Few-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles
Few-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles
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DOI：
10.1038/s41467-019-12580-0
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发表时间：
2019-10-11
影响因子：
16.6
通讯作者：
Kling, Matthias F.
中科院分区：
文献类型：
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作者：
Rupp, Philipp;Burger, Christian;Kling, Matthias F.
纳米粒子作为具有大表面积的光催化剂具有独特的性能。在光照射下，相关的近场可以诱导、增强和控制纳米级的分子吸附反应。然而，到目前为止，还没有简单的方法可以在空间上解析纳米颗粒表面的近场诱导反应产率。在这里，我们通过引入基于三维动量分辨光电离的反应纳米技术来缩小这一差距。该技术被证明可在 SiO2 纳米颗粒上的少周期激光诱导乙醇和水解离电离中产生空间选择性质子，从而解决了颗粒表面的显着变化。通过静电和准经典平均场 Mie Monte-Carlo ((MC)-C-3) 计算对结果进行定性建模和再现。反应纳米显微镜适用于各种孤立的纳米系统，可以提供纳米颗粒、簇和液滴的空间分辨超快反应动力学。
Nanoparticles offer unique properties as photocatalysts with large surface areas. Under irradiation with light, the associated near-fields can induce, enhance, and control molecular adsorbate reactions on the nanoscale. So far, however, there is no simple method available to spatially resolve the near-field induced reaction yield on the surface of nanoparticles. Here we close this gap by introducing reaction nanoscopy based on three-dimensional momentum-resolved photoionization. The technique is demonstrated for the spatially selective proton generation in few-cycle laser-induced dissociative ionization of ethanol and water on SiO2 nanoparticles, resolving a pronounced variation across the particle surface. The results are modeled and reproduced qualitatively by electrostatic and quasi-classical mean-field Mie Monte-Carlo ((MC)-C-3) calculations. Reaction nanoscopy is suited for a wide range of isolated nanosystems and can provide spatially resolved ultrafast reaction dynamics on nanoparticles, clusters, and droplets.