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Title: Ultrafast relaxation dynamics in bimetallic plasmonic catalysts

Abstract

Combining a plasmonic metal, such as gold, with other popular catalysts, such as Ni or Pt, can extend its benefits to many energy-extensive reactions catalyzed by those metals. The efficiency of a plasmon-enhanced catalytic reaction is mainly determined by the light absorption cross section and the photoexcited charge carrier relaxation dynamics of the nanoparticles. Here we have investigated the charge carrier relaxation dynamics of gold/nickel (Au/Ni) and gold/platinum (Au/Pt) bimetallic nanoparticles. We found that the addition of Ni or Pt to gold can reduce light absorption in gold nanoparticles. However, electron–phonon coupling rates of Au/Ni and Au/Pt nanoparticles are significantly faster than that of pure Au nanoparticles. This is due to the fact that both Ni and Pt possess significantly larger electron–phonon coupling constants and higher densities of states near the Fermi level in comparison with Au. Additionally, the phonon–phonon coupling rate of bimetallic Au/Pt and Au/Ni nanoparticles was significantly different from that of pure gold nanoparticles, due to the acoustic impedance mismatch at the nanoparticle/substrate interface. Our findings provide important insights into the rational design of bimetallic plasmonic catalysts.

Authors:
 [1];  [2];  [2];  [2]; ORCiD logo [3]; ORCiD logo [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); Hanyang Univ., Ansan (Korea, Republic of)
  2. New Mexico Institute of Mining and Technology, Socorro, NM (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1739983
Alternate Identifier(s):
OSTI ID: 1617063
Report Number(s):
LA-UR-20-20520
Journal ID: ISSN 2040-3364
Grant/Contract Number:  
89233218CNA000001; AC52-06NA25396; NA-0003525
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 12; Journal Issue: 18; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sim, Sangwan, Beierle, Alyssa, Mantos, Philip, McCrory, Steven, Prasankumar, Rohit P., and Chowdhury, Sanchari. Ultrafast relaxation dynamics in bimetallic plasmonic catalysts. United States: N. p., 2020. Web. doi:10.1039/d0nr00831a.
Sim, Sangwan, Beierle, Alyssa, Mantos, Philip, McCrory, Steven, Prasankumar, Rohit P., & Chowdhury, Sanchari. Ultrafast relaxation dynamics in bimetallic plasmonic catalysts. United States. https://doi.org/10.1039/d0nr00831a
Sim, Sangwan, Beierle, Alyssa, Mantos, Philip, McCrory, Steven, Prasankumar, Rohit P., and Chowdhury, Sanchari. Mon . "Ultrafast relaxation dynamics in bimetallic plasmonic catalysts". United States. https://doi.org/10.1039/d0nr00831a. https://www.osti.gov/servlets/purl/1739983.
@article{osti_1739983,
title = {Ultrafast relaxation dynamics in bimetallic plasmonic catalysts},
author = {Sim, Sangwan and Beierle, Alyssa and Mantos, Philip and McCrory, Steven and Prasankumar, Rohit P. and Chowdhury, Sanchari},
abstractNote = {Combining a plasmonic metal, such as gold, with other popular catalysts, such as Ni or Pt, can extend its benefits to many energy-extensive reactions catalyzed by those metals. The efficiency of a plasmon-enhanced catalytic reaction is mainly determined by the light absorption cross section and the photoexcited charge carrier relaxation dynamics of the nanoparticles. Here we have investigated the charge carrier relaxation dynamics of gold/nickel (Au/Ni) and gold/platinum (Au/Pt) bimetallic nanoparticles. We found that the addition of Ni or Pt to gold can reduce light absorption in gold nanoparticles. However, electron–phonon coupling rates of Au/Ni and Au/Pt nanoparticles are significantly faster than that of pure Au nanoparticles. This is due to the fact that both Ni and Pt possess significantly larger electron–phonon coupling constants and higher densities of states near the Fermi level in comparison with Au. Additionally, the phonon–phonon coupling rate of bimetallic Au/Pt and Au/Ni nanoparticles was significantly different from that of pure gold nanoparticles, due to the acoustic impedance mismatch at the nanoparticle/substrate interface. Our findings provide important insights into the rational design of bimetallic plasmonic catalysts.},
doi = {10.1039/d0nr00831a},
journal = {Nanoscale},
number = 18,
volume = 12,
place = {United States},
year = {Mon Apr 13 00:00:00 EDT 2020},
month = {Mon Apr 13 00:00:00 EDT 2020}
}

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