Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect

IF 5.2 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES Atmospheric Chemistry and Physics Pub Date : 2024-07-03 DOI:10.5194/egusphere-2024-1579
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, Vlassis A. Karydis
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Abstract

Abstract. Nitrate (NO3-) aerosol is projected to increase dramatically in the coming decades and may become the dominant inorganic particle species. This is due to the continued strong decrease in SO2 emissions, which is not accompanied by a corresponding decrease in NOx and especially NH3 emissions. Thus, the radiative effect (RE) of NO3- aerosol may become more important than that of SO42- aerosol in the future. The physicochemical interactions of mineral dust particles with gas and aerosol tracers play an important role in influencing the overall RE of dust and non-dust aerosols but can be a major source of uncertainty due to their lack of representation in many global climate models. Therefore, this study investigates how and to what extent dust affects the current global NO3- aerosol radiative effect through both radiation (REari) and cloud interactions (REaci) at the top of the atmosphere (TOA). For this purpose, multi-year simulations nudged towards the observed atmospheric circulation were performed with the global atmospheric chemistry and climate model EMAC, while the thermodynamics of the interactions between inorganic aerosols and mineral dust were simulated with the thermodynamic equilibrium model ISORROPIA-lite. The emission flux of the mineral cations Na+, Ca2+, K+ and Mg2+ is calculated as a fraction of the total aeolian dust emission based on the unique chemical composition of the major deserts worldwide. Our results reveal positive and negative shortwave and longwave radiative effects in different regions of the world via aerosol-radiation interactions and cloud adjustments. Overall, the NO3- aerosol direct effect contributes a global cooling of -0.11 W/m2, driven by coarse-mode particle cooling at short wavelengths. Regarding the indirect effect, it is noteworthy that NO3- aerosol exerts a global mean warming of +0.17 W/m2. While the presence of NO3- aerosol enhances the ability of mineral dust particles to act as cloud condensation nuclei (CCN), it simultaneously inhibits the formation of cloud droplets from the smaller anthropogenic particles. This is due to the coagulation of fine anthropogenic CCN particles with the larger nitrate-coated mineral dust particles, which leads to a reduction in total aerosol number concentration. This mechanism results in an overall reduced cloud albedo effect and is thus attributed as warming.
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矿物尘埃对全球硝酸盐气溶胶直接和间接辐射效应的影响
摘要预计硝酸盐(NO3-)气溶胶在未来几十年将急剧增加,并可能成为主要的无机颗粒物种类。这是由于二氧化硫排放量持续大幅减少,而氮氧化物(NOx),特别是氮氧化物(NH3)的排放量并没有相应减少。因此,未来 NO3- 气溶胶的辐射效应(RE)可能比 SO42- 气溶胶更为重要。矿物尘埃粒子与气体和气溶胶示踪剂的物理化学相互作用在影响尘埃和非尘埃气溶胶的总体辐射效应方面发挥着重要作用,但由于它们在许多全球气候模式中缺乏代表性,因此可能成为不确定性的主要来源。因此,本研究通过大气顶部(TOA)的辐射(REari)和云相互作用(REaci),探讨了尘埃如何以及在多大程度上影响当前全球 NO3-气溶胶辐射效应。为此,利用全球大气化学和气候模式 EMAC 对观测到的大气环流进行了多年模拟,同时利用热力学平衡模式 ISORROPIA-lite 模拟了无机气溶胶和矿物尘埃之间相互作用的热力学。根据全球主要沙漠的独特化学成分,计算出矿物阳离子 Na+、Ca2+、K+ 和 Mg2+ 的排放通量占风化尘排放总量的比例。我们的研究结果表明,通过气溶胶与辐射的相互作用和云的调节,在世界不同地区产生了正负两方面的短波和长波辐射效应。总体而言,在短波长粗模粒子冷却的驱动下,NO3-气溶胶的直接效应导致全球降温-0.11 W/m2。在间接效应方面,值得注意的是,NO3-气溶胶导致全球平均变暖+0.17 W/m2。虽然 NO3- 气溶胶的存在增强了矿物尘埃粒子作为云凝结核(CCN)的能力,但同时也抑制了较小的人为粒子形成云滴。这是由于细小的人为 CCN 颗粒与较大的硝酸盐包裹的矿物尘埃颗粒凝结在一起,导致气溶胶总数量浓度降低。这一机制导致云反照率效应总体降低,因此被归因于气候变暖。
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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