Quantifying Wavelength-Dependent Plasmonic Hot Carrier Energy Distributions at Metal/Semiconductor Interfaces
Abstract
Hot carriers generated from the nonradiative decay of localized surface plasmons are capable of driving charge-transfer reactions at the surfaces of metal nanostructures. Photocatalytic devices utilizing plasmonic hot carriers are often based on metal nanoparticle/semiconductor heterostructures owing to their efficient electron–hole separation ability. The rapid thermalization of hot carriers generated at the metal nanoparticles yields a distribution of carrier energies that determines the capability of the photocatalytic device to drive redox reactions. Here in this paper, we quantify the thermalized hot carrier energy distribution generated at Au/TiO2 nanostructures using wavelength-dependent scanning electrochemical microscopy and a series of molecular probes with different redox potentials. We determine the quantum efficiencies and oxidizing power of the hot carriers from wavelength-dependent reaction rates and photocurrent across the metal/semiconductor interface. The wavelength-dependent reaction efficiency tracks the surface plasmon resonance spectrum of the Au nanoparticles, showing that the reaction is facilitated by plasmon excitation, while the responses from molecules with different redox potentials shed light on the energy distribution of the hot holes generated at metal nanoparticle/semiconductor heterostructures. The results provide important insight into the energies of the plasmon-generated hot carriers and quantum efficiencies of plasmonic photocatalytic devices.
- Authors:
-
- Temple Univ., Philadelphia, PA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Temple Univ., Philadelphia, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1608032
- Grant/Contract Number:
- SC0012575
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 3; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; plasmon; hot-hole; hot carriers
Citation Formats
Yu, Yun, Wijesekara, Kanishka D., Xi, Xiaoxing, and Willets, Katherine A. Quantifying Wavelength-Dependent Plasmonic Hot Carrier Energy Distributions at Metal/Semiconductor Interfaces. United States: N. p., 2019.
Web. doi:10.1021/acsnano.9b00219.
Yu, Yun, Wijesekara, Kanishka D., Xi, Xiaoxing, & Willets, Katherine A. Quantifying Wavelength-Dependent Plasmonic Hot Carrier Energy Distributions at Metal/Semiconductor Interfaces. United States. https://doi.org/10.1021/acsnano.9b00219
Yu, Yun, Wijesekara, Kanishka D., Xi, Xiaoxing, and Willets, Katherine A. Tue .
"Quantifying Wavelength-Dependent Plasmonic Hot Carrier Energy Distributions at Metal/Semiconductor Interfaces". United States. https://doi.org/10.1021/acsnano.9b00219. https://www.osti.gov/servlets/purl/1608032.
@article{osti_1608032,
title = {Quantifying Wavelength-Dependent Plasmonic Hot Carrier Energy Distributions at Metal/Semiconductor Interfaces},
author = {Yu, Yun and Wijesekara, Kanishka D. and Xi, Xiaoxing and Willets, Katherine A.},
abstractNote = {Hot carriers generated from the nonradiative decay of localized surface plasmons are capable of driving charge-transfer reactions at the surfaces of metal nanostructures. Photocatalytic devices utilizing plasmonic hot carriers are often based on metal nanoparticle/semiconductor heterostructures owing to their efficient electron–hole separation ability. The rapid thermalization of hot carriers generated at the metal nanoparticles yields a distribution of carrier energies that determines the capability of the photocatalytic device to drive redox reactions. Here in this paper, we quantify the thermalized hot carrier energy distribution generated at Au/TiO2 nanostructures using wavelength-dependent scanning electrochemical microscopy and a series of molecular probes with different redox potentials. We determine the quantum efficiencies and oxidizing power of the hot carriers from wavelength-dependent reaction rates and photocurrent across the metal/semiconductor interface. The wavelength-dependent reaction efficiency tracks the surface plasmon resonance spectrum of the Au nanoparticles, showing that the reaction is facilitated by plasmon excitation, while the responses from molecules with different redox potentials shed light on the energy distribution of the hot holes generated at metal nanoparticle/semiconductor heterostructures. The results provide important insight into the energies of the plasmon-generated hot carriers and quantum efficiencies of plasmonic photocatalytic devices.},
doi = {10.1021/acsnano.9b00219},
journal = {ACS Nano},
number = 3,
volume = 13,
place = {United States},
year = {Tue Feb 26 00:00:00 EST 2019},
month = {Tue Feb 26 00:00:00 EST 2019}
}
Web of Science
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