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Title: Polyvinylpyrrolidone-induced anisotropic growth of gold nanoprisms in plasmon-driven synthesis

After more than a decade, it is still unknown whether the plasmon-mediated growth of silver nanostructures can be extended to the synthesis of other noble metals, as the molecular mechanisms governing the growth process remain elusive. In this paper, we demonstrate the plasmon-driven synthesis of gold nanoprisms and elucidate the details of the photochemical growth mechanism at the single-nanoparticle level. Our investigation reveals that the surfactant polyvinylpyrrolidone preferentially adsorbs along the nanoprism perimeter and serves as a photochemical relay to direct the anisotropic growth of gold nanoprisms. This discovery confers a unique function to polyvinylpyrrolidone that is fundamentally different from its widely accepted role as a crystal-face-blocking ligand. Additionally, we find that nanocrystal twinning exerts a profound influence on the kinetics of this photochemical process by controlling the transport of plasmon-generated hot electrons to polyvinylpyrrolidone. Finally, these insights establish a molecular-level description of the underlying mechanisms regulating the plasmon-driven synthesis of gold nanoprisms.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [4] ; ORCiD logo [3] ; ORCiD logo [3] ;  [4] ;  [1]
  1. Univ. of Florida, Gainesville, FL (United States). Dept. of Chemistry. Center for Nanostructured Electronic Materials
  2. Univ. of Florida, Gainesville, FL (United States). Dept. of Chemistry. Center for Nanostructured Electronic Materials; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.
Publication Date:
Report Number(s):
BNL-113407-2017-JA
Journal ID: ISSN 1476-1122; R&D Project: 16060; 16060; KC0403020; TRN: US1701804
Grant/Contract Number:
SC0012704; AC06-76RLO1930; FA9550-14-1-0304; CHE-1308644; CHE-1038015
Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 15; Journal Issue: 8; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Florida, Gainesville, FL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Center for Functional Nanomaterials; nanoparticles
OSTI Identifier:
1341679