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Title: Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis

Abstract

Plasmonic metal nanoparticles enhance chemical reactions on their surface when illuminated with light of particular frequencies. It has been shown that these processes are driven by excitation of localized surface plasmon resonance (LSPR). The interaction of LSPR with adsorbate orbitals can lead to the injection of energized charge carriers into the adsorbate, which can result in chemical transformations. The mechanism of the charge injection process (and role of LSPR) is not well understood. Here we shed light on the specifics of this mechanism by coupling optical characterization methods, mainly wavelength-dependent Stokes and anti-Stokes SERS, with kinetic analysis of photocatalytic reactions in an Ag nanocube–methylene blue plasmonic system. We propose that localized LSPR-induced electric fields result in a direct charge transfer within the molecule–adsorbate system. Lastly, these observations provide a foundation for the development of plasmonic catalysts that can selectively activate targeted chemical bonds, since the mechanism allows for tuning plasmonic nanomaterials in such a way that illumination can selectively enhance desired chemical pathways.

Authors:
 [1];  [1];  [1];  [1]
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  1. Univ. of Michigan, Ann Arbor, MI (United States)
Publication Date:
Research Org.:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1242978
Grant/Contract Number:  
FG02-05ER15686
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; chemical sciences; catalysis; physical chemistry

Citation Formats

Boerigter, Calvin, Campana, Robert, Morabito, Matthew, and Linic, Suljo. Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis. United States: N. p., 2016. Web. doi:10.1038/ncomms10545.
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Boerigter, Calvin, Campana, Robert, Morabito, Matthew, & Linic, Suljo. Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis. United States. https://doi.org/10.1038/ncomms10545
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Boerigter, Calvin, Campana, Robert, Morabito, Matthew, and Linic, Suljo. Thu . "Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis". United States. https://doi.org/10.1038/ncomms10545. https://www.osti.gov/servlets/purl/1242978.
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@article{osti_1242978,
title = {Evidence and implications of direct charge excitation as the dominant mechanism in plasmon-mediated photocatalysis},
author = {Boerigter, Calvin and Campana, Robert and Morabito, Matthew and Linic, Suljo},
abstractNote = {Plasmonic metal nanoparticles enhance chemical reactions on their surface when illuminated with light of particular frequencies. It has been shown that these processes are driven by excitation of localized surface plasmon resonance (LSPR). The interaction of LSPR with adsorbate orbitals can lead to the injection of energized charge carriers into the adsorbate, which can result in chemical transformations. The mechanism of the charge injection process (and role of LSPR) is not well understood. Here we shed light on the specifics of this mechanism by coupling optical characterization methods, mainly wavelength-dependent Stokes and anti-Stokes SERS, with kinetic analysis of photocatalytic reactions in an Ag nanocube–methylene blue plasmonic system. We propose that localized LSPR-induced electric fields result in a direct charge transfer within the molecule–adsorbate system. Lastly, these observations provide a foundation for the development of plasmonic catalysts that can selectively activate targeted chemical bonds, since the mechanism allows for tuning plasmonic nanomaterials in such a way that illumination can selectively enhance desired chemical pathways.},
doi = {10.1038/ncomms10545},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Thu Jan 28 00:00:00 EST 2016},
month = {Thu Jan 28 00:00:00 EST 2016}
}
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https://doi.org/10.1038/ncomms10545
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    The UV Plasmonic Behavior of Distorted Rhodium Nanocubes
    journal, December 2017

    • Gutiérrez, Yael; Ortiz, Dolores; Saiz, José
    • Nanomaterials, Vol. 7, Issue 12
    • DOI: 10.3390/nano7120425

    Mechanistic Studies of Plasmon Chemistry on Metal Catalysts
    journal, April 2019

    Plasmonic Surface Lattice Resonances: A Review of Properties and Applications
    journal, June 2018

    Structural and Optical Properties of Discrete Dendritic Pt Nanoparticles on Colloidal Au Nanoprisms
    journal, May 2016

    • Leary, Rowan K.; Kumar, Anjli; Straney, Patrick J.
    • The Journal of Physical Chemistry C, Vol. 120, Issue 37
    • DOI: 10.1021/acs.jpcc.6b02103

    Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation
    journal, February 2017

    • Zhang, Xiao; Li, Xueqian; Zhang, Du
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14542

    Plasmonic photoluminescence for recovering native chemical information from surface-enhanced Raman scattering
    journal, March 2017

    • Lin, Kai-Qiang; Yi, Jun; Zhong, Jin-Hui
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14891

    Atomic dispensers for thermoplasmonic control of alkali vapor pressure in quantum optical applications
    journal, May 2019

    • Rusimova, Kristina R.; Slavov, Dimitar; Pradaux-Caggiano, Fabienne
    • Nature Communications, Vol. 10, Issue 1
    • DOI: 10.1038/s41467-019-10158-4

    The UV Plasmonic Behavior of Distorted Rhodium Nanocubes
    journal, December 2017

    • Gutiérrez, Yael; Ortiz, Dolores; Saiz, José
    • Nanomaterials, Vol. 7, Issue 12
    • DOI: 10.3390/nano7120425

    Pulsed laser synthesis of highly active Ag–Rh and Ag–Pt antenna–reactor-type plasmonic catalysts
    journal, September 2019

    • Kane, Kenneth A.; Bertino, Massimo F.
    • Beilstein Journal of Nanotechnology, Vol. 10
    • DOI: 10.3762/bjnano.10.192

    Silver-copper oxide heteronanostructures for the plasmonic-enhanced photocatalytic oxidation of N-hexane in the visible-NIR range
    text, January 2019

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