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DOI10.5194/acp-22-9033-2022
Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources
Cheng, Zezhen; Morgenstern, Megan; Zhang, Bo; Fraund, Matthew; Lata, Nurun Nahar; Brimberry, Rhenton; Marcus, Matthew A.; Mazzoleni, Lynn; Fialho, Paulo; Henning, Silvia; Wehner, Birgit; Mazzoleni, Claudio; China, Swarup
发表日期2022
ISSN1680-7316
EISSN1680-7324
起始页码9033
结束页码9057
卷号22期号:13页码:25
英文摘要Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The LEXPART analysis showed that the sampled air masses were highly aged (average plume age > 10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (similar to 29.9 % to 82.0 %), sea salt (similar to 0.3 % to 31.6 %), and sea salt with sulfate (similar to 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (similar to 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (similar to 0 % to 30 % and similar to 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.
学科领域Environmental Sciences; Meteorology & Atmospheric Sciences
语种英语
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号WOS:000823511000001
来源期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/273077
作者单位United States Department of Energy (DOE); Pacific Northwest National Laboratory; Michigan Technological University; National Institute for Aerospace; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; Leibniz Institut fur Tropospharenforschung (TROPOS)
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Cheng, Zezhen,Morgenstern, Megan,Zhang, Bo,et al. Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources[J],2022,22(13):25.
APA Cheng, Zezhen.,Morgenstern, Megan.,Zhang, Bo.,Fraund, Matthew.,Lata, Nurun Nahar.,...&China, Swarup.(2022).Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(13),25.
MLA Cheng, Zezhen,et al."Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.13(2022):25.
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