Inderjeet Singh, Randall V. Martin, Liam Bindle, Deepangsu Chatterjee, Chi Li, Christopher Oxford, Xiaoguang Xu, Jun Wang
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引用次数: 0
摘要
许多化学传输模型将矿物尘埃视为球形。太阳后向散射痕量气体探测(如 OMI 和 TROPOMI)隐含地将矿物尘埃视为球形。我们研究了矿物尘埃颗粒形态的影响,以评估其对全球化学传输模式(GEOS-Chem)模拟和紫外线和可见光(UV-Vis)波长太阳后向散射痕量气体探测的影响。我们研究了矿物尘埃粒子的形态如何影响模拟尘埃气溶胶光学深度;异质化学的表面积、反应和扩散参数;相功能以及用于太阳反向散射检索的空气质量因子(AMF)计算的散射权重。我们使用不同长宽比的球形颗粒来模拟尘埃光学特性,并结合形状和孔隙率来模拟表面积、反应和扩散参数。我们发现,假定颗粒为球形,则模拟尘埃消光效率会产生高达 14%的大小误差和波长误差,模拟尘埃光学深度的相应误差通常在 5%以内。我们发现,使用球形颗粒而不是球形颗粒会增加前向散射辐射,减少后向散射,这反过来又会降低二氧化氮太阳后向散射检索对气溶胶的灵敏度,降低系数为 2.0-2.5。我们开发并应用了一个基于孔隙率和表面分形维度的理论框架,在增加表面积和物种反应性的驱动下,反应吸收系数会相应增加。两者之间的差异很大,足以证明在化学传输模型和紫外-可见痕量气体检索中需要考虑尘埃的非球形性。
Effect of Dust Morphology on Aerosol Optics in the GEOS-Chem Chemical Transport Model, on UV-Vis Trace Gas Retrievals, and on Surface Area Available for Reactive Uptake
Many chemical transport models treat mineral dust as spherical. Solar backscatter retrievals of trace gases (e.g., OMI and TROPOMI) implicitly treat mineral dust as spherical. The impact of the morphology of mineral dust particles is studied to assess its implications for global chemical transport model (GEOS-Chem) simulations and solar backscatter trace gas retrievals at ultraviolet and visible (UV-Vis) wavelengths. We investigate how the morphology of mineral dust particles affects the simulated dust aerosol optical depth; surface area, reaction, and diffusion parameters for heterogeneous chemistry; phase function, and scattering weights for air mass factor (AMF) calculations used in solar backscatter retrievals. We use a mixture of various aspect ratios of spheroids to model the dust optical properties and a combination of shape and porosity to model the surface area, reaction, and diffusion parameters. We find that assuming spherical particles can introduce size-dependent and wavelength-dependent errors of up to 14% in simulated dust extinction efficiency with corresponding error in simulated dust optical depth typically within 5%. We find that use of spheroids rather than spheres increases forward scattered radiance and decreases backward scattering that in turn decrease the sensitivity of solar backscatter retrievals of NO2 to aerosols by factors of 2.0–2.5. We develop and apply a theoretical framework based on porosity and surface fractal dimension with corresponding increase in the reactive uptake coefficient driven by increased surface area and species reactivity. Differences are large enough to warrant consideration of dust non-sphericity for chemical transport models and UV-Vis trace gas retrievals.
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