Accurate and Direct Measurements of Brown Carbon Aerosol Optical Properties During Formation and Atmospherically-Relevant Ageing Processes
准确、直接测量地层和大气相关老化过程中棕碳气溶胶的光学特性
基本信息
- 批准号:NE/S014314/2
- 负责人:
- 金额:$ 17.63万
- 依托单位:
- 依托单位国家:英国
- 项目类别:Fellowship
- 财政年份:2023
- 资助国家:英国
- 起止时间:2023 至 无数据
- 项目状态:未结题
- 来源:
- 关键词:
项目摘要
Aerosols are liquid or solid particles suspended in a gas and are pervasive in our atmosphere, with sources including anthropogenic emissions from burning of fossil fuels, and natural sources including from sea spray, desert dust and wildfire biomass burning. These aerosols have significant impacts on our atmosphere, affecting human health through, for example, smog events and global climate through interacting with Sun light and cloud droplets. Indeed, aerosols represent one of the largest uncertainties in predicting future climate change. The net aerosol cooling effect, provided by aerosol scattering sunlight back to space, partially offsets the warming impact of greenhouse gases. However, large uncertainties in this aerosol-light interaction degrade the confidence we have in models of future climate. Improvements to our understanding of aerosol-light interactions could lead to more effective risk mitigation strategies in managing climate change impacts.The important parameters to measure for constraining estimates of aerosol-light interactions are the magnitudes of light scattering and absorption by aerosol. In particular, light absorption is studied poorly for carbonaceous aerosol, with the optical properties of a class of aerosol called brown carbon aerosol (BrC) understood very poorly. BrC particles are formed readily in biomass burning regions where gaseous organic molecules emitted during burning rapidly condense onto liquid or solid particles, with these organic molecules reacting on particle surfaces or inside liquid particles to form light absorbing chromophores. The subsequent BrC particles possess strong wavelength-dependent absorption spectra, with stronger absorption at shorter (blue) optical wavelengths compared to longer (red) wavelengths giving a brown appearance. Also, atmospheric BrC consists of a variety of molecular species with differing light absorption spectra, while the compositions of these chromophores evolve significantly with atmospheric ageing. The uncertainties in BrC optical properties, and how they evolve with time and atmospheric processing, are understood so poorly that many climate models - including UK Met Office climate models - are devoid of any BrC representation. Thus, it is of paramount importance that our understanding of BrC optical properties is improved for better BrC representations in climate models.Traditional measurement approaches have shortcomings in measuring BrC optical properties accurately due to the relatively weak absorption by BrC. Moreover, common laboratory techniques for probing aerosol properties do not access the long ageing timescales of >50 hours that often pertain to atmospheric BrC. This work uses new state-of-the-art instruments available only in the UK to provide measurements of both light scattering and absorption by weakly absorbing aerosol with unrivalled accuracy, precision and sensitivity. Such tools include Single Particle Cavity Ring-Down Spectroscopy (SP-CRDS) and photoacoustic spectroscopy, with single particle trapping techniques such as SP-CRDS allowing measurements of aerosol optical properties on unlimited ageing timescales while particles are subjected to controlled ambient conditions. BrC optical properties will be measured during the BrC formation process and for subsequent ageing and atmospheric processing, such as changes in humidity, exposure to ultraviolet light and reaction with ozone. Furthermore, the proposal addresses both of the common BrC formation pathways, from reaction of gas precursors in aqueous droplets or from the heterogeneous reactions of gas precursors directly on particle surfaces. These results will be used to assess the sensitivity of aerosol-radiation models used at the UK Met Office to measured variations in BrC optical properties and to develop parameterisations of the ageing of BrC optical properties for comparison to recent field studies and future implementation in the next generation of climate models.
气溶胶是悬浮在气体中的液体或固体颗粒,在我们的大气中无处不在,其来源包括燃烧化石燃料产生的人为排放,以及海洋喷雾,沙漠灰尘和野火生物质燃烧等自然来源。这些气溶胶对我们的大气层有重大影响,通过与阳光和云滴相互作用,影响人类健康,例如烟雾事件和全球气候。事实上,气溶胶是预测未来气候变化的最大不确定因素之一。气溶胶将阳光散射回太空所产生的净气溶胶冷却效应,部分抵消了温室气体的变暖影响。然而,这种气溶胶-光相互作用的巨大不确定性降低了我们对未来气候模型的信心。提高我们对气溶胶-光相互作用的理解,可以导致更有效的风险缓解战略,在管理气候变化的影响。重要的参数来衡量限制气溶胶-光相互作用的估计是气溶胶的光散射和吸收的幅度。特别是,光吸收的碳质气溶胶的研究很少,一类气溶胶的光学特性称为棕色碳气溶胶(BrC)的理解非常少。BrC颗粒在生物质燃烧区域中容易形成,其中在燃烧期间排放的气态有机分子快速冷凝到液体或固体颗粒上,这些有机分子在颗粒表面或液体颗粒内部反应以形成光吸收发色团。随后的BrC颗粒具有强的波长依赖性吸收光谱,与较长的(红色)波长相比,在较短的(蓝色)光学波长处具有更强的吸收,从而产生棕色外观。此外,大气中的溴化碳由具有不同光吸收光谱的各种分子物种组成,而这些发色团的组成随着大气老化而显著变化。BrC光学性质的不确定性,以及它们如何随着时间和大气过程而演变,人们对许多气候模型(包括英国气象局气候模型)的理解非常有限,以至于没有任何BrC表示。因此,提高对BrC光学性质的认识,以便更好地在气候模式中描述BrC具有重要意义。由于BrC的吸收相对较弱,传统的测量方法在准确测量BrC光学性质方面存在不足。此外,用于探测气溶胶特性的普通实验室技术无法获得通常与大气BrC有关的>50小时的长老化时间尺度。这项工作使用仅在英国可用的最先进的仪器,以无与伦比的准确度,精度和灵敏度提供弱吸收气溶胶的光散射和吸收测量。这些工具包括单粒子腔衰荡光谱(SP-CRDS)和光声光谱,其中SP-CRDS等单粒子捕获技术允许在粒子经受受控环境条件的同时在无限老化时间尺度上测量气溶胶光学性质。将在溴化碳形成过程中以及随后的老化和大气处理过程中测量溴化碳的光学特性,例如湿度变化、暴露于紫外光以及与臭氧的反应。此外,该提案解决了两个共同的BrC形成途径,从反应的气体前体在水液滴或从气体前体直接在颗粒表面上的非均相反应。这些结果将被用来评估在英国气象局使用的气溶胶辐射模型的敏感性,以测量的变化,在BrC光学特性和开发参数化的老化BrC光学特性的比较,最近的实地研究和未来的实施,在下一代的气候模型。
项目成果
期刊论文数量(0)
专著数量(0)
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Michael Cotterell其他文献
Michael Cotterell的其他文献
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{{ truncateString('Michael Cotterell', 18)}}的其他基金
Light Absorption for Volatile Aerosol Particles: A New Measurement Approach
挥发性气溶胶颗粒的光吸收:一种新的测量方法
- 批准号:
NE/X000036/1 - 财政年份:2023
- 资助金额:
$ 17.63万 - 项目类别:
Research Grant
New Approaches for Measuring Accelerated Chemical Reactions in Single Aerosol Particles
测量单个气溶胶颗粒中加速化学反应的新方法
- 批准号:
EP/W009528/2 - 财政年份:2023
- 资助金额:
$ 17.63万 - 项目类别:
Research Grant
New Approaches for Measuring Accelerated Chemical Reactions in Single Aerosol Particles
测量单个气溶胶颗粒中加速化学反应的新方法
- 批准号:
EP/W009528/1 - 财政年份:2022
- 资助金额:
$ 17.63万 - 项目类别:
Research Grant
Accurate and Direct Measurements of Brown Carbon Aerosol Optical Properties During Formation and Atmospherically-Relevant Ageing Processes
准确、直接测量地层和大气相关老化过程中棕碳气溶胶的光学特性
- 批准号:
NE/S014314/1 - 财政年份:2019
- 资助金额:
$ 17.63万 - 项目类别:
Fellowship
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