Direct Spectroscopic Quantification of the Absorption and Scattering Properties for Single Aerosol Particles.

Direct Spectroscopic Quantification of the Absorption and Scattering Properties for Single Aerosol Particles.
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单个气溶胶颗粒的吸收和散射特性的直接光谱定量。

DOI:
10.1021/acs.jpca.2c00532
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发表时间:
2022-03-10
影响因子:
2.9
通讯作者:
Cotterell, Michael, I
Cotterell, Michael, I
中科院分区:
化学3区
文献类型:
--
作者:
Knight, Jamie W.;Egan, Joanna, V;Orr-Ewing, Andrew J.;Cotterell, Michael, I

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了解微米级吸光气溶胶颗粒的光学特性对于应对大气和物理化学方面的关键挑战至关重要。例如,大气气溶胶对太阳辐射的吸收是气候模型中最大的不确定性之一。此外,在气溶胶液滴的独特环境中的反应加速不能在本体溶液中复制。这些反应速率增强的原因仍然存在争议,但不断变化的气溶胶光学特性的超灵敏光谱测量应该提供新的见解。我们展示了一种新的方法,使用腔衰荡光谱,允许第一次直接光谱量化的连续不断发展的吸收和散射截面为单一的,悬浮的,微米级的颗粒,因为它们的大小和发色团浓度的变化。对于由苯胺黑和1,2,6-己三醇组成的双组分液滴,我们测量的前所未有的灵敏度揭示了随着1,2,6-己三醇缓慢蒸发而由浓度变化引起的折射率的演变的真实的和虚的分量。
Understanding the optical properties of micrometer-scale light-absorbing aerosol particles is of paramount importance in addressing key challenges in atmospheric and physical chemistry. For example, the absorption of solar radiation by atmospheric aerosols represents one of the largest uncertainties in climate models. Moreover, reaction acceleration within the unique environments of aerosol droplets cannot be replicated in bulk solutions. The causes of these reaction rate enhancements remain controversial, but ultrasensitive spectroscopic measurements of evolving aerosol optical properties should provide new insights. We demonstrate a new approach using cavity ring-down spectroscopy that allows the first direct spectroscopic quantification of the continuously evolving absorption and scattering cross sections for single, levitated, micrometer-scale particles as their size and chromophore concentration change. For two-component droplets composed of nigrosin and 1,2,6-hexanetriol, the unprecedented sensitivity of our measurements reveals the evolving real and imaginary components of the refractive index caused by changes in concentration as 1,2,6-hexanetriol slowly evaporates.
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