Electronic Structure of the Plasmons in Metal Nanocrystals: Fundamental Limitations for the Energy Efficiency of Hot Electron Generation

Chang, Le; Besteiro, Lucas V.; Sun, Jiachen; Santiago, Eva Yazmin; Gray, Stephen K.; Wang, Zhiming; Govorov, Alexander O.

doi:10.1021/acsenergylett.9b01617

Electronic Structure of the Plasmons in Metal Nanocrystals: Fundamental Limitations for the Energy Efficiency of Hot Electron Generation

Journal Article · Mon Sep 16 00:00:00 EDT 2019 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.9b01617· OSTI ID:1608036

Chang, Le ^[1]; ^[2]; Sun, Jiachen ^[1]; Santiago, Eva Yazmin ^[3]; Gray, Stephen K. ^[4]; Wang, Zhiming ^[1]; ^[5]

Univ. of Electronic Science and Technology of China, Chengdu (China). Inst. of Fundamental and Frontier Sciences
Univ. of Electronic Science and Technology of China, Chengdu (China). Inst. of Fundamental and Frontier Sciences; Inst. National de la Recherche Scientifique (INRS), Québec (Canada). Centre Énergie Matériaux et Télécommunications
Ohio Univ., Athens, OH (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
Univ. of Electronic Science and Technology of China, Chengdu (China). Inst. of Fundamental and Frontier Sciences; Ohio Univ., Athens, OH (United States)

This Review discusses the electronic structure of plasmonic resonances in metal nanostructures, clarifying existing misconceptions on the topic. Here we underscore the key property of the plasmonic response in metal nanocrystals: the plasmon and its wave function are mostly composed of a large number of low-energy excitations, which involve electrons near the Fermi level. Simultaneously, some number of high-energy hot electrons are excited in a nanocrystal due to the scattering of electrons by surfaces and in hot spots. It is an established fact that plasmon excitations are well described by classical frameworks, considering the collective oscillation of low-energy carriers moving as the result of classical acceleration. This classical motion is intrinsically dissipative and leads to heating. On the other hand, the generation of hot electrons in nanocrystals is a quantum surface effect. The energy efficiency of such Metal Semiconductor hot-electron processes is always limited. However, there are interesting possibilities for the hot-electron enhancement, which we discuss here in the context of applications for plasmonic photodetectors, photocatalysis, and ultrafast spectroscopy.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: China Postdoctoral Science Foundation; National Basic Research Program of China; National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); University of Electronic Science and Technology of China (UESTC); Volkswagen Foundation

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1608036

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 10 Vol. 4; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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