Chemical Characterization of Arctic Atmospheric Particles on the North Slope of Alaska using Single-Particle Microscopy and High-Resolution Mass Spectrometry
EMSL Project ID
49331
Abstract
Single-particle microscopy and high-resolution mass spectrometry will be utilized to characterize the chemical composition of Arctic atmospheric particles. Given recent sea ice loss, we hypothesize that sea spray and local combustion sources control primary and secondary aerosol generation and chemical transformation in the Arctic. To test this hypothesis, EMSL resources will be utilized to 1) determine individual particle sources and mixing of primary and secondary species and 2) determine organic molecular composition for various aerosol source influences. By connecting to aerosol optical properties and cloud formation efficiencies measured during particle sampling, these analyses will provide insights into how changing natural and anthropogenic emissions, along with atmospheric processing, are driving interactions with radiation and clouds in the Arctic region. In these ways, the proposed project will fill a critical gap in our understanding of the Arctic system by improving our knowledge of the sources and processing of atmospheric particles through the molecular-level chemical composition measurements. Model estimates of atmospheric aerosol radiative forcing are currently limited in part by the dearth of measurement data available for evaluation; therefore, it is estimated that this project will ultimately lead to improved estimates of aerosol-climate feedbacks. Atmospheric particle samples have been collected near Barrow, AK over three seasons (2014-2016), and future sampling (2016) will occur at Barrow, AK and Oliktok Point, AK. Additional sampling will occur across Bering Strait and Chukchi Sea as part of the 2017 Russian-American Long-term Census of the Arctic Cruise. The proposed EMSL project will directly support the Department of Energy Atmospheric Radiation Measurement (DOE ARM) program 2015-2016 field campaign "Summertime Aerosol across the North Slope of Alaska." The unique mass spectrometry and microscopy measurement capabilities, available at EMSL with the leading researchers in the use of this instrumentation for aerosol analysis, are essential to the success of the proposed project. Access to computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (CCSEM-EDX) and direct infusion electrospray ionization (ESI) coupled to Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry is limited at the University of Michigan. The nano-DESI technique was developed at EMSL, such that interactions with the EMSL researchers and use of the high-resolution mass spectrometer coupled to this ionization technique are required for this analysis. Further, time-of-flight secondary ion mass spectrometry (TOF-SIMS), NanoSIMS, and nano-desorption electrospray ionization (nano-DESI) coupled to an Orbitrap mass spectrometer are not available at the University of Michigan. Therefore, access to these EMSL resources is required for the proposed project, during which the morphology, chemical speciation, and isotopic composition of individual atmospheric particles and the organic molecular composition of the bulk particulate matter will be determined. Therefore, use of EMSL instrumentation is necessary and paramount to the success of this project, which will only be possible with the proposed EMSL collaboration and is expected to yield significant insights into our understanding of aerosol-climate feedbacks in the Arctic.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Bondy AL, B Wang, A Laskin, RL Craig, MV Nhliziyo, S Bertman, KA Pratt, PB Shepson, and AP Ault. 2017. "Inland Sea Spray Aerosol Transport and Incomplete Chloride Depletion: Varying Degrees of Reactive Processing Observed during SOAS." Environmental Science & Technology 51(17):9533-9542. doi:10.1021/acs.est.7b02085
Cook R.D., Y. Lin, Z. Peng, E.J. Boone, R.K. Chu, J.E. Dukett, and M.J. Gunsch, et al. 2017. "Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water." Atmospheric Chemistry and Physics 17, no. 24:15167-15180. PNNL-SA-130575. doi:10.5194/acp-17-15167-2017
Creamean J., R.M. Kirpes, K.A. Pratt, N.J. Spada, M. Maahn, G. de Boer, and R.C. Schnell, et al. 2018. "Marine and terrestrial influences on ice nucleating particles during continuous springtime measurements in an Arctic oilfield location." Atmospheric Chemistry and Physics Discussions 18, no. 24:18023-18042. PNNL-SA-135739. doi:10.5194/acp-18-18023-2018
Gunsch MJ, RM Kirpes, KR Kolesar, TE Berrett, S China, RJ Sheesley, A Laskin, A Wiedensohler, T Tuch, and KA Pratt. 2017. "Contributions of Transported Prudhoe Bay Oilfield Emissions to the Aerosol Population in Utqia?vik, Alaska." Atmospheric Chemistry and Physics 17(17):, doi:10.5194/acp-17-10879-2017
Kirpes R.M., A.L. Bondy, D. Bonanno, R. Moffet, B. Wang, A. Laskin, and A.P. Ault, et al. 2018. "Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic." Atmospheric Chemistry and Physics 18, no. 6:3937-3949. PNNL-SA-136257. doi:10.5194/acp-18-3937-2018
Kirpes R.M., B.L. Rodriguez, S. Kim, S. China, A. Laskin, K. Park, and J. Jung, et al. 2020. "Influence of Marine Emissions and Atmospheric Processing on Individual Particle Composition of Summertime Arctic Aerosol in the Bering Strait and Chukchi Sea." Environmental Science Processes & Impacts 22, no. 5:1201-1213. PNNL-SA-148936. doi:10.1039/C9EM00495E
May N.W., M.J. Gunsch, N.E. Olson, A.L. Bondy, R.M. Kirpes, S. Bertman, and S. China, et al. 2018. "Unexpected contributions of sea spray and lake spray aerosol to inland particulate matter." Environmental Science & Technology Letters 5, no. 7:405-412. PNNL-SA-132459. doi:10.1021/acs.estlett.8b00254
May NW, N Olson, MH Panas, JL Axson, PN Tirella, RM Kirpes, RL Craig, MJ Gunsch, S China, A Laskin, AP Ault, and KA Pratt. 2018. "Aerosol Emissions from Great Lakes Harmful Algal Blooms." Environmental Science & Technology 52(2):397-405. doi:10.1021/acs.est.7b03609
McNamara S.M., K.R. Kolesar, S. Wang, R.M. Kirpes, N.W. May, M.J. Gunsch, and R.D. Cook, et al. 2020. "Observation of Road Salt Aerosol Driving Inland Wintertime Atmospheric Chlorine Chemistry." ACS Central Science 6, no. 5:684-694. PNNL-SA-144344. doi:10.1021/acscentsci.9b00994
Raso AR, KD Custard, NW May, D Tanner, MK Newburn, LR Walker, RJ Moore, LG Huey, L Alexander, PB Shepson, and KA Pratt. 2017. "Active molecular iodine photochemistry in the Arctic." Proceedings of the National Academy of Sciences of the United States of America 114(38):10053-10058. doi:10.1073/pnas.1702803114