Monitoring plasmonic hot-carrier chemical reactions at the single particle level

Faraday Discussions
Sabrina SimoncelliEmiliano Cortés

Abstract

Plasmon excitation in metal nanoparticles triggers the generation of highly energetic charge carriers that, when properly manipulated and exploited, can mediate chemical reactions. Single-particle techniques are key to unearthing the underlying mechanisms of hot-carrier generation, transport and injection, as well as to disentangling the role of the temperature increase and the enhanced near-field at the nanoparticle-molecule interface. Gaining nanoscopic insight into these processes and their interplay could aid in the rational design of plasmonic photocatalysts. Here, we present three different approaches to monitor hot-carrier reactivity at the single-particle level. We use a combination of dark-field microscopy and photoelectrochemistry to track a hot-hole driven reaction on a single Au nanoparticle. We image hot-electron reactivity with sub-particle spatial resolution using nanoscopy techniques. Finally, we push the limits by looking for a hot-electron induced chemical reaction that generates a fluorescent product, which should enable imaging plasmonic photocatalysis at the single-particle and single-molecule levels.

References

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Citations

Oct 18, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·William O F Carvalho, J R Mejía-Salazar
Feb 24, 2021·Analytical Chemistry·Peng Fei GaoCheng Zhi Huang
Aug 8, 2021·International Journal of Molecular Sciences·Yingxia GaoLéon Sanche
Aug 21, 2019·Accounts of Chemical Research·Julian GargiuloEmiliano Cortés
May 18, 2019·The Journal of Physical Chemistry Letters·Yanfang DongLéon Sanche
Dec 15, 2020·ACS Nano·Emiliano CortésPrineha Narang
Nov 13, 2021·Photochemistry and Photobiology·Chaochao LiuLéon Sanche

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Methods Mentioned

BETA
fluorescence microscopy
super-resolution nanoscopy
Fluorescence
electron beam lithography
scanning electron microscopy

Software Mentioned

Lumerical FDTD 2017a
PAINT
rainSTORM
Matlab
Comsol Multiphysics
Matlab application

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