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Title: Plasmonic Hot Hole Transfer in Gold Nanoparticle-Decorated Transition Metal Dichalcogenide Nanosheets

Abstract

This work studies photogenerated carrier dynamics in gold nanoparticle (AuNP)-decorated mono- to few-layer transition metal dichalcogenide (TMD) nanosheets using transient absorption spectroscopy (TA). TA unveiled the presence of a long-lived photoinduced absorption (PIA) feature in both MoSe2 and WSe2 decorated with covalently bound AuNPs. This long-lived PIA feature emerges only from direct Au interband excitation in AuNP-decorated MoSe2 and WSe2; it does not manifest from intraband excitation nor in AuNP-decorated MoS2 or WS2. Based on X-ray/ultraviolet photoelectron spectroscopy and previous theoretical studies, it is proposed that this PIA signature arises from hot hole transfer from the AuNP to the adjacent TMD, producing a charge-separated state. This suggests charge separation at the metal-semiconductor interface may be used to extend the lifetime of interband excitation generated hot holes. We conclude this development could represent an important advance in harnessing plasmonic dissipation pathways to generate long-lived carriers suited for solar-driven light harvesting and catalysis.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center; Boston College, Chestnut Hill, MA (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1593691
Report Number(s):
NREL/JA-5900-74989
Journal ID: ISSN 2330-4022; TRN: US2102027
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Photonics
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2330-4022
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; hot carriers; molybdenum diselenide; transient absorption; ultrafast spectroscopy; carrier dynamics; interband transitions; intraband

Citation Formats

Dunklin, Jeremy R., Rose, Aaron H., Zhang, Hanyu, Link, Elisa M., and van de Lagemaat, Jao. Plasmonic Hot Hole Transfer in Gold Nanoparticle-Decorated Transition Metal Dichalcogenide Nanosheets. United States: N. p., 2019. Web. doi:10.1021/acsphotonics.9b01393.
Dunklin, Jeremy R., Rose, Aaron H., Zhang, Hanyu, Link, Elisa M., & van de Lagemaat, Jao. Plasmonic Hot Hole Transfer in Gold Nanoparticle-Decorated Transition Metal Dichalcogenide Nanosheets. United States. https://doi.org/10.1021/acsphotonics.9b01393
Dunklin, Jeremy R., Rose, Aaron H., Zhang, Hanyu, Link, Elisa M., and van de Lagemaat, Jao. Tue . "Plasmonic Hot Hole Transfer in Gold Nanoparticle-Decorated Transition Metal Dichalcogenide Nanosheets". United States. https://doi.org/10.1021/acsphotonics.9b01393. https://www.osti.gov/servlets/purl/1593691.
@article{osti_1593691,
title = {Plasmonic Hot Hole Transfer in Gold Nanoparticle-Decorated Transition Metal Dichalcogenide Nanosheets},
author = {Dunklin, Jeremy R. and Rose, Aaron H. and Zhang, Hanyu and Link, Elisa M. and van de Lagemaat, Jao},
abstractNote = {This work studies photogenerated carrier dynamics in gold nanoparticle (AuNP)-decorated mono- to few-layer transition metal dichalcogenide (TMD) nanosheets using transient absorption spectroscopy (TA). TA unveiled the presence of a long-lived photoinduced absorption (PIA) feature in both MoSe2 and WSe2 decorated with covalently bound AuNPs. This long-lived PIA feature emerges only from direct Au interband excitation in AuNP-decorated MoSe2 and WSe2; it does not manifest from intraband excitation nor in AuNP-decorated MoS2 or WS2. Based on X-ray/ultraviolet photoelectron spectroscopy and previous theoretical studies, it is proposed that this PIA signature arises from hot hole transfer from the AuNP to the adjacent TMD, producing a charge-separated state. This suggests charge separation at the metal-semiconductor interface may be used to extend the lifetime of interband excitation generated hot holes. We conclude this development could represent an important advance in harnessing plasmonic dissipation pathways to generate long-lived carriers suited for solar-driven light harvesting and catalysis.},
doi = {10.1021/acsphotonics.9b01393},
journal = {ACS Photonics},
number = 1,
volume = 7,
place = {United States},
year = {Tue Dec 17 00:00:00 EST 2019},
month = {Tue Dec 17 00:00:00 EST 2019}
}

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Cited by: 15 works
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