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Rupp, Philipp; Burger, Christian; Kling, Nora G.; Kuebel, Matthias; Mitra, Sambit; Rosenberger, Philipp; Weatherby, Thomas; Saito, Nariyuki; Itatani, Jiro; Alnaser, Ali S.; Raschke, Markus B.; Ruehl, Eckart; Schlander, Annika; Gallei, Markus; Seiffert, Lennart; Fennel, Thomas; Bergues, Boris und Kling, Matthias F. (2019): Few-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles. In: Nature Communications, Bd. 10, 4655 [PDF, 2MB]

Abstract

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.

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