Journal
ACS PHOTONICS
Volume 7, Issue 1, Pages 197-202Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.9b01393
Keywords
hot carriers; molybdenum diselenide; transient absorption; ultrafast spectroscopy; carrier dynamics; interband transitions; intraband
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Funding
- U.S. Department of Energy (DOE) [DE-AC36-08GO28308]
- DOE Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, Solar Photochemistry Program
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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. 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.
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