddad, Rujin Huang, Maofa Ge, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 19, 2343–2359,Short summary
We used the WRF-CHEM model to simulate wintertime secondary organic aerosol (SOA) concentrations over Beijing–Tianjin–Hebei (BTH), China. Heterogeneous HONO sources increased the near-surface SOA by 46.3 % in BTH. Direct emissions of glyoxal and methylglyoxal from residential sources contributed 25.5 % to the total SOA mass. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation in winter over BTH.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298,Short summary
We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Mingjin Tang, Wenjun Gu, Qingxin Ma, Yong Jie Li, Cheng Zhong, Sheng Li, Xin Yin, Ru-Jin Huang, Hong He, and Xinming Wang
Atmos. Chem. Phys., 19, 2247–2258,
Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232,Short summary
VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Weiguo Liu, Ting Zhang, Meng Wang, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 18, 16363–16383,Short summary
Seasonal changes in organic carbon (OC) and elemental carbon (EC) sources in Xi'an, China, are investigated based on measurements of radiocarbon and the stable isotope 13C. Relative contributions to EC from biomass burning, coal combustion, and vehicle emissions change substantially between different seasons. Biomass burning contributes 60 % to the EC increment in winter. Comparing concentrations and sources of primary OC to total OC suggests non-negligible OC loss due to active photochemistry.
Inken Heidke, Denis Scholz, and Thorsten Hoffmann
Biogeosciences, 15, 5831–5845,Short summary
We developed a sensitive method to analyze the lignin composition of organic traces contained in speleothems. Lignin is a main constituent of woody plants and its composition contains information about the type of vegetation. This method offers new possibilities to reconstruct the vegetation of past millennia since it combines the advantages of lignin analysis as a highly specific vegetation biomarker with the benefits of speleothems as unique terrestrial climate archives.
Jorge Saturno, Bruna A. Holanda, Christopher Pöhlker, Florian Ditas, Qiaoqiao Wang, Daniel Moran-Zuloaga, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Jeannine Ditas, Thorsten Hoffmann, Isabella Hrabe de Angelis, Tobias Könemann, Jošt V. Lavrič, Nan Ma, Jing Ming, Hauke Paulsen, Mira L. Pöhlker, Luciana V. Rizzo, Patrick Schlag, Hang Su, David Walter, Stefan Wolff, Yuxuan Zhang, Paulo Artaxo, Ulrich Pöschl, and Meinrat O. Andreae
Atmos. Chem. Phys., 18, 12817–12843,Short summary
Biomass burning emits light-absorbing aerosol particles that warm the atmosphere. One of them is the primarily emitted black carbon, which strongly absorbs radiation in the visible and UV spectral regions. Another one is the so-called brown carbon, a fraction of organic aerosol particles that are able to absorb radiation, especially in the UV spectral region. The contribution of both kinds of aerosol particles to light absorption over the Amazon rainforest is studied in this paper.
Sarah S. Steimer, Aurélie Delvaux, Steven J. Campbell, Peter J. Gallimore, Peter Grice, Duncan J. Howe, Dominik Pitton, Magda Claeys, Thorsten Hoffmann, and Markus Kalberer
Atmos. Chem. Phys., 18, 10973–10983,Short summary
Aerosol particles are a major public health concern, but particle properties contributing to their toxicity are not well known. Oxidising components such as peroxy acids might contribute significantly to particle toxicity. However, there is a lack of analytical methods for their characterisation. We synthesized three peroxy acids, developed an analysis method and showed that degradation affects peracid yield, likely leading to underestimation of their concentration in conventional analyses.
Xia Li, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Rujin Huang, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 18, 10675–10691,
Ru-Jin Huang, Junji Cao, Yang Chen, Lu Yang, Jincan Shen, Qihua You, Kai Wang, Chunshui Lin, Wei Xu, Bo Gao, Yongjie Li, Qi Chen, Thorsten Hoffmann, Colin D. O'Dowd, Merete Bilde, and Marianne Glasius
Atmos. Meas. Tech., 11, 3447–3456,
Doğuşhan Kılıç, Imad El Haddad, Benjamin T. Brem, Emily Bruns, Carlo Bozetti, Joel Corbin, Lukas Durdina, Ru-Jin Huang, Jianhui Jiang, Felix Klein, Avi Lavi, Simone M. Pieber, Theo Rindlisbacher, Yinon Rudich, Jay G. Slowik, Jing Wang, Urs Baltensperger, and Andre S. H. Prévôt
Atmos. Chem. Phys., 18, 7379–7391,Short summary
We study primary emissions and secondary aerosol (SA) from an aircraft turbofan. By monitoring the chemical composition of both gaseous and particulate emissions at different engine loads, we explained SA formed in an oxidation flow reactor (PAM) by the oxidation of gaseous species. At idle, more than 90 % of the secondary particle mass was organic and could be explained by the oxidation of gaseous aromatic species, while at an approximated cruise load sulfates comprised 85 % of the total SA.
Julian Rüdiger, Jan-Lukas Tirpitz, J. Maarten de Moor, Nicole Bobrowski, Alexandra Gutmann, Marco Liuzzo, Martha Ibarra, and Thorsten Hoffmann
Atmos. Meas. Tech., 11, 2441–2457,Short summary
Volcanic gas emission studies are important for monitoring active volcanoes, obtaining insights into subsurface processes and opening up an interesting domain for atmospheric chemistry investigations. Using an unmanned aerial vehicle, commonly called a drone, we were able to study various volcanic gases at sites which are typically too dangerous to access otherwise. The use of drones for volcano monitoring and gas measurements in harsh environments was successfully assessed.
Yan-Lin Zhang, Imad El-Haddad, Ru-Jin Huang, Kin-Fai Ho, Jun-Ji Cao, Yongming Han, Peter Zotter, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Gary Salazar, André S. H. Prévôt, and Sönke Szidat
Atmos. Chem. Phys., 18, 4005–4017,Short summary
Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time of flight aerosol mass spectrometer measurements. We demonstrate a dominant contribution of non-fossil emissions to WSOC aerosols in the Northern Hemisphere. However, the fossil fraction is substantially larger in aerosols from East Asia and the east Asian pollution outflow, especially during winter, due to increasing coal combustion.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815,Short summary
Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813,Short summary
The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Naifang Bei, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Xia Li, Rujin Huang, Zhengqiang Li, Xin Long, Li Xing, Shuyu Zhao, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 17, 14579–14591,
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss.,
Revised manuscript not acceptedShort summary
Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833,Short summary
In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Yunfei Wu, Xiaojia Wang, Jun Tao, Rujin Huang, Ping Tian, Junji Cao, Leiming Zhang, Kin-Fai Ho, Zhiwei Han, and Renjian Zhang
Atmos. Chem. Phys., 17, 7965–7975,Short summary
As black carbon (BC) aerosols play an important role in the climate and environment, the size distribution of refractory BC (rBC) was investigated. On this basis, the source of rBC was further analyzed. The local traffic exhausts contributed greatly to the rBC in urban areas. However, its contribution decreased significantly in the polluted period compared to the clean period, implying the increasing contribution of other sources, e.g., coal combustion or biomass burning, in the polluted period.
Guohui Li, Naifang Bei, Junji Cao, Rujin Huang, Jiarui Wu, Tian Feng, Yichen Wang, Suixin Liu, Qiang Zhang, Xuexi Tie, and Luisa T. Molina
Atmos. Chem. Phys., 17, 3301–3316,
Jiarui Wu, Guohui Li, Junji Cao, Naifang Bei, Yichen Wang, Tian Feng, Rujin Huang, Suixin Liu, Qiang Zhang, and Xuexi Tie
Atmos. Chem. Phys., 17, 2035–2051,
Martin Brüggemann, Laurent Poulain, Andreas Held, Torsten Stelzer, Christoph Zuth, Stefanie Richters, Anke Mutzel, Dominik van Pinxteren, Yoshiteru Iinuma, Sarmite Katkevica, René Rabe, Hartmut Herrmann, and Thorsten Hoffmann
Atmos. Chem. Phys., 17, 1453–1469,Short summary
Using complementary mass spectrometric techniques during a field study in central Europe, characteristic contributors to the organic aerosol mass were identified. Besides common marker compounds for biogenic secondary organic aerosol, highly oxidized sulfur species were detected in the particle phase. High-time-resolution measurements revealed correlations between these organosulfates and particulate sulfate as well as gas-phase peroxyradicals, giving hints to underlying formation mechanisms.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493,Short summary
There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
Stephen J. Andrews, Lucy J. Carpenter, Eric C. Apel, Elliot Atlas, Valeria Donets, James R. Hopkins, Rebecca S. Hornbrook, Alastair C. Lewis, Richard T. Lidster, Richard Lueb, Jamie Minaeian, Maria Navarro, Shalini Punjabi, Daniel Riemer, and Sue Schauffler
Atmos. Meas. Tech., 9, 5213–5225,Short summary
We present a comparison of aircraft measurements of important trace gases from a co-ordinated campaign in Jan–Feb 2014 in the tropical west Pacific involving the NASA Global Hawk, NCAR GV and FAAM BAe-146 aircraft. The paper studies the comparability of separate measurements across platforms and demonstrates that aircraft measurements are relevant for characterising the vertical uplift of important gases, such as those with ozone-depleting potential, to the upper troposphere–lower stratosphere.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271,Short summary
We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Guo Li, Hang Su, Xin Li, Uwe Kuhn, Hannah Meusel, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Yafang Cheng
Atmos. Chem. Phys., 16, 10299–10311,Short summary
Indoor and outdoor formaldehyde (HCHO) are both of considerable concern because of its health effects and its role in atmospheric chemistry. The heterogeneous reactions between gaseous HCHO with soils can pose important impact on both HCHO budget and soil ecosystem. Our results confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions. Soil and soil-derived airborne particles can either act as a source or a sink for HCHO.
Tian Feng, Guohui Li, Junji Cao, Naifang Bei, Zhenxing Shen, Weijian Zhou, Suixin Liu, Ting Zhang, Yichen Wang, Ru-jin Huang, Xuexi Tie, and Luisa T. Molina
Atmos. Chem. Phys., 16, 10045–10061,Short summary
The springtime organic aerosol (OA) concentrations in the Guanzhong Basin, China are simulated using the WRF-Chem model with two secondary OA (SOA) modules. Model results are verified with near-surface observations. The non-traditional SOA module significantly improves SOA simulation. Oxidation and partitioning of primary OAs is the most important pathway in SOA formation. Residential emissions are the dominant anthropogenic OA source.
Xin Long, Xuexi Tie, Junji Cao, Rujin Huang, Tian Feng, Nan Li, Suyu Zhao, Jie Tian, Guohui Li, and Qiang Zhang
Atmos. Chem. Phys., 16, 9675–9691,Short summary
We studied the impact of crop field burning (CFB) on air pollution in North China Plain (NCP) using MODIS observations and the numerical model WRF-CHEM. The CFB plume emitted in southern NCP and went through a long-range transport to northern NCP. The long-range transport and the effect of mountains obviously enhanced the PM2.5 pollution in northern NCP. The prohibition of CFB should be strict not just in or around Beijing, but also on the ulterior crop growth areas of southern NCP.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187,
Naifang Bei, Guohui Li, Ru-Jin Huang, Junji Cao, Ning Meng, Tian Feng, Suixin Liu, Ting Zhang, Qiang Zhang, and Luisa T. Molina
Atmos. Chem. Phys., 16, 7373–7387,Short summary
Rapid industrialization and urbanization have caused severe air pollution in the Guanzhong basin, northwestern China with heavy haze events occurring frequently in recent winters. Due to frequent occurrence of unfavorable synoptic situations during wintertime, mitigation of emissions is the optimum approach to mitigate the air pollution in the Guanzhong basin.
Chris Reed, Charlotte A. Brumby, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Paul W. Seakins, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 9, 2483–2495,Short summary
A new method of measuring nitrous acid (HONO), a potent mediator of air quality in the atmosphere as well as an important indoor pollutant, is presented. The new method relies on simple, proven techniques already widely applied to other atmospheric compounds. The technique can be retrofitted to existing analysers at minimal cost, or developed into instruments capable of very fast measurement which allow for more complex analysis of the behaviour of HONO.
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724,Short summary
The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Tian Feng, Naifang Bei, Ru-Jin Huang, Junji Cao, Qiang Zhang, Weijian Zhou, Xuexi Tie, Suixin Liu, Ting Zhang, Xiaoli Su, Wenfang Lei, Luisa T. Molina, and Guohui Li
Atmos. Chem. Phys., 16, 4323–4342,Short summary
The occurrence of high O3 levels with high PM2.5 concentrations constitutes a dilemma for the design of O3 control strategies in Xi’an and surrounding areas. If the O3 mitigation approach decreases aerosols in the atmosphere directly or indirectly, the enhanced photolysis caused by aerosol reduction would compensate for the O3 loss. If only the PM2.5 control strategy is implemented, the O3 pollution will decrease.
Miriam Elser, Ru-Jin Huang, Robert Wolf, Jay G. Slowik, Qiyuan Wang, Francesco Canonaco, Guohui Li, Carlo Bozzetti, Kaspar R. Daellenbach, Yu Huang, Renjian Zhang, Zhengqiang Li, Junji Cao, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 3207–3225,Short summary
This work represents the first online chemical characterization of the PM2.5 using a high-resolution time-of flight aerosol mass spectrometer during extreme haze events China. The application of novel source apportionment techniques allowed for an improved identification and quantification of the sources of organic aerosols. The main sources and processes driving the extreme haze events are assessed.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186,Short summary
Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
K. R. Daellenbach, C. Bozzetti, A. Křepelová, F. Canonaco, R. Wolf, P. Zotter, P. Fermo, M. Crippa, J. G. Slowik, Y. Sosedova, Y. Zhang, R.-J. Huang, L. Poulain, S. Szidat, U. Baltensperger, I. El Haddad, and A. S. H. Prévôt
Atmos. Meas. Tech., 9, 23–39,Short summary
In this study, we developed an offline technique using the AMS for the characterization of the chemical fingerprints of aerosols collected on quartz filters, and evaluated the suitability of the organic mass spectral data for source apportionment. This technique may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.
Q. Y. Wang, R.-J. Huang, J. J. Cao, X. X. Tie, H. Y. Ni, Y. Q. Zhou, Y. M. Han, T. F. Hu, C. S. Zhu, T. Feng, N. Li, and J. D. Li
Atmos. Chem. Phys., 15, 13059–13069,Short summary
An intensive campaign was conducted at the Qinghai-Tibetan Plateau using a ground-based single particle soot photometer and a photoacoustic extinctiometer. Significant enhancements of rBC loadings and number fraction of coated rBC were observed during the pollution episode. Biomass burning from N. India is determined to be an important potential source influencing the northeastern Qinghai-Tibetan Plateau. The rBC mixing state is important in determining absorption during the pollution episode.
A. Saiz-Lopez, C. S. Blaszczak-Boxe, and L. J. Carpenter
Atmos. Chem. Phys., 15, 9731–9746,
J. D. Allan, P. I. Williams, J. Najera, J. D. Whitehead, M. J. Flynn, J. W. Taylor, D. Liu, E. Darbyshire, L. J. Carpenter, R. Chance, S. J. Andrews, S. C. Hackenberg, and G. McFiggans
Atmos. Chem. Phys., 15, 5599–5609,Short summary
New particle formation (NPF) is an important contributor to aerosol number concentrations in the Arctic and thus has a major role in dictating cloud properties and climate in this region. Here we present direct evidence that the oxidation of iodine in the atmosphere causes NPF in the Greenland Sea. This is important because this is a NPF mechanism that has not previously been considered in modelling studies at these latitudes.
S. J. Andrews, S. C. Hackenberg, and L. J. Carpenter
Ocean Sci., 11, 313–321,Short summary
The oceans are a key source of a number of atmospherically important volatile gases. The accurate and robust determination of trace gases in seawater is a significant analytical challenge. Here we describe a gas chromatograph mass spectrometer based purge and trap system that was developed for the fully automated analysis of dissolved very short-lived species (VSLS) in seawater sampled from a research ship.
K. F. Ho, R.-J. Huang, K. Kawamura, E. Tachibana, S. C. Lee, S. S. H. Ho, T. Zhu, and L. Tian
Atmos. Chem. Phys., 15, 3111–3123,Short summary
The objective of this study is to identify the influence of traffic emissions and regional transport to the atmosphere in Beijing during the CAREBeijing-2007 in summer. This study demonstrates that even when primary exhaust was controlled by traffic restrictions, the contribution of secondary organic species formed from photochemical processes was critical with long-range atmospheric transport of pollutants.
Y.-L. Zhang, R.-J. Huang, I. El Haddad, K.-F. Ho, J.-J. Cao, Y. Han, P. Zotter, C. Bozzetti, K. R. Daellenbach, F. Canonaco, J. G. Slowik, G. Salazar, M. Schwikowski, J. Schnelle-Kreis, G. Abbaszade, R. Zimmermann, U. Baltensperger, A. S. H. Prévôt, and S. Szidat
Atmos. Chem. Phys., 15, 1299–1312,Short summary
Source apportionment of fine carbonaceous aerosols using radiocarbon and other organic markers measurements during 2013 winter haze episodes was conducted at four megacities in China. Our results demonstrate that fossil emissions predominate EC with a mean contribution of 75±8%, whereas non-fossil sources account for 55±10% of OC; and the increment of TC on heavily polluted days was mainly driven by the increase of secondary OC from both fossil-fuel and non-fossil emissions.
R. Oswald, M. Ermel, K. Hens, A. Novelli, H. G. Ouwersloot, P. Paasonen, T. Petäjä, M. Sipilä, P. Keronen, J. Bäck, R. Königstedt, Z. Hosaynali Beygi, H. Fischer, B. Bohn, D. Kubistin, H. Harder, M. Martinez, J. Williams, T. Hoffmann, I. Trebs, and M. Sörgel
Atmos. Chem. Phys., 15, 799–813,Short summary
Nitrous acid (HONO) is a key species in atmospheric photochemistry since the photolysis leads to the important hydroxyl radical (OH). Although the importance of HONO as a precursor of OH is known, the formation pathways of HONO, especially during daytime, are a major challenge in atmospheric science. We present a detailed analysis of sources and sinks for HONO in the atmosphere for a field measurement campaign in the boreal forest in Finland and wonder if there is really a source term missing.
P. Zotter, V. G. Ciobanu, Y. L. Zhang, I. El-Haddad, M. Macchia, K. R. Daellenbach, G. A. Salazar, R.-J. Huang, L. Wacker, C. Hueglin, A. Piazzalunga, P. Fermo, M. Schwikowski, U. Baltensperger, S. Szidat, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 13551–13570,
R.-J. Huang, W.-B. Li, Y.-R. Wang, Q. Y. Wang, W. T. Jia, K.-F. Ho, J. J. Cao, G. H. Wang, X. Chen, I. EI Haddad, Z. X. Zhuang, X. R. Wang, A. S. H. Prévôt, C. D. O'Dowd, and T. Hoffmann
Atmos. Meas. Tech., 7, 2027–2035,
S. M. MacDonald, J. C. Gómez Martín, R. Chance, S. Warriner, A. Saiz-Lopez, L. J. Carpenter, and J. M. C. Plane
Atmos. Chem. Phys., 14, 5841–5852,
J. Wildt, T. F. Mentel, A. Kiendler-Scharr, T. Hoffmann, S. Andres, M. Ehn, E. Kleist, P. Müsgen, F. Rohrer, Y. Rudich, M. Springer, R. Tillmann, and A. Wahner
Atmos. Chem. Phys., 14, 2789–2804,
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321,
F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi
Atmos. Chem. Phys., 13, 8915–8934,
R.-J. Huang, U. R. Thorenz, M. Kundel, D. S. Venables, D. Ceburnis, K. F. Ho, J. Chen, A. L. Vogel, F. C. Küpper, P. P. A. Smyth, U. Nitschke, D. B. Stengel, H. Berresheim, C. D. O'Dowd, and T. Hoffmann
Atmos. Chem. Phys., 13, 5255–5264,
A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867,
Related subject area
Subject: Gases | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Atmospheric photooxidation and ozonolysis of Δ3-carene and 3-caronaldehyde: rate constants and product yieldsMeasurement report: Biogenic volatile organic compound emission profiles of rapeseed leaf litter and its secondary organic aerosol formation potentialHighly oxygenated organic molecules produced by the oxidation of benzene and toluene in a wide range of OH exposure and NOx conditionsMolecular composition and volatility of multi-generation products formed from isoprene oxidation by nitrate radicalHighly oxygenated organic molecule (HOM) formation in the isoprene oxidation by NO3 radicalAtmospheric oxidation of α,β-unsaturated ketones: kinetics and mechanism of the OH radical reactionCharacterization of ambient volatile organic compounds, source apportionment, and the ozone-NOx-VOC sensitivities in a heavily polluted megacity of central China: Effect of sporting events and the emission reductionsReactions of NO3 with Aromatic Aldehydes: Gas Phase Kinetics and Insights into the Mechanism of the ReactionVolatile organic compound emissions from solvent- and water-borne coatings – compositional differences and tracer compound identificationsEvaluated kinetic and photochemical data for atmospheric chemistry: volume VIII – gas-phase reactions of organic species with four, or more, carbon atoms ( ≥ C4)Chemical characterisation of benzene oxidation products under high- and low-NOx conditions using chemical ionisation mass spectrometryEmissions of non-methane volatile organic compounds from combustion of domestic fuels in Delhi, IndiaA comparative and experimental study of the reactivity with nitrate radical of two terpenes: α-terpinene and γ-terpinenePhotooxidation of pinonaldehyde at ambient conditions investigated in the atmospheric simulation chamber SAPHIRReaction between CH3C(O)OOH (peracetic acid) and OH in the gas phase: a combined experimental and theoretical study of the kinetics and mechanismSnow heterogeneous reactivity of bromide with ozone lost during snow metamorphismEvaluated kinetic and photochemical data for atmospheric chemistry: Volume VII – Criegee intermediatesTechnical Note: Effect of varying the λ = 185 and 254 nm photon flux ratio on radical generation in oxidation flow reactorsKinetics of dimethyl sulfide (DMS) reactions with isoprene-derived Criegee intermediates studied with direct UV absorptionDetermination of the absorption cross sections of higher-order iodine oxides at 355 and 532 nmEvolution of NO3 reactivity during the oxidation of isopreneRate coefficients for reactions of OH with aromatic and aliphatic volatile organic compounds determined by the multivariate relative rate techniqueAtmospheric fate of two relevant unsaturated ketoethers: kinetics, products and mechanisms for the reaction of hydroxyl radicals with (E)-4-methoxy-3-buten-2-one and (1E)-1-methoxy-2-methyl-1-penten-3-oneThe nitrogen budget of laboratory-simulated western US wildfires during the FIREX 2016 Fire Lab studyImportance of isomerization reactions for OH radical regeneration from the photo-oxidation of isoprene investigated in the atmospheric simulation chamber SAPHIRKinetics of the OH + NO2 reaction: effect of water vapour and new parameterization for global modellingKinetic and mechanistic study of the reaction between methane sulfonamide (CH3S(O)2NH2) and OHDimensionality-reduction techniques for complex mass spectrometric datasets: application to laboratory atmospheric organic oxidation experimentsAtmospheric fate of a series of saturated alcohols: kinetic and mechanistic studyMulti-generation OH oxidation as a source for highly oxygenated organic molecules from aromaticsPhotolysis and oxidation by OH radicals of two carbonyl nitrates: 4-nitrooxy-2-butanone and 5-nitrooxy-2-pentanonePotential dual effect of anthropogenic emissions on the formation of biogenic secondary organic aerosol (BSOA)Effect of NOx on 1,3,5-trimethylbenzene (TMB) oxidation product distribution and particle formationMechanistic study of the formation of ring-retaining and ring-opening products from the oxidation of aromatic compounds under urban atmospheric conditionsOH chemistry of non-methane organic gases (NMOGs) emitted from laboratory and ambient biomass burning smoke: evaluating the influence of furans and oxygenated aromatics on ozone and secondary NMOG formationSecondary organic aerosol formation from photooxidation of furan: effects of NOx and humidityCarboxylic acids from limonene oxidation by ozone and hydroxyl radicals: insights into mechanisms derived using a FIGAERO-CIMSTrapping of HCl and oxidised organic trace gases in growing ice at temperatures relevant to cirrus cloudsInvestigation of the α-pinene photooxidation by OH in the atmospheric simulation chamber SAPHIRChamber-based insights into the factors controlling epoxydiol (IEPOX) secondary organic aerosol (SOA) yield, composition, and volatilityKinetics of the OH + NO2 reaction: rate coefficients (217–333 K, 16–1200 mbar) and fall-off parameters for N2 and O2 bath gasesTrends in N2O and SF6 mole fractions in archived air samples from Cape Meares, Oregon (USA), 1978–1996Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysispH-dependent production of molecular chlorine, bromine, and iodine from frozen saline surfacesSolubility and solution-phase chemistry of isocyanic acid, methyl isocyanate, and cyanogen halidesROOOH: a missing piece of the puzzle for OH measurements in low-NO environments?Measurements of I/SVOCs in biomass-burning smoke using solid-phase extraction disks and two-dimensional gas chromatographyPrimary emissions of glyoxal and methylglyoxal from laboratory measurements of open biomass burningReactive quenching of electronically excited NO2∗ and NO3∗ by H2O as potential sources of atmospheric HOx radicalsEvaluation of OH and HO2 concentrations and their budgets during photooxidation of 2-methyl-3-butene-2-ol (MBO) in the atmospheric simulation chamber SAPHIR
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,Short summary
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.
Letizia Abis, Carmen Kalalian, Bastien Lunardelli, Tao Wang, Liwu Zhang, Jianmin Chen, Sébastien Perrier, Benjamin Loubet, Raluca Ciuraru, and Christian George
Atmos. Chem. Phys., 21, 12613–12629,Short summary
Biogenic volatile organic compound (BVOC) emissions from rapeseed leaf litter have been investigated by means of a controlled atmospheric simulation chamber. The diversity of emitted VOCs increased also in the presence of UV light irradiation. SOA formation was observed when leaf litter was exposed to both UV light and ozone, indicating a potential contribution to particle formation or growth at local scales.
Xi Cheng, Qi Chen, Yong Jie Li, Yan Zheng, Keren Liao, and Guancong Huang
Atmos. Chem. Phys., 21, 12005–12019,Short summary
In this study, we conducted laboratory studies to investigate the formation of gas-phase highly oxygenated organic molecules (HOMs). We provide a thorough analysis on the importance of multistep auto-oxidation and multigeneration OH reactions. We also give an intensive investigation on the roles of high-NO2 conditions that represent a wide range of anthropogenically influenced environments.
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,Short summary
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.
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,Short summary
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.
Niklas Illmann, Rodrigo Gastón Gibilisco, Iustinian Gabriel Bejan, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Within this work we determined the rate coefficients and products of the reaction of unsaturated ketones with OH radicals in an effort to complete the gaps in the knowledge needed for modelling chemistry in the atmosphere. Both substances are potentially emitted by biomass burning, industrial activities or formed in the troposphere by oxidation of terpenes. As products we identified aldehydes and ketones which in turn are known to be responsible for the transportation of NOx species.
Shijie Yu, Fangcheng Su, Shasha Yin, Shenbo Wang, Ruixin Xu, Bing He, Xiangge Fan, Minghao Yuan, and Ruiqin Zhang
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study measured 106 VOC species using GC-MS/FID. Meanwhile, the WRF/CMAQ models were used to investigate the nonlinearity of O3 response to precursor reductions. This study highlights the effectiveness of stringent emission controls in relation to solvent utilization and coal combustion. However, unreasonable emission reduction may aggravate ozone pollution during control periods. It is suggested that emission reduction ratios of the precursors (VOC : NOx) should be more than 2.
Yangang Ren, Li Zhou, Abdelwahid Mellouki, Véronique Daële, Mahmoud Idir, Steven S. Brown, Branko Ruscic, Robert S. Paton, Max R. McGillen, and Akkihebbal R. Ravishankara
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Aromatic aldehydes are a family of compounds emitted into the atmosphere from both anthropogenic and biogenic sources and also formed from the degradation of aromatic hydrocarbons. Their atmospheric degradation may impact air quality. We report a study on their atmospheric degradation through reaction with NO3 which are useful to estimate their atmospheric lifetimes. We have also attempted to elucidate the mechanism of these reactions via studies of isotopic substitution and quantum chemistry.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022,Short summary
Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808,Short summary
Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
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,Short summary
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.
Gareth J. Stewart, W. Joe F. Acton, Beth S. Nelson, Adam R. Vaughan, James R. Hopkins, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Rachel E. Dunmore, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2383–2406,Short summary
Biomass burning is a major source of trace gases to the troposphere; however, the composition and quantity of emissions vary greatly between different fuel types. This work provided near-total quantitation of non-methane volatile organic compounds from combustion of biofuels from India. Emissions from cow dung cake combustion were significantly larger than conventional fuelwood combustion, potentially indicating that this source has a disproportionately large impact on regional air quality.
Axel Fouqueau, Manuela Cirtog, Mathieu Cazaunau, Edouard Pangui, Jean-François Doussin, and Bénédicte Picquet-Varrault
Atmos. Chem. Phys., 20, 15167–15189,
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,Short summary
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.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555,Short summary
Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
Jacinta Edebeli, Jürg C. Trachsel, Sven E. Avak, Markus Ammann, Martin Schneebeli, Anja Eichler, and Thorsten Bartels-Rausch
Atmos. Chem. Phys., 20, 13443–13454,Short summary
Earth’s snow cover is very dynamic and can change its physical properties within hours, as is well known by skiers. Snow is also a well-known host of chemical reactions – the products of which impact air composition and quality. Here, we present laboratory experiments that show how the dynamics of snow make snow essentially inert with respect to gas-phase ozone with time despite its content of reactive chemicals. Impacts on polar atmospheric chemistry are discussed.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519,Short summary
Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Jake P. Rowe, Andrew T. Lambe, and William H. Brune
Atmos. Chem. Phys., 20, 13417–13424,Short summary
We conducted a series of experiments in which the 185 to 254 nm photon flux ratio (I185 : I254) emitted by low-pressure mercury lamps installed in an oxidation flow reactor (OFR) was systematically varied using multiple novel lamp configurations. Integrated OH exposure values achieved for each lamp type were obtained as a function of OFR operating conditions. A photochemical box model was used to develop a generalized OH exposure estimation equation as a function of [H2O], [O3], and OH reactivity.
Mei-Tsan Kuo, Isabelle Weber, Christa Fittschen, Luc Vereecken, and Jim Jr-Min Lin
Atmos. Chem. Phys., 20, 12983–12993,Short summary
Dimethyl sulfide (DMS) is the major sulfur-containing species in the troposphere. Previous work by Newland et al. (2015) reported very high reactivity of isoprene-derived Criegee intermediates (CIs) towards DMS. By monitoring CIs with direct UV absorption, we found CI + DMS reactions are very slow, in contrast to the results of Newland et al. (2015), suggesting these CIs would not oxidize atmospheric DMS at any substantial level.
Thomas R. Lewis, Juan Carlos Gómez Martín, Mark A. Blitz, Carlos A. Cuevas, John M. C. Plane, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 10865–10887,Short summary
Iodine-bearing gasses emitted from the sea surface are chemically processed in the atmosphere, leading to iodine accumulation in aerosol and transport to continental ecosystems. Such processing involves light-induced break-up of large, particle-forming iodine oxides into smaller, ozone-depleting molecules. We combine experiments and theory to report the photolysis efficiency of iodine oxides required to assess the impact of iodine on ozone depletion and particle formation.
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,Short summary
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.
Jacob T. Shaw, Andrew R. Rickard, Mike J. Newland, and Terry J. Dillon
Atmos. Chem. Phys., 20, 9725–9736,Short summary
This work expands upon the recently developed multivariate relative rate technique, presented in Shaw et al. (2019), for the measurement of rates of reaction between aromatic and aliphatic volatile organic compounds (VOCs) and OH. Knowledge of the rates of such reactions are important for understanding air quality in urban environments. This work also provides a key validation of structure–activity relationship models, which provide a theoretical method for estimating OH + VOC kinetics.
Rodrigo Gastón Gibilisco, Ian Barnes, Iustinian Gabriel Bejan, and Peter Wiesen
Atmos. Chem. Phys., 20, 8939–8951,Short summary
Environmental chamber studies were performed to evaluate atmospheric degradation initiated by OH radicals for two unsaturated methoxy ketones. The main gas-phase oxidation products identified and quantified from these reactions are carbonyls and long-lived nitrogen-containing compounds such as peroxyacetyl nitrate and peroxypropionyl nitrate. The kinetic rate constants and atmospheric lifetimes were estimated, degradation mechanisms were developed, and atmospheric implications were assessed.
James M. Roberts, Chelsea E. Stockwell, Robert J. Yokelson, Joost de Gouw, Yong Liu, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, Kyle J. Zarzana, Steven S. Brown, Cristina Santin, Stefan H. Doerr, and Carsten Warneke
Atmos. Chem. Phys., 20, 8807–8826,Short summary
We measured total reactive nitrogen, Nr, in lab fires from western North American fuels, along with measurements of individual nitrogen compounds. We measured the amount of N that gets converted to inactive compounds (avg. 70 %), and the amount that is accounted for by individual species (85 % of remaining N). We provide guidelines for how the reactive nitrogen is distributed among individual compounds such as NOx and ammonia. This will help estimates and predictions of wildfire emissions.
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,Short summary
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.
Damien Amedro, Matias Berasategui, Arne J. C. Bunkan, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3091–3105,Short summary
Our laboratory experiments show that the rate coefficient for the termolecular reaction between OH and NO2 is enhanced in the presence of water vapour. Using a chemistry transport model we show that our new parameterization of the temperature, pressure, and bath-gas dependence of this reaction has a significant impact on, for example, NOx and the HNO2 / NO2 ratio when compared to present recommendations.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707,Short summary
We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Abigail R. Koss, Manjula R. Canagaratna, Alexander Zaytsev, Jordan E. Krechmer, Martin Breitenlechner, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joseph R. Roscioli, Frank N. Keutsch, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 1021–1041,Short summary
Oxidation chemistry of organic compounds in the atmosphere produces a diverse spectrum of products. This diversity is difficult to represent in air quality and climate models, and in laboratory experiments it results in large and complex datasets. This work evaluates several methods to simplify the chemistry of oxidation systems in environmental chambers, including positive matrix factorization, hierarchical clustering analysis, and gamma kinetics parameterization.
Inmaculada Colmenar, Pilar Martin, Beatriz Cabañas, Sagrario Salgado, Araceli Tapia, and Inmaculada Aranda
Atmos. Chem. Phys., 20, 699–720,Short summary
Saturated alcohols (SAs), such as (E)-4-methylcyclohexanol, 3,3-dimethyl-1-butanol, and 3,3-dimethyl-2-butanol, could be used as biofuels. The atmospheric reactivity of these compounds must be established in order to understand the consequences of the presence of these compounds in the atmosphere. The experimental results obtained in this work reveal that uncontrolled emissions of these saturated alcohols could have important atmospheric implications.
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,Short summary
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.
Bénédicte Picquet-Varrault, Ricardo Suarez-Bertoa, Marius Duncianu, Mathieu Cazaunau, Edouard Pangui, Marc David, and Jean-François Doussin
Atmos. Chem. Phys., 20, 487–498,Short summary
Multifunctional organic nitrates are important atmospheric species that are known to play a key role in the transport of reactive nitrogen and in aerosol composition. However, very little is known about their atmospheric reactivity. Here we provide an experimental study on the photolysis and reaction of two carbonyl nitrates with OH radicals. Atmospheric implications and the influence of the chemical structure on the reactivity are discussed.
Eetu Kari, Liqing Hao, Arttu Ylisirniö, Angela Buchholz, Ari Leskinen, Pasi Yli-Pirilä, Ilpo Nuutinen, Kari Kuuspalo, Jorma Jokiniemi, Celia L. Faiola, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 15651–15671,Short summary
We present, for the first time, the dual effect of GDI-vehicle exhaust on α-pinene SOA mass yield suppression. The first effect is a well-known NOx effect, but the second effect is more complex. Our results imply that this second effect is related to change of reaction pathways of α-pinene in the presence of GDI exhaust. The presence of vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of GDI emissions.
Epameinondas Tsiligiannis, Julia Hammes, Christian Mark Salvador, Thomas F. Mentel, and Mattias Hallquist
Atmos. Chem. Phys., 19, 15073–15086,Short summary
The role of anthropogenic VOCs (AVOCs) for SOA formation needs to be scrutinised. The aromatic 1,3,5-trimethylbenzene (TMB) was shown to form highly oxygenated organic molecules (HOMs) in NOx-free environments, possibly contributing to new particle formation (NPF). However, formation of HOMs and particles was suppressed in the presence of NOx, while the formation of organonitrates (ONs) was increased. Thus, aromatic AVOCs may not enhance NPF in urban air masses.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129,Short summary
Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899,Short summary
Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Xiaotong Jiang, Narcisse T. Tsona, Long Jia, Shijie Liu, Hailiang Zhang, Yongfu Xu, and Lin Du
Atmos. Chem. Phys., 19, 13591–13609,Short summary
Atmospheric furan is a primary and secondary pollutant in the atmosphere, and its emission contributes to the formation of ultrafine particles and ground-level ozone. The present study demonstrates the effect of NOx and humidity on secondary organic aerosol (SOA) formation during the furan–NOx–NaCl photooxidation. Furthermore, the results illustrate the importance of studying SOA formation over a comprehensive range of environmental conditions.
Julia Hammes, Anna Lutz, Thomas Mentel, Cameron Faxon, and Mattias Hallquist
Atmos. Chem. Phys., 19, 13037–13052,Short summary
Identifying the chemical pathways of condensable products such as carboxylic acids is essential for predicting SOA formation. This identification is inherently difficult, as such products reside in both the gas and particulate phases. We measured acids, produced from atmospheric oxidation of limonene, in both phases and scrutinised the mechanistic understanding of their formation. The mechanisms explain nearly 75 % of the gas-phase signal at the lowest concentration (8.4 ppb, 23 % acid yield).
Matthias Kippenberger, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 11939–11951,Short summary
We investigated the uptake of several trace gases to growing ice surfaces at temperatures relevant to cirrus clouds. HCl, a strong inorganic acid that ionises at the surface, was efficiently trapped in the growing ice, whereas oxidised organic trace gases, which attach to ice by hydrogen bonding, were not. HCl can be efficiently and rapidly removed from the gas phase in supersaturated ice clouds.
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,Short summary
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.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265,Short summary
Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Damien Amedro, Arne J. C. Bunkan, Matias Berasategui, and John N. Crowley
Atmos. Chem. Phys., 19, 10643–10657,Short summary
The reaction between the OH radical and nitrogen dioxide plays a critical role in controlling abundances of HOx and NOx from the boundary layer to the stratosphere. Uncertainties associated with the rate coefficient for this reaction lead to uncertainty in model predictions of the oxidizing capacity of the atmosphere and photochemical ozone production. We present accurate measurements of the rate coefficient over a range of temperatures and pressures.
Terry C. Rolfe and Andrew L. Rice
Atmos. Chem. Phys., 19, 8967–8977,Short summary
We present 159 measurements of the atmospheric mole fraction of nitrous oxide (N2O) and sulfur hexaflouride (SF6) from historic archived air samples collected at Cape Meares, Oregon (USA, 45.5°N, 124.0°W), between 1978 and 1996. These measurements add significantly to the historical record of the atmospheric composition for these important greenhouse gases. Results provide an analysis of the average atmospheric mixing ratio, growth rate, and seasonality for N2O and SF6 at midlatitudes.
Lauriane L. J. Quéléver, Kasper Kristensen, Louise Normann Jensen, Bernadette Rosati, Ricky Teiwes, Kaspar R. Daellenbach, Otso Peräkylä, Pontus Roldin, Rossana Bossi, Henrik B. Pedersen, Marianne Glasius, Merete Bilde, and Mikael Ehn
Atmos. Chem. Phys., 19, 7609–7625,Short summary
Highly oxygenated organic molecules (HOMs) form rapidly in oxidation of monoterpenes and have been shown to be crucial for secondary organic aerosol formation. We studied the formation of HOMs under different temperatures, finding a strong dependence on their yields. As temperatures decrease, the isomerization reactions that allow rapid oxidation by molecular oxygen slow down, and competing reaction pathways can suppress the HOM formation almost completely, especially at high VOC loadings.
John W. Halfacre, Paul B. Shepson, and Kerri A. Pratt
Atmos. Chem. Phys., 19, 4917–4931,Short summary
In this study, we found that a chemical called hydroxyl radical can help create chlorine, bromine, and iodine (i.e., halogens) from acidic frozen imitation seawater. Even more halogens are created if we also add ozone. This result helps our understanding of how halogens are released from the frozen Arctic ice and snow into the atmosphere, where they alter the atmosphere's oxidation ability.
James M. Roberts and Yong Liu
Atmos. Chem. Phys., 19, 4419–4437,Short summary
Condensed-phase reactions are important removal processes for reduced nitrogen species, isocyanic acid (HNCO), methyl isocyanate (CH3NCO), and cyanogen halides (XCN, X = Cl, Br, I). This chemistry is not well understood, so we measured aqueous-phase solubilities and reaction rates under a range of temperatures and conditions and in n-octanol, a proxy for non-polar media and biological membranes. The results were used to estimate atmospheric removal rates and fates of these nitrogen compounds.
Christa Fittschen, Mohamad Al Ajami, Sebastien Batut, Valerio Ferracci, Scott Archer-Nicholls, Alexander T. Archibald, and Coralie Schoemaecker
Atmos. Chem. Phys., 19, 349–362,Short summary
Concentrations of OH, the main oxidant in the atmosphere, were measured in biogenic environments up to a factor of 10 higher than predicted by models. This was interpreted as a major lack in our understanding of biogenic volatile organic compound chemistry. But interferences of unknown origin have also been discovered, and we present experimental and modelling evidence that the interference might be due to the unexpected decomposition of a new class of molecule, ROOOH, in the FAGE instruments.
Lindsay E. Hatch, Albert Rivas-Ubach, Coty N. Jen, Mary Lipton, Allen H. Goldstein, and Kelley C. Barsanti
Atmos. Chem. Phys., 18, 17801–17817,Short summary
We demonstrate the use of solid-phase extraction (SPE) disks for the untargeted analysis of gas-phase intermediate volatility and semi-volatile organic compounds emitted from biomass burning. SPE and Teflon filter samples collected from laboratory fires were analyzed by two-dimensional gas chromatography, with distinct differences in the observed chromatographic profiles as a function of fuel type. Fuel-dependent emissions and volatility differences among benzenediol isomers were captured.
Kyle J. Zarzana, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, William P. Dubé, Robert J. Yokelson, Carsten Warneke, Joost A. de Gouw, James M. Roberts, and Steven S. Brown
Atmos. Chem. Phys., 18, 15451–15470,Short summary
Emissions of glyoxal and methylglyoxal from fuels common to the western United States were measured using cavity-enhanced spectroscopy, which provides a more selective measurement of those compounds than was previously available. Primary emissions of glyoxal were lower than previously reported and showed variability between the different fuel groups. However, emissions of glyoxal relative to formaldehyde were constant across almost all the fuel groups at 6 %–7 %.
Terry J. Dillon and John N. Crowley
Atmos. Chem. Phys., 18, 14005–14015,Short summary
The reactions between electronically excited NO2* and NO3* with water vapour were studied using laser excitation of NO2 (532–647 nm) or NO3 (623–662 nm). No evidence for OH production was observed in either reaction. The reaction of NO2* with water is not a significant source of OH in the atmosphere.
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,Short summary
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.
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Phytoplankton suspensions were treated with high and low ozone levels, and volatile iodine (I2)-containing compounds were measured. Iodocarbon emissions were independent of the ozone level. I2 emission showed a strong dependency on the ozone level in the air as well as on the iodide concentration in the sample suspension. The experiments show that microalgae suspensions are capable of emitting I2 by the reaction of ozone with dissolved iodide at the air-water interface under natural conditions.
Phytoplankton suspensions were treated with high and low ozone levels, and volatile iodine...