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Photomodulated Spatially Confined Chemical Reactivity in a Single Silver Nanoprism.

Authors
  • Bhanushali, Sushrut1
  • Mahasivam, Sanje2
  • Ramanathan, Rajesh2
  • Singh, Mandeep2
  • Harrop Mayes, Edwin Lawrence3
  • Murdoch, Billy James3
  • Bansal, Vipul2
  • Sastry, Murali1, 4
  • 1 Department of Materials Science and Engineering, Monash University, Clayton, Victoria 3800, Australia. , (Australia)
  • 2 Ian Potter NanoBioSensing Facility, NanoBiotechnology Research Laboratory, School of Science, RMIT University, Melbourne, Victoria 3001, Australia. , (Australia)
  • 3 RMIT Microscopy and Microanalysis Facility, College of Science, Engineering & Health, RMIT University, Melbourne, Victoria 3001, Australia. , (Australia)
  • 4 IITB-Monash Research Academy, Indian Institute of Technology Bombay, Mumbai 400076, India. , (India)
Type
Published Article
Journal
ACS Nano
Publisher
American Chemical Society
Publication Date
Aug 24, 2020
Identifiers
DOI: 10.1021/acsnano.0c00966
PMID: 32790283
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

Single-atom and single-particle catalysis is an area of considerable topical interest due to their potential in explaining important fundamental processes and applications across several areas. An interesting avenue in single-particle catalysis is spatial control of chemical reactivity within the particle by employing light as an external stimulus. To demonstrate this concept, we report galvanic replacement reactions (GRRs) as a spatial marker of subparticle chemical reactivity of a silver nanoprism with AuCl4- ions under optical excitation. The location of a GRR within a single Ag nanoprism can be spatially controlled depending on the plasmon mode excited. This leads to chemomorphological transformation of Ag nanoprisms into interesting Ag-Au structures. This spatial biasing effect is attributed to localized hot electron injection from the tips and edges of the silver nanoprisms to the adjacent reactants that correlate with excitation of different surface plasmon modes. The study also employs low-energy-loss EELS mapping to additionally probe the spatially confined redox reaction within a silver nanoprism. The findings presented here allow the visualization of a plasmon-driven subparticle chemical transformation with high resolution. The selective optical excitation of surface plasmon eigenmodes of anisotropic nanoparticles offers opportunities to spatially modulate chemical transformations mediated by hot electron transfer.

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