Harvesting multiple electron-hole pairs generated through plasmonic excitation of Au nanoparticles

Youngsoo Kim, Jeremy G. Smith, Prashant K. Jain

Research output: Contribution to journalArticle

Abstract

Multi-electron redox reactions, although central to artificial photosynthesis, are kinetically sluggish. Amidst the search for synthetic catalysts for such processes, plasmonic nanoparticles have been found to catalyse multi-electron reduction of CO2 under visible light. This example motivates the need for a general, insight-driven framework for plasmonic catalysis of such multi-electron chemistry. Here, we elucidate the principles underlying the extraction of multiple redox equivalents from a plasmonic photocatalyst. We measure the kinetics of electron harvesting from a gold nanoparticle photocatalyst as a function of photon flux. Our measurements, supported by theoretical modelling, reveal a regime where two-electron transfer from the excited gold nanoparticle becomes prevalent. Multiple electron harvesting becomes possible under continuous-wave, visible-light excitation of moderate intensity due to strong interband transitions in gold and electron-hole separation accomplished using a hole scavenger. These insights will help expand the utility of plasmonic photocatalysis beyond CO2 reduction to other challenging multi-electron, multi-proton transformations such as N2 fixation.

Original languageEnglish (US)
Pages (from-to)763-769
Number of pages7
JournalNature Chemistry
Volume10
Issue number7
DOIs
StatePublished - Jul 1 2018

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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