Articles | Volume 16, issue 15
Research article 02 Aug 2016
Research article | 02 Aug 2016
Hydroxyl radical in/on illuminated polar snow: formation rates, lifetimes, and steady-state concentrations
Zeyuan Chen et al.
No articles found.
Richie Kaur, Jacqueline R. Labins, Scarlett S. Helbock, Wenqing Jiang, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 19, 6579–6594,Short summary
We measured hydroxyl radical (•OH), singlet oxygen (1O2*), and organic triplets (3C*) in illuminated aqueous particle extracts. After measuring the impact of dilution on oxidant concentrations, we extrapolated our results to predict them in ambient particles – 1O2* and 3C* concentrations appear to be greatly enhanced, while •OH appears largely unchanged. Two of these oxidants (1O2*, 3C*) are not yet included in atmospheric models, and our results make it possible to include them in the future.
Richie Kaur, Brandi M. Hudson, Joseph Draper, Dean J. Tantillo, and Cort Anastasio
Atmos. Chem. Phys., 19, 5021–5032,Short summary
Organic triplets are an important class of aqueous photooxidants, but little is known about their reactions with most atmospheric organic compounds. We measured the reaction rate constants of a model triplet with 17 aliphatic alkenes; using their correlation with oxidation potential, we predicted rate constants for some atmospherically relevant alkenes. Depending on their reactivities, triplets can be minor to important sinks for isoprene- and limonene-derived alkenes in cloud or fog drops.
Ted Hullar and Cort Anastasio
The Cryosphere, 10, 2057–2068,Short summary
We study chemical reactions in snow and ice by freezing solutions in the laboratory. Although it is important to know where these chemicals are in the frozen sample (at the surface or buried in the ice), we do not understand this well. In this paper, we used X-rays to look at the chemical location in frozen samples. We found chemical location is sensitive to freezing method, sample container, and chemical characteristics, requiring careful experimental design and interpretation of results.
Lu Yu, Jeremy Smith, Alexander Laskin, Katheryn M. George, Cort Anastasio, Julia Laskin, Ann M. Dillner, and Qi Zhang
Atmos. Chem. Phys., 16, 4511–4527,Short summary
The chemical evolution of SOA formed during aqueous reactions of phenolic compounds is studied via combined bulk and molecular analysis. Phenolic SOA evolve dynamically during photochemical aging, with different reaction mechanisms (oligomerization, fragmentation, and functionalization) leading to different generations of products that span an enormous range in volatilities and a large range in oxidation state and composition. Aqueous reactions of phenols are likely an important source of ELVOC.
J. G. Charrier, N. K. Richards-Henderson, K. J. Bein, A. S. McFall, A. S. Wexler, and C. Anastasio
Atmos. Chem. Phys., 15, 2327–2340,Short summary
We measured the oxidative potential of airborne particles – a property that has been linked to health problems caused by particles – from different emission source mixtures in Fresno, CA. Copper was responsible for the majority of the oxidative potential (as measured by the DTT assay), followed by unknown species (likely organics) and manganese. Sources of copper-rich particles, including vehicles, had higher oxidative potentials.
L. Yu, J. Smith, A. Laskin, C. Anastasio, J. Laskin, and Q. Zhang
Atmos. Chem. Phys., 14, 13801–13816,
Related subject area
Subject: Clouds and Precipitation | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)A link between the ice nucleation activity and the biogeochemistry of seawaterImpact of convection on the upper-tropospheric composition (water vapor and ozone) over a subtropical site (Réunion island; 21.1° S, 55.5° E) in the Indian OceanChemical characteristics of cloud water and the impacts on aerosol properties at a subtropical mountain site in Hong Kong SARDiurnal cycle of iodine, bromine, and mercury concentrations in Svalbard surface snowWet deposition of inorganic ions in 320 cities across China: spatio-temporal variation, source apportionment, and dominant factorsDeposition of ionic species and black carbon to the Arctic snowpack: combining snow pit observations with modelingMercury and trace metal wet deposition across five stations in Alaska: controlling factors, spatial patterns, and source regionsDrivers of atmospheric deposition of polycyclic aromatic hydrocarbons at European high-altitude sitesCloud scavenging of anthropogenic refractory particles at a mountain site in North ChinaComposition of ice particle residuals in mixed-phase clouds at Jungfraujoch (Switzerland): enrichment and depletion of particle groups relative to total aerosolSnow scavenging and phase partitioning of nitrated and oxygenated aromatic hydrocarbons in polluted and remote environments in central Europe and the European ArcticContinuous non-marine inputs of per- and polyfluoroalkyl substances to the High Arctic: a multi-decadal temporal recordBiogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud waterThe single-particle mixing state and cloud scavenging of black carbon: a case study at a high-altitude mountain site in southern ChinaComposition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah firesFive-year records of mercury wet deposition flux at GMOS sites in the Northern and Southern hemispheresAtmospheric wet and litterfall mercury deposition at urban and rural sites in ChinaCloud water composition during HCCT-2010: Scavenging efficiencies, solute concentrations, and droplet size dependence of inorganic ions and dissolved organic carbonFog composition at Baengnyeong Island in the eastern Yellow Sea: detecting markers of aqueous atmospheric oxidationsWet deposition of atmospheric inorganic nitrogen at five remote sites in the Tibetan PlateauAtmospheric wet and dry deposition of trace elements at 10 sites in Northern ChinaNatural or anthropogenic? On the origin of atmospheric sulfate deposition in the Andes of southeastern EcuadorTemporal variations in rainwater methanolComprehensive assessment of meteorological conditions and airflow connectivity during HCCT-2010Influence of cloud processing on CCN activation behaviour in the Thuringian Forest, Germany during HCCT-2010Classification of clouds sampled at the puy de Dôme (France) based on 10 yr of monitoring of their physicochemical propertiesPreliminary signs of the initiation of deep convection by GNSSDissolved organic carbon (DOC) and select aldehydes in cloud and fog water: the role of the aqueous phase in impacting trace gas budgetsInsights into dissolved organic matter complexity in rainwater from continental and coastal storms by ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometryDynamics of the chemical composition of rainwater throughout Hurricane IreneSpatial and temporal distributions of total and methyl mercury in precipitation in core urban areas, Chongqing, ChinaWet and dry deposition of atmospheric nitrogen at ten sites in Northern ChinaSpatial distribution of mercury deposition fluxes in Wanshan Hg mining area, Guizhou province, ChinaMolecular characterization of water soluble organic nitrogen in marine rainwater by ultra-high resolution electrospray ionization mass spectrometryFive-year record of atmospheric precipitation chemistry in urban Beijing, ChinaMercury deposition in Southern New Hampshire, 2006–2009Chemical composition of rainwater at Maldives Climate Observatory at Hanimaadhoo (MCOH)Chemistry of rain events in West Africa: evidence of dust and biogenic influence in convective systemsAtmospheric deposition of mercury and major ions to the Pensacola (Florida) watershed: spatial, seasonal, and inter-annual variabilityAtmospheric wet deposition of mercury and other trace elements in Pensacola, FloridaAcetaldehyde in the Alaskan subarctic snowpack
Martin J. Wolf, Megan Goodell, Eric Dong, Lilian A. Dove, Cuiqi Zhang, Lesly J. Franco, Chuanyang Shen, Emma G. Rutkowski, Domenic N. Narducci, Susan Mullen, Andrew R. Babbin, and Daniel J. Cziczo
Atmos. Chem. Phys., 20, 15341–15356,Short summary
Sea spray is the largest aerosol source on Earth. These aerosol particles can impact climate by inducing ice formation in clouds. The role that ocean biology plays in determining the composition and ice nucleation abilities of sea spray aerosol is unclarified. In this study, we demonstrate that atomized seawater from highly productive ocean regions is more effective at nucleating ice than seawater from lower-productivity regions.
Damien Héron, Stéphanie Evan, Jérôme Brioude, Karen Rosenlof, Françoise Posny, Jean-Marc Metzger, and Jean-Pierre Cammas
Atmos. Chem. Phys., 20, 8611–8626,Short summary
Using a statistical method, summer variations (between 2013 and 2016) of ozone and water vapor are characterized in the upper troposphere above Réunion island (21° S, 55° E). It suggests a convective influence between 9 and 13 km. As deep convection is rarely observed near Réunion island, this study provides new insights on the long-range impact of deep convective outflow from the Intertropical Convergence Zone (ITCZ) on the upper troposphere over a subtropical site.
Tao Li, Zhe Wang, Yaru Wang, Chen Wu, Yiheng Liang, Men Xia, Chuan Yu, Hui Yun, Weihao Wang, Yan Wang, Jia Guo, Hartmut Herrmann, and Tao Wang
Atmos. Chem. Phys., 20, 391–407,Short summary
This work presents a field study of cloud water chemistry and interactions of cloud, gas, and aerosols in the polluted coastal boundary layer in southern China. Substantial dissolved organic matter in the acidic cloud water was observed, and the gas- and aqueous-phase partitioning of carbonyl compounds was investigated. The results demonstrated the significant role of cloud processing in altering aerosol properties, especially in producing aqueous organics and droplet-mode aerosols.
Andrea Spolaor, Elena Barbaro, David Cappelletti, Clara Turetta, Mauro Mazzola, Fabio Giardi, Mats P. Björkman, Federico Lucchetta, Federico Dallo, Katrine Aspmo Pfaffhuber, Hélène Angot, Aurelien Dommergue, Marion Maturilli, Alfonso Saiz-Lopez, Carlo Barbante, and Warren R. L. Cairns
Atmos. Chem. Phys., 19, 13325–13339,Short summary
The main aims of the study are to (a) detect whether mercury in the surface snow undergoes a daily cycle as determined in the atmosphere, (b) compare the mercury concentration in surface snow with the concentration in the atmosphere, (c) evaluate the effect of snow depositions, (d) detect whether iodine and bromine in the surface snow undergo a daily cycle, and (e) evaluate the role of metereological and atmospheric conditions. Different behaviours were determined during different seasons.
Rui Li, Lulu Cui, Yilong Zhao, Ziyu Zhang, Tianming Sun, Junlin Li, Wenhui Zhou, Ya Meng, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 19, 11043–11070,Short summary
Acid deposition is still an important environmental issue in China. Rainwater samples in 320 cities in China were collected to determine the acidic ion concentrations and identify their spatiotemporal variations and sources. The higher acidic ions showed higher concentrations in winter. Furthermore, the highest acidic ion concentrations were mainly distributed in YRD and SB. These acidic ions were mainly sourced from industrial emissions and agricultural activities.
Hans-Werner Jacobi, Friedrich Obleitner, Sophie Da Costa, Patrick Ginot, Konstantinos Eleftheriadis, Wenche Aas, and Marco Zanatta
Atmos. Chem. Phys., 19, 10361–10377,Short summary
By combining atmospheric, precipitation, and snow measurements with snowpack simulations for a high Arctic site in Svalbard, we find that during wintertime the transfer of sea salt components to the snowpack was largely dominated by wet deposition. However, dry deposition contributed significantly for nitrate, non-sea-salt sulfate, and black carbon. The comparison of monthly deposition and snow budgets indicates an important redistribution of the impurities in the snowpack even during winter.
Christopher Pearson, Dean Howard, Christopher Moore, and Daniel Obrist
Atmos. Chem. Phys., 19, 6913–6929,Short summary
Precipitation-based deposition of mercury and other trace metals throughout Alaska provides a significant input of pollutants. Deposition shows significant seasonal and spatial variability, largely driven by precipitation patterns. Annual wet deposition of Hg at all AK collection sites is consistently lower than other monitoring stations throughout the CONUS. Hg showed no clear relationship to other metals, likely due to its highly volatile nature and capability of long-range transport.
Lourdes Arellano, Pilar Fernández, Barend L. van Drooge, Neil L. Rose, Ulrike Nickus, Hansjoerg Thies, Evzen Stuchlík, Lluís Camarero, Jordi Catalan, and Joan O. Grimalt
Atmos. Chem. Phys., 18, 16081–16097,Short summary
Mountain areas are key for studying the impact of diffuse pollution due to human activities on the continental areas. Polycyclic aromatic hydrocarbons (PAHs), human carcinogens with increased levels since the 1950s, are significant constituents of this pollution. We determined PAHs in monthly atmospheric deposition collected in European high mountain areas. The number of sites, period of study and sampling frequency provide the most comprehensive description of PAH fallout at remote sites.
Lei Liu, Jian Zhang, Liang Xu, Qi Yuan, Dao Huang, Jianmin Chen, Zongbo Shi, Yele Sun, Pingqing Fu, Zifa Wang, Daizhou Zhang, and Weijun Li
Atmos. Chem. Phys., 18, 14681–14693,Short summary
Using transmission electron microscopy, we studied individual cloud droplet residual and interstitial particles collected in cloud events at Mt. Tai in the polluted North China region. We found that individual cloud droplets were an extremely complicated mixture containing abundant refractory soot (i.e., black carbon), fly ash, and metals. The complicated cloud droplets have not been reported in clean continental or marine air before.
Stine Eriksen Hammer, Stephan Mertes, Johannes Schneider, Martin Ebert, Konrad Kandler, and Stephan Weinbruch
Atmos. Chem. Phys., 18, 13987–14003,Short summary
It is important to study ice-nucleating particles in the environment to learn more about cloud formation. We studied the composition of ice particle residuals and total aerosol particles sampled in parallel during mixed-phase cloud events at Jungfraujoch and discovered that soot and complex secondary particles were not present. In contrast, silica, aluminosilicates, and other aluminosilicates were the most important ice particle residual groups at site temperatures between −11 and −18 °C.
Pourya Shahpoury, Zoran Kitanovski, and Gerhard Lammel
Atmos. Chem. Phys., 18, 13495–13510,
Heidi M. Pickard, Alison S. Criscitiello, Christine Spencer, Martin J. Sharp, Derek C. G. Muir, Amila O. De Silva, and Cora J. Young
Atmos. Chem. Phys., 18, 5045–5058,Short summary
Perfluoroalkyl acids (PFAAs) are persistent, bioaccumulative compounds found in the environment far from source regions, including the remote Arctic. We collected a 15 m ice core from the Canadian High Arctic to measure a 38-year deposition record of PFAAs, proving information about major pollutant sources and production changes over time. Our results demonstrate that PFAAs have continuous and increasing deposition, despite recent North American regulations and phase-outs.
Ryan D. Cook, Ying-Hsuan Lin, Zhuoyu Peng, Eric Boone, Rosalie K. Chu, James E. Dukett, Matthew J. Gunsch, Wuliang Zhang, Nikola Tolic, Alexander Laskin, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 15167–15180,Short summary
Reactions occur within water in both atmospheric particles and cloud droplets, yet little is known about the organic compounds in cloud water. In this work, cloud water samples were collected at Whiteface Mountain, New York, and analyzed using ultra-high-resolution mass spectrometry to investigate the molecular composition of the dissolved organic compounds. The results focus on changes in cloud water composition with air mass origin – influences of forest, urban, and wildfire emissions.
Guohua Zhang, Qinhao Lin, Long Peng, Xinhui Bi, Duohong Chen, Mei Li, Lei Li, Fred J. Brechtel, Jianxin Chen, Weijun Yan, Xinming Wang, Ping'an Peng, Guoying Sheng, and Zhen Zhou
Atmos. Chem. Phys., 17, 14975–14985,Short summary
The mixing state of black carbon (BC)-containing particles and the mass scavenging efficiency of BC in cloud were investigated at a mountain site (1690 m a.s.l.) in southern China. The measured BC-containing particles were internally mixed extensively with sulfate, and thus the number fraction of scavenged BC-containing particles is close to that of all the measured particles. BC-containing particles with higher fractions of organics were scavenged relatively less.
Marc D. Mallet, Luke T. Cravigan, Andelija Milic, Joel Alroe, Zoran D. Ristovski, Jason Ward, Melita Keywood, Leah R. Williams, Paul Selleck, and Branka Miljevic
Atmos. Chem. Phys., 17, 3605–3617,Short summary
This paper presents data on the size, composition and concentration of aerosol particles emitted from north Australian savannah fires and how these properties influence cloud condensation nuclei (CCN) concentrations. Both the size and composition of aerosol were found to be important in determining CCN. Despite large CCNc enhancements during periods of close biomass burning, the aerosol was very weakly hygroscopic which should be accounted for in climate models to avoid large CCNc overestimates.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Helene Angot, Carlo Barbante, Ernst-Günther Brunke, Flor Arcega-Cabrera, Warren Cairns, Sara Comero, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Xuewu Fu, Patricia Elizabeth Garcia, Bernd Manfred Gawlik, Ulla Hageström, Katarina Hansson, Milena Horvat, Jože Kotnik, Casper Labuschagne, Olivier Magand, Lynwill Martin, Nikolay Mashyanov, Thumeka Mkololo, John Munthe, Vladimir Obolkin, Martha Ramirez Islas, Fabrizio Sena, Vernon Somerset, Pia Spandow, Massimiliano Vardè, Chavon Walters, Ingvar Wängberg, Andreas Weigelt, Xu Yang, and Hui Zhang
Atmos. Chem. Phys., 17, 2689–2708,Short summary
The results on total mercury (THg) wet deposition flux obtained within the GMOS network have been presented and discussed to understand the atmospheric Hg cycling and its seasonal depositional patterns over the 2011–2015 period. The data set provides new insight into baseline concentrations of THg concentrations in precipitation particularly in regions where wet deposition and atmospheric Hg species were not investigated before, opening the way for additional measurements and modeling studies.
Xuewu Fu, Xu Yang, Xiaofang Lang, Jun Zhou, Hui Zhang, Ben Yu, Haiyu Yan, Che-Jen Lin, and Xinbin Feng
Atmos. Chem. Phys., 16, 11547–11562,
Dominik van Pinxteren, Khanneh Wadinga Fomba, Stephan Mertes, Konrad Müller, Gerald Spindler, Johannes Schneider, Taehyoung Lee, Jeffrey L. Collett, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 3185–3205,
A. J. Boris, T. Lee, T. Park, J. Choi, S. J. Seo, and J. L. Collett Jr.
Atmos. Chem. Phys., 16, 437–453,Short summary
Samples of fog water collected in the Yellow Sea during summer 2014 represent fog downwind of polluted regions and provide new insight into the fate of regional emissions. Organic and inorganic components reveal contributions from urban, biogenic, marine, and biomass burning emissions, as well as evidence of aqueous organic processing reactions. Many fog components are products of extensive photochemical aging during multiday transport, including oxidation within wet aerosols or fogs.
Y. W. Liu, Xu-Ri, Y. S. Wang, Y. P. Pan, and S. L. Piao
Atmos. Chem. Phys., 15, 11683–11700,Short summary
We investigated inorganic N wet deposition at five sites in the Tibetan Plateau (TP). Combining in situ measurements in this and previous studies, the average wet deposition of NH4+-N, NO3--N, and inorganic N in the TP was estimated to be 1.06, 0.51, and 1.58 kg N ha−1 yr−1, respectively. Results suggest that earlier estimations based on chemical transport model simulations and/or limited field measurements likely overestimated substantially the regional inorganic N wet deposition in the TP.
Y. P. Pan and Y. S. Wang
Atmos. Chem. Phys., 15, 951–972,Short summary
This paper presents the first concurrent measurements of wet and dry deposition of various trace elements in Northern China, covering an extensive area over 3 years in a global hotspot of air pollution. The unique field data can serve as a sound basis for the validation of regional emission inventories and biogeochemical or atmospheric chemistry models. The findings are very important for policy makers to create legislation to reduce the emissions and protect soil and water from air pollution.
S. Makowski Giannoni, R. Rollenbeck, K. Trachte, and J. Bendix
Atmos. Chem. Phys., 14, 11297–11312,
J. D. Felix, S. B. Jones, G. B. Avery, J. D. Willey, R. N. Mead, and R. J. Kieber
Atmos. Chem. Phys., 14, 10509–10516,
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Atmos. Chem. Phys., 14, 9105–9128,
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Atmos. Chem. Phys., 14, 7859–7868,
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Atmos. Chem. Phys., 14, 1485–1506,
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Atmos. Chem. Phys., 13, 5425–5449,
B. Ervens, Y. Wang, J. Eagar, W. R. Leaitch, A. M. Macdonald, K. T. Valsaraj, and P. Herckes
Atmos. Chem. Phys., 13, 5117–5135,
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Atmos. Chem. Phys., 13, 4829–4838,
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Atmos. Chem. Phys., 13, 2321–2330,
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Atmos. Chem. Phys., 12, 6515–6535,
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We made the first measurements of the concentrations of hydroxyl radical (•OH), a dominant environmental oxidant, in snow grains. Concentrations of •OH in snow at Summit, Greenland, are comparable to values reported for midlatitude cloud and fog drops, even though impurity levels in the snow are much lower. At these concentrations, the lifetimes of organics and bromide in Summit snow are approximately 3 days and 7 h, respectively, suggesting that OH is a major oxidant for both species.
We made the first measurements of the concentrations of hydroxyl radical (•OH), a dominant...