Aerosol size distribution and radiative forcing response to anthropogenically driven historical changes in biogenic secondary organic aerosol formation
Aerosol size distribution and radiative forcing response to anthropogenically driven historical changes in biogenic secondary organic aerosol formation
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DOI：
10.5194/acp-15-2247-2015
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发表时间：
2015-01-01
影响因子：
6.3
通讯作者：
Pierce, J. R.
中科院分区：
文献类型：
--
作者：
D'Andrea, S. D.;Navarro, J. C. Acosta;Pierce, J. R.
在过去的千年里，由于土地利用、温度和二氧化碳浓度的变化，生物源挥发性有机化合物(BVOCs)的排放发生了变化。最近对BVOC排放量的重建预测了全球异戊二烯排放量的减少，而单萜和倍半萜排放量的增加；然而，由于各种影响因素之间的竞争，这三个排放量都显示出区域差异。在这项工作中，我们使用两个对1000-2000年间BVOC排放量的模拟估计来检验人为变化对BVOC排放的影响，使用GEOS-Chem-TOMAS(戈达德地球观测系统；两时刻气溶胶分段)全球气溶胶微物理模式来检验BVOC排放的人为变化对二次有机气溶胶(SOA)形成、全球气溶胶尺寸分布和辐射效应的影响。随着人为排放(如SO2、NOx、初级气溶胶)的关闭和BVOC排放量从公元1000年变为公元2000年的数值变化，预计自公元1000年以来土地利用发生广泛变化的地区，2000年尺寸为D-p>；80 nm(N80)的>；25%的颗粒物的数量浓度将比公元1000年减少，这导致这些地区的>；0.5W m(-2)的综合气溶胶辐射效应(直接和间接)区域增加。我们测试了我们的结果对BVOC排放清单、SOA收益率和人为排放的存在的敏感性；然而，该模型对历史BVOC变化的定性响应在所有情况下都是相同的。考虑到这些不确定性，我们估计，BVOC排放的千禧年变化造成的全球平均直接影响在+0.022至+0.163W m(-2)之间，全球平均云-反照率气溶胶间接影响在-0.008至-0.056 W m(-2)之间。气溶胶的这种变化，以及相关的辐射强迫，可能是对区域气候的一种很大程度上被忽视的重要的人为气溶胶效应。
Emissions of biogenic volatile organic compounds (BVOCs) have changed in the past millennium due to changes in land use, temperature, and CO2 concentrations. Recent reconstructions of BVOC emissions have predicted that global isoprene emissions have decreased, while monoterpene and sesquiterpene emissions have increased; however, all three show regional variability due to competition between the various influencing factors.In this work, we use two modeled estimates of BVOC emissions from the years 1000 to 2000 to test the effect of anthropogenic changes to BVOC emissions on secondary organic aerosol (SOA) formation, global aerosol size distributions, and radiative effects using the GEOS-Chem-TOMAS (Goddard Earth Observing System; TwO-Moment Aerosol Sectional) global aerosol microphysics model. With anthropogenic emissions (e.g., SO2, NOx, primary aerosols) turned off and BVOC emissions changed from year 1000 to year 2000 values, decreases in the number concentration of particles of size D-p > 80 nm (N80) of > 25% in year 2000 relative to year 1000 were predicted in regions with extensive land-use changes since year 1000 which led to regional increases in the combined aerosol radiative effect (direct and indirect) of > 0.5W m(-2) in these regions. We test the sensitivity of our results to BVOC emissions inventory, SOA yields, and the presence of anthropogenic emissions; however, the qualitative response of the model to historic BVOC changes remains the same in all cases. Accounting for these uncertainties, we estimate millennial changes in BVOC emissions cause a global mean direct effect of between +0.022 and +0.163W m(-2) and the global mean cloud-albedo aerosol indirect effect of between -0.008 and -0.056 W m(-2). This change in aerosols, and the associated radiative forcing, could be a largely overlooked and important anthropogenic aerosol effect on regional climates.