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首页> 外文期刊>Atmospheric chemistry and physics >Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing
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Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing

机译：对流层硫酸铵-硝酸盐颗粒的物理状态对全球气溶胶直接辐射强迫的影响

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The effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US) and once for lower side (LS) of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2 (g SO4-2)-1, which compare to US values of 0.030 and 13.9 m2 (g SO4-2)-1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m-2) are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL=-0.750, FU=-0.930, and face="Symbol">DFU,L=24% for full sky calculations without clouds and FL=-0.485, FU=-0.605, and face="Symbol">DFU,L=25% when clouds are included. Regionally, face="Symbol">DFU,L=48% over the USA, 55% over Europe, and 34% over East Asia. Seasonally, face="Symbol">DFU,L varies from 18% in DJF to 75% in SON over the USA. The global annual average contribution from anthropogenic aerosol is FL=-0.314 and FU=-0.404, which yield normalized direct radiative forcings (G) of GL=-205 W (g SO4-2)-1 and GU=-264 W (g SO4-2)-1.
机译：评估了水对结晶硫酸盐-硝酸盐-铵对流层颗粒对总体气溶胶直接辐射强迫的影响。全球三维化学迁移模型预测硫酸盐，硝酸盐和铵气溶胶的质量。气溶胶热力学模型被称为两次，一次用于颗粒相滞后回线的上侧（US），下侧（LS）。在LS上，硫酸盐质量预算为40％固体硫酸铵，12％锂钛矿，11％硫酸氢铵和37％水溶液。 LS硝酸盐的质量预算是由于结晶时挥发性增加而释放的固体硝酸铵为26％，水溶液为7％，气相硝酸为67％。 LS铵的预算为45％的固体硫酸铵，10％的锂铁矿，6％的硫酸氢铵，4％的硝酸铵，7％的由于挥发性增加而释放的氨和28％的水溶液。 LS气溶胶的水量分配为22％流向气相，其余78％为气溶胶。在Mie散射模型中使用预测的US / LS气溶胶质量全局场来生成US / LS气溶胶全局光学特性，包括散射效率，单次散射反照率和不对称参数。全球年平均LS光学深度和质量散射效率分别为0.023和10.7 m 2 （g SO 4 -2 ） -1 ，与美国的0.030和13.9 m 2 （g SO 4 -2 ）- 1 。首先计算没有气溶胶的基本情况，然后计算与磁滞回线的US和LS对应的两个全局场的辐射传输。 LS和US（ F L 和 F 的大气顶气溶胶辐射强迫的区域，全球，季节性和年度平均值分别计算W m -2 中的U 。包括人为排放量和自然排放量，我们获得的全球年平均值为 F L =-0.750， F U = -0.930，并且 face =“ Symbol”> D F U，L = 24％用于不包括云和 F < sub> L =-0.485， F U =-0.605和 face =“ Symbol”> D <当包含云时，i> F U，L = 25％。在地区上， face =“ Symbol”> D F U，L =美国的48％，欧洲的55％和东部的34％亚洲。季节性地，美国的 face =“ Symbol”> D F U，L 从DJF的18％变为SON的75％。人为气溶胶的全球年平均贡献为 F L =-0.314和 F U =-0.404，产生 G L =-205 W（g SO 4 ）的归一化直接辐射强迫（ G ） -2 ） -1 和 G U =-264 W（g SO 4 -2 ） -1 。

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