论文标题
从亚波长丙二醇滴的离子发射的反应纳米镜检查
Reaction Nanoscopy of Ion Emission from Sub-wavelength Propanediol Droplets
论文作者
论文摘要
液滴为研究激光诱导的表面化学反应提供了独特的机会。带电液滴表面上的化学反应本质上是普遍存在的,可以为工业化学生产的更有效的过程提供关键的见解。在这里,我们证明了反应纳米镜技术在丙二醇(PDO)的强场离子化纳米圆形中的应用。该技术对液滴周围近场的敏感性允许平均液滴尺寸和电荷的原位表征。使用超短激光脉冲可以通过激光强度控制表面电荷的量。此外,我们通过比较异构体1,2-PDO和1,3-PDO的离子发射和片段化通道的液滴来证明反应纳米镜检查的表面化学敏感性。将离子产量引用到气相数据中,我们发现从1,2-PDO异构体的液滴中增强了甲基阳离子的产生。密度功能理论模拟支持这种增强是由于表面上1,2-PDO分子的比对。结果铺平了泵探针研究中液滴的电荷动力学和表面反应的时空观察的道路。
Droplets provide unique opportunities for the investigation of laser-induced surface chemistry. Chemical reactions on the surface of charged droplets are ubiquitous in nature and can provide critical insight into more efficient processes for industrial chemical production. Here, we demonstrate the application of the reaction nanoscopy technique to strong-field ionized nanodroplets of propanediol (PDO). The technique's sensitivity to the near-field around the droplet allows for the in-situ characterization of the average droplet size and charge. The use of ultrashort laser pulses enables control of the amount of surface charge by the laser intensity. Moreover, we demonstrate the surface chemical sensitivity of reaction nanoscopy by comparing droplets of the isomers 1,2-PDO and 1,3-PDO in their ion emission and fragmentation channels. Referencing the ion yields to gas-phase data, we find an enhanced production of methyl cations from droplets of the 1,2-PDO isomer. Density functional theory simulations support that this enhancement is due to the alignment of 1,2-PDO molecules on the surface. The results pave the way towards spatio-temporal observations of charge dynamics and surface reactions on droplets in pump-probe studies.