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Title: Hot Holes Assist Plasmonic Nanoelectrode Dissolution

Abstract

Strong light-absorbing properties allow plasmonic metal nanoparticles to serve as antennas for other catalysts to function as photocatalysts. To achieve plasmonic photocatalysis, the hot charge carriers created when light is absorbed must be harnessed before they decay through internal relaxation pathways. We demonstrate the role of photogenerated hot holes in the oxidative dissolution of individual gold nanorods with millisecond time resolution while tuning charge-carrier density and photon energy using snapshot hyperspectral imaging. In this work, we show that light-induced hot charge carriers enhance the rate of gold oxidation and subsequent electrodissolution. Importantly, we distinguish how hot holes generated from interband transitions versus hot holes around the Fermi level contribute to photooxidative dissolution. The results provide new insights into hot-hole-driven processes with relevance to photocatalysis while emphasizing the need for statistical descriptions of nonequilibrium processes on innately heterogeneous nanoparticle supports.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [2]
  1. Rice Univ., Houston, TX (United States)
  2. Rice Univ., Houston, TX (United States). Smalley-Curl Inst.
Publication Date:
Research Org.:
Rice Univ., Houston, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1595785
Grant/Contract Number:  
SC0016534
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 19; Journal Issue: 2; Related Information: 10.1021/acs.nanolett.8b04894; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Scattering; Dissolution; Light; Nanorods; Lasers; Nanoantenna; photocatalysis; electrodissolution; hot carrier dynamics; interband transitions; snapshot hyperspectral imaging

Citation Formats

Al-Zubeidi, Alexander, Hoener, Benjamin S., Collins, Sean S. E., Wang, Wenxiao, Kirchner, Silke R., Hosseini Jebeli, Seyyed Ali, Joplin, Anneli, Chang, Wei-Shun, Link, Stephan, and Landes, Christy F. Hot Holes Assist Plasmonic Nanoelectrode Dissolution. United States: N. p., 2019. Web. doi:10.1021/acs.nanolett.8b04894.
Al-Zubeidi, Alexander, Hoener, Benjamin S., Collins, Sean S. E., Wang, Wenxiao, Kirchner, Silke R., Hosseini Jebeli, Seyyed Ali, Joplin, Anneli, Chang, Wei-Shun, Link, Stephan, & Landes, Christy F. Hot Holes Assist Plasmonic Nanoelectrode Dissolution. United States. https://doi.org/10.1021/acs.nanolett.8b04894
Al-Zubeidi, Alexander, Hoener, Benjamin S., Collins, Sean S. E., Wang, Wenxiao, Kirchner, Silke R., Hosseini Jebeli, Seyyed Ali, Joplin, Anneli, Chang, Wei-Shun, Link, Stephan, and Landes, Christy F. Tue . "Hot Holes Assist Plasmonic Nanoelectrode Dissolution". United States. https://doi.org/10.1021/acs.nanolett.8b04894. https://www.osti.gov/servlets/purl/1595785.
@article{osti_1595785,
title = {Hot Holes Assist Plasmonic Nanoelectrode Dissolution},
author = {Al-Zubeidi, Alexander and Hoener, Benjamin S. and Collins, Sean S. E. and Wang, Wenxiao and Kirchner, Silke R. and Hosseini Jebeli, Seyyed Ali and Joplin, Anneli and Chang, Wei-Shun and Link, Stephan and Landes, Christy F.},
abstractNote = {Strong light-absorbing properties allow plasmonic metal nanoparticles to serve as antennas for other catalysts to function as photocatalysts. To achieve plasmonic photocatalysis, the hot charge carriers created when light is absorbed must be harnessed before they decay through internal relaxation pathways. We demonstrate the role of photogenerated hot holes in the oxidative dissolution of individual gold nanorods with millisecond time resolution while tuning charge-carrier density and photon energy using snapshot hyperspectral imaging. In this work, we show that light-induced hot charge carriers enhance the rate of gold oxidation and subsequent electrodissolution. Importantly, we distinguish how hot holes generated from interband transitions versus hot holes around the Fermi level contribute to photooxidative dissolution. The results provide new insights into hot-hole-driven processes with relevance to photocatalysis while emphasizing the need for statistical descriptions of nonequilibrium processes on innately heterogeneous nanoparticle supports.},
doi = {10.1021/acs.nanolett.8b04894},
journal = {Nano Letters},
number = 2,
volume = 19,
place = {United States},
year = {Tue Jan 08 00:00:00 EST 2019},
month = {Tue Jan 08 00:00:00 EST 2019}
}

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Cited by: 52 works
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Works referencing / citing this record:

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