Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog Weg 2, CH-8093 Zürich, Switzerland.
J Chem Phys. 2016 Dec 7;145(21):211907. doi: 10.1063/1.4960050.
We report on molecular-level studies of the condensation of propane gas and propane/ethane gas mixtures in the uniform (constant pressure and temperature) postnozzle flow of Laval expansions using soft single-photon ionization by vacuum ultraviolet light and mass spectrometric detection. The whole process, from the nucleation to the growth to molecular aggregates of sizes of several nanometers (∼5 nm), can be monitored at the molecular level with high time-resolution (∼3 μs) for a broad range of pressures and temperatures. For each time, pressure, and temperature, a whole mass spectrum is recorded, which allows one to determine the critical cluster size range for nucleation as well as the kinetics and mechanisms of cluster-size specific growth. The detailed information about the size, composition, and population of individual molecular clusters upon condensation provides unique experimental data for comparison with future molecular-level simulations.
我们报告了在使用真空紫外软单光子电离和质谱检测的拉瓦尔膨胀后喷嘴均匀(恒压和恒温)流中,对丙烷气体和丙烷/乙烷气体混合物的冷凝进行的分子水平研究。整个过程,从成核到生长到几个纳米(约 5nm)大小的分子聚集体,都可以在分子水平上进行监测,具有高时间分辨率(约 3μs),适用于广泛的压力和温度范围。对于每个时间、压力和温度,都会记录整个质谱,这允许确定成核的临界团簇尺寸范围以及团簇尺寸特定生长的动力学和机制。关于冷凝时单个分子团簇的大小、组成和分布的详细信息为与未来的分子水平模拟进行比较提供了独特的实验数据。