Organic coating on sulfate and soot particles during late summer in the Svalbard Archipelago

Abstract. Interaction of anthropogenic particles with radiation and clouds plays an important role in Arctic climate change. The mixing state of aerosols is a key parameter to influence aerosol radiation and aerosol–cloud interactions. However, little is known of this parameter in the Arctic, preventing an accurate representation of this information in global models. Here we used transmission electron microscopy with energy-dispersive X-ray spectrometry, scanning electron microscopy, nanoscale secondary ion mass spectrometry, and atomic forces microscopy to determine the size and mixing state of individual sulfate and carbonaceous particles at 100 nm to 2 µm collected in the Svalbard Archipelago in summer. We found that 74 % by number of non-sea-salt sulfate particles were coated with organic matter (OM); 20 % of sulfate particles also had soot inclusions which only appeared in the OM coating. The OM coating is estimated to contribute 63 % of the particle volume on average. To understand how OM coating influences optical properties of sulfate particles, a Mie core–shell model was applied to calculate optical properties of individual sulfate particles. Our result shows that the absorption cross section of individual OM-coated particles significantly increased when assuming the OM coating as light-absorbing brown carbon. Microscopic observations here suggest that OM modulates the mixing structure of fine Arctic sulfate particles, which may determine their hygroscopicity and optical properties.

[1]  Matthew West,et al.  Aerosol Mixing State: Measurements, Modeling, and Impacts , 2019, Reviews of Geophysics.

[2]  N. Mahowald,et al.  Glacially sourced dust as a potentially significant source of ice nucleating particles , 2019, Nature Geoscience.

[3]  L. Bi,et al.  How the Inhomogeneity of Wet Sea Salt Aerosols Affects Direct Radiative Forcing , 2019, Geophysical Research Letters.

[4]  R. Bahreini,et al.  Brown Carbon Formation from Nighttime Chemistry of Unsaturated Heterocyclic Volatile Organic Compounds , 2019, Environmental Science & Technology Letters.

[5]  R. Martin,et al.  Overview paper: New insights into aerosol and climate in the Arctic , 2018, Atmospheric Chemistry and Physics.

[6]  Y. Kondo,et al.  Effects of mixing state on optical and radiative properties of black carbon in the European Arctic , 2018, Atmospheric Chemistry and Physics.

[7]  P. Rasch,et al.  Sulfate Aerosol in the Arctic: Source Attribution and Radiative Forcing , 2018 .

[8]  U. Lohmann,et al.  How important are future marine and shipping aerosol emissions in a warming Arctic summer and autumn? , 2017, Atmospheric Chemistry and Physics.

[9]  G. McFarquhar,et al.  The observed influence of local anthropogenic pollution on northern Alaskan cloud properties , 2017 .

[10]  A. Laskin,et al.  Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic , 2017 .

[11]  R. Martin,et al.  Source attribution of Arctic black carbon constrained by aircraft and surface measurements , 2017 .

[12]  J. Jimenez,et al.  Exploring the observational constraints on the simulation of brown carbon , 2017 .

[13]  Roy M Harrison,et al.  Arctic sea ice melt leads to atmospheric new particle formation , 2017, Scientific Reports.

[14]  J. Schneider,et al.  Summertime observations of elevated levels of ultrafine particles in the high Arctic marine boundary layer , 2017 .

[15]  C. Ritter,et al.  Morphochemical characteristics and mixing state of long range transported wildfire particles at Ny-Ålesund (Svalbard Islands) , 2017 .

[16]  R. Harrison,et al.  Air pollution–aerosol interactions produce more bioavailable iron for ocean ecosystems , 2017, Science Advances.

[17]  A. Stohl,et al.  Siberian Arctic black carbon sources constrained by model and observation , 2017, Proceedings of the National Academy of Sciences.

[18]  Nicole Riemer,et al.  A conceptual framework for mixing structures in individual aerosol particles , 2016 .

[19]  A. Stohl,et al.  The sources of atmospheric black carbon at a European gateway to the Arctic , 2016, Nature Communications.

[20]  Qinbin Li,et al.  Factors controlling black carbon distribution in the Arctic , 2016 .

[21]  K. Salzen,et al.  Arctic air pollution : Challenges and opportunities for the next decadeArctic air pollution : Challenges and opportunities for the next decade , 2016 .

[22]  Armando D. Estillore,et al.  Substrate-Deposited Sea Spray Aerosol Particles: Influence of Analytical Method, Substrate, and Storage Conditions on Particle Size, Phase, and Morphology. , 2015, Environmental science & technology.

[23]  Xiaoye Zhang,et al.  Sea salt aerosols as a reactive surface for inorganic and organic acidic gases in the Arctic troposphere , 2015 .

[24]  D. Brus,et al.  Black carbon concentrations and mixing state in the Finnish Arctic , 2015 .

[25]  C. Leck,et al.  Importance of aerosol composition and mixing state for cloud droplet activation over the Arctic pack ice in summer , 2015 .

[26]  A. Laskin,et al.  Chemistry of atmospheric brown carbon. , 2015, Chemical reviews.

[27]  M. Chin,et al.  Modelled black carbon radiative forcing and atmospheric lifetime in AeroCom Phase II constrained by aircraft observations , 2014 .

[28]  U. Lohmann,et al.  Single-particle characterization of the high-Arctic summertime aerosol , 2014 .

[29]  A. Laskin,et al.  Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry , 2014 .

[30]  Kihong Park,et al.  Mixing state of size-selected submicrometer particles in the Arctic in May and September 2012. , 2014, Environmental science & technology.

[31]  Gerhard Wotawa,et al.  The Lagrangian particle dispersion model FLEXPART-WRF version 3.1 , 2013 .

[32]  Gregory T. Carroll,et al.  Atmospheric Chemistry and Physics Spectro-microscopic Measurements of Carbonaceous Aerosol Aging in Central California , 2022 .

[33]  H. Ólafsson,et al.  Long-term frequency and characteristics of dust storm events in Northeast Iceland (1949–2011) , 2013 .

[34]  V. Ramanathan,et al.  Brown carbon: a significant atmospheric absorber of solar radiation? , 2013 .

[35]  A. Schmidt,et al.  Impact of future Arctic shipping on high‐latitude black carbon deposition , 2013 .

[36]  A. Robinson,et al.  Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions , 2013 .

[37]  J. Heintzenberg,et al.  Marine nanogels as a source of atmospheric nanoparticles in the high Arctic , 2013 .

[38]  J. Gabrieli,et al.  Molecular markers of biomass burning in arctic aerosols. , 2013, Environmental science & technology.

[39]  S. Warren,et al.  Observed vertical redistribution of black carbon and other insoluble light‐absorbing particles in melting snow , 2013 .

[40]  B. DeAngelo,et al.  Bounding the role of black carbon in the climate system: A scientific assessment , 2013 .

[41]  K. Hungerbuhler,et al.  Emissions, fate and transport of persistent organic pollutants to the Arctic in a changing global climate. , 2013, Environmental science & technology.

[42]  Sergey A. Nizkorodov,et al.  Formation of brown carbon via reactions of ammonia with secondary organic aerosols from biogenic and anthropogenic precursors , 2012 .

[43]  A. Laskin,et al.  Heterogeneous ice nucleation and water uptake by field‐collected atmospheric particles below 273 K , 2012 .

[44]  M. Cubison,et al.  Analysis of CCN activity of Arctic aerosol and Canadian biomass burning during summer 2008 , 2012 .

[45]  A. Middlebrook,et al.  Brown carbon and internal mixing in biomass burning particles , 2012, Proceedings of the National Academy of Sciences.

[46]  A. Bertram,et al.  Images reveal that atmospheric particles can undergo liquid–liquid phase separations , 2012, Proceedings of the National Academy of Sciences.

[47]  J. Kay,et al.  The Arctic response to remote and local forcing of black carbon , 2012 .

[48]  J. Ström,et al.  Chemical composition and sources of aerosol particles at Zeppelin Mountain (Ny Ålesund, Svalbard): An electron microscopy study , 2012 .

[49]  A. Nenes,et al.  Hygroscopicity and composition of Alaskan Arctic CCN during April 2008 , 2011 .

[50]  U. Lohmann,et al.  Cloud condensation nuclei closure study on summer arctic aerosol , 2011 .

[51]  A. Stohl,et al.  Aerosol composition and sources in the central Arctic Ocean during ASCOS , 2011 .

[52]  Glen P. Peters,et al.  Future emissions from shipping and petroleum activities in the Arctic , 2011 .

[53]  S. Warren,et al.  Sources of light-absorbing aerosol in arctic snow and their seasonal variation , 2010 .

[54]  P. Pilewskie,et al.  Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project , 2010 .

[55]  Glenn E. Shaw,et al.  The Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission: design, execution, and first results , 2010 .

[56]  C. Ro,et al.  Single-particle characterization of summertime arctic aerosols collected at Ny-Alesund, Svalbard. , 2010, Environmental science & technology.

[57]  L. Barrie,et al.  Photochemical and other sources of organic compounds in the Canadian high arctic aerosol pollution during winter-spring. , 2009, Environmental science & technology.

[58]  R. C. Easter,et al.  Simulating the evolution of soot mixing state with a particle-resolved aerosol model , 2008, 0809.0875.

[59]  Peter A. Crozier,et al.  Brown Carbon Spheres in East Asian Outflow and Their Optical Properties , 2008, Science.

[60]  Chemical properties of Arctic aerosol particles collected at the Zeppelin station during the aerosol transition period in May and June of 2004 , 2008 .

[61]  G. Powers,et al.  A Description of the Advanced Research WRF Version 3 , 2008 .

[62]  D. Shindell Local and remote contributions to Arctic warming , 2007 .

[63]  A. Stohl,et al.  Arctic Air Pollution: Origins and Impacts , 2007, Science.

[64]  P. Quinn,et al.  Arctic haze: current trends and knowledge gaps , 2007 .

[65]  Harro A. J. Meijer,et al.  Radiocarbon analyses along the EDML ice core in Antarctica , 2007 .

[66]  D. Murphy,et al.  Nano-scale secondary ion mass spectrometry — A new analytical tool in biogeochemistry and soil ecology: A review article , 2007 .

[67]  M. Andreae,et al.  Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols , 2006 .

[68]  U. Lohmann,et al.  Summertime pollution events in the Arctic and potential implications , 2006 .

[69]  C. Leck,et al.  Comparison of sources and nature of the tropical aerosol with the summer high Arctic aerosol , 2008 .

[70]  J. Hansen,et al.  Distant origins of Arctic black carbon: A Goddard Institute for Space Studies ModelE experiment , 2005 .

[71]  J. Hansen,et al.  Soot climate forcing via snow and ice albedos. , 2004, Proceedings of the National Academy of Sciences of the United States of America.

[72]  Yasunobu Iwasaka,et al.  Mixing states of individual aerosol particles in spring Arctic troposphere during ASTAR 2000 campaign , 2003 .

[73]  P. Buseck,et al.  Airborne minerals and related aerosol particles: effects on climate and the environment. , 1999, Proceedings of the National Academy of Sciences of the United States of America.

[74]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1998 .

[75]  G. Shaw Arctic air pollution , 1988 .

[76]  P. Barber Absorption and scattering of light by small particles , 1984 .

[77]  Hiroaki Minoura,et al.  The transport and spacial scale of Asian dust‐storm clouds: a case study of the dust‐storm event of April 1979 , 1983 .