气候变化领域集成服务门户(CCPortal): Hot carrier multiplication in plasmonic photocatalysis

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DOI	10.1073/pnas.2022109118
	Hot carrier multiplication in plasmonic photocatalysis
	Zhou L.; Lou M.; Bao J.L.; Zhang C.; Liu J.G.; Martirez J.M.P.; Tian S.; Yuan L.; Swearer D.F.; Robatjazi H.; Carter E.A.; Nordlander P.; Halas N.J.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:20
英文摘要	Light-induced hot carriers derived from the surface plasmons of metal nanostructures have been shown to be highly promising agents for photocatalysis. While both nonthermal and thermalized hot carriers can potentially contribute to this process, their specific role in any given chemical reaction has generally not been identified. Here, we report the observation that the H2–D2 exchange reaction photocatalyzed by Cu nanoparticles is driven primarily by thermalized hot carriers. The external quantum yield shows an intriguing S-shaped intensity dependence and exceeds 100% for high light intensities, suggesting that hot carrier multiplication plays a role. A simplified model for the quantum yield of thermalized hot carriers reproduces the observed kinetic features of the reaction, validating our hypothesis of a thermalized hot carrier mechanism. A quantum mechanical study reveals that vibrational excitations of the surface Cu–H bond is the likely activation mechanism, further supporting the effectiveness of low-energy thermalized hot carriers in photocatalyzing this reaction. © 2021 National Academy of Sciences. All rights reserved.
语种	英语
scopus关键词	copper; copper nanoparticle; hydrogen; Article; carrier multiplication; chemical bond; chemical reaction kinetics; controlled study; deuterium hydrogen exchange; electron; excitation; hot electron; light intensity; photocatalysis; photochemistry; physics; plasmon; quantum mechanics; quantum yield; surface property; vibration
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238567
作者单位	Department of Chemistry, Rice University, Houston, TX 77005, United States; Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005, United States; Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ 08544, United States; Department of Chemistry, Boston College, Chestnut Hill, MA 02467, United States; Department of Physics and Astronomy, Rice University, Houston, TX 77005, United States; Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA 90095, United States; Office of the Chancellor, University of California, Los Angeles, CA 90095, United States
推荐引用方式 GB/T 7714	Zhou L.,Lou M.,Bao J.L.,et al. Hot carrier multiplication in plasmonic photocatalysis[J],2021,118(20).
APA	Zhou L..,Lou M..,Bao J.L..,Zhang C..,Liu J.G..,...&Halas N.J..(2021).Hot carrier multiplication in plasmonic photocatalysis.Proceedings of the National Academy of Sciences of the United States of America,118(20).
MLA	Zhou L.,et al."Hot carrier multiplication in plasmonic photocatalysis".Proceedings of the National Academy of Sciences of the United States of America 118.20(2021).