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

University of Electronic Science and Technology of China; University of Electronic Science and Technology of China; University of Electronic Science and Technology of China; Ohio University; Argonne National Laboratory; University of Electronic Science and Technology of China; Ohio University
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Publisher: ACS
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Abstract AITranslate

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 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.

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DOI:https://doi.org/10.1021/acsenergylett.9b01617

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Citation Information:

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 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.

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GB/T 7714-2015 [1] Le Chang, Lucas V. Besteiro, Jiachen Sun, et al. ACS Energy Letters, 2019(4). DOI:10.1021/acsenergylett.9b01617.
MLA [1] Le Chang, et al., ACS Energy Letters, no. 4, 2019, https://doi.org/10.1021/acsenergylett.9b01617.
APA [1] Le Chang, Lucas V. Besteiro, Jiachen Sun, Eva Yazmin Santiago, Stephen K. Gray, Zhiming Wang, & Alexander O. Govorov. (2019). ACS Energy Letters(4). https://doi.org/10.1021/acsenergylett.9b01617
IEEE [1] Le Chang, Lucas V. Besteiro, Jiachen Sun, Eva Yazmin Santiago, Stephen K. Gray, Zhiming Wang, and Alexander O. Govorov, ACS Energy Letters, no. 4, 2019, doi: 10.1021/acsenergylett.9b01617.