Quantifying structural errors in cloud condensation nuclei activity from reduced representation of aerosol size distributions

IF 3.9 3区 环境科学与生态学 Q2 ENGINEERING, CHEMICAL Journal of Aerosol Science Pub Date : 2024-05-23 DOI:10.1016/j.jaerosci.2024.106388
Laura Fierce, Yu Yao, Richard Easter, Po-Lun Ma, Jian Sun, Hui Wan, Kai Zhang
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Abstract

Aerosol effects on clouds and radiation are a large source of uncertainty in our understanding of human impacts on the climate system. Uncertainty in aerosol effects results from uncertainty in parameter values, known as parametric uncertainty, and from uncertainty from the model’s structure, known as structural uncertainty. While previous studies have assessed the impact of parametric uncertainty on modeled forcing, structural errors from the numerical representation of particle distributions and their dynamics have not been well quantified. Here we present a framework for quantifying error in aerosol size distributions and cloud condensation nuclei activity, which we apply to the widely used 4-mode version of the Modal Aerosol Module (MAM4). Box model predictions from the MAM4 are evaluated against the Particle Monte Carlo Model for Simulating Aerosol Interactions and Chemistry (PartMC-MOSAIC), a benchmark model that tracks the evolution of individual particles. We show that size distributions simulated by MAM4 diverge from those simulated by PartMC-MOSAIC after only a few hours of aging by condensation and coagulation in polluted conditions, which leads to large errors in modeled cloud condensation nuclei concentrations. We find that differences between MAM4 and PartMC-MOSAIC are largest under polluted conditions, where the size distribution evolves rapidly though aging. These findings indicate that structural error in modeled aerosol properties is a key factor contributing to uncertainty in aerosol forcing.

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从气溶胶粒度分布的简化表示量化云凝结核活动的结构误差
气溶胶对云层和辐射的影响是我们了解人类对气候系统影响的一大不确定因素。气溶胶效应的不确定性来自参数值的不确定性(称为参数不确定性)和模型结构的不确定性(称为结构不确定性)。以往的研究已经评估了参数不确定性对模型强迫的影响,但对粒子分布及其动态的数值表示所产生的结构误差还没有进行很好的量化。在此,我们提出了一个气溶胶粒径分布和云凝结核活动误差量化框架,并将其应用于广泛使用的四模式气溶胶模态(MAM4)版本。我们将 MAM4 的盒式模型预测结果与模拟气溶胶相互作用和化学的粒子蒙特卡罗模型(PartMC-MOSAIC)进行了对比评估,后者是一个跟踪单个粒子演变的基准模型。我们发现,在污染条件下,MAM4 模拟的粒度分布与 PartMC-MOSAIC 模拟的粒度分布在凝结和凝结老化几个小时后就出现了偏差,从而导致云凝结核浓度模型出现较大误差。我们发现,在污染条件下,MAM4 和 PartMC-MOSAIC 之间的差异最大,因为在污染条件下,尺寸分布会随着老化而迅速变化。这些发现表明,模拟气溶胶特性的结构误差是造成气溶胶强迫不确定性的关键因素。
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来源期刊
Journal of Aerosol Science
Journal of Aerosol Science 环境科学-工程:化工
CiteScore
8.80
自引率
8.90%
发文量
127
审稿时长
35 days
期刊介绍: Founded in 1970, the Journal of Aerosol Science considers itself the prime vehicle for the publication of original work as well as reviews related to fundamental and applied aerosol research, as well as aerosol instrumentation. Its content is directed at scientists working in engineering disciplines, as well as physics, chemistry, and environmental sciences. The editors welcome submissions of papers describing recent experimental, numerical, and theoretical research related to the following topics: 1. Fundamental Aerosol Science. 2. Applied Aerosol Science. 3. Instrumentation & Measurement Methods.
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