Hopkins Rebecca J, Reid Jonathan P
School of Chemistry, University of Bristol, Cantock's Close, Bristol BS8 1TS, UK.
J Phys Chem A. 2005 Sep 8;109(35):7923-31. doi: 10.1021/jp0516543.
The evolving size, composition, and temperature of evaporating ethanol/water aerosol droplets 25-57 microm in radius are probed by cavity enhanced Raman scattering (CERS) and laser induced fluorescence. This represents the first study in which the evolving composition of volatile droplets has been probed with spatial selectivity on the millisecond time scale, providing a new strategy for exploring mass and heat transfer in aerosols. The Raman scattering intensity is shown to depend exponentially on species concentration due to the stimulated nature of the CERS technique, providing a sensitive measure of the concentration of the volatile ethanol component. The accuracy with which we can determine droplet size, composition, and temperature is discussed. We demonstrate that the CERS measurements of evolving size and composition of droplets falling in a train can be used to characterize, and thus avoid, droplet coagulation. By varying the surrounding gas pressure (7-77 kPa), we investigate the dependence of the rate of evaporation on the rate of gas diffusion, and behavior consistent with gas diffusion-limited evaporation is observed. We suggest that such measurements can allow the determination of the vapor pressures of components within the droplet and can allow the determination of activity coefficients of volatile species.
通过腔增强拉曼散射(CERS)和激光诱导荧光技术,对半径为25 - 57微米的乙醇/水蒸发气溶胶液滴不断变化的尺寸、成分和温度进行了探测。这是首次在毫秒时间尺度上对挥发性液滴不断变化的成分进行空间选择性探测的研究,为探索气溶胶中的质量和热传递提供了一种新策略。由于CERS技术的受激性质,拉曼散射强度显示出与物种浓度呈指数关系,为挥发性乙醇成分的浓度提供了灵敏的测量方法。讨论了我们确定液滴尺寸、成分和温度的精度。我们证明,对成串下落液滴不断变化的尺寸和成分进行的CERS测量可用于表征并避免液滴凝聚。通过改变周围气体压力(7 - 77千帕),我们研究了蒸发速率对气体扩散速率的依赖性,并观察到与气体扩散限制蒸发一致的行为。我们认为,此类测量能够确定液滴内各成分的蒸气压,并能够确定挥发性物种的活度系数。