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Title: The fast and the furious: Ultrafast hot electrons in plasmonic metastructures. Size and structure matter

Abstract

This review focuses on the generation of energetic (hot) electrons in plasmonic metastructures and nanomaterials, and their characterization through time-resolved spectroscopy. Excitation of hot electrons under illumination occurs in any metal or conductor, but their number will vary for each type of nanostructure. While plasmonic resonances are well described classically, the excitation of hot electrons (HEs) is a quantum process and its description requires further elaboration. Some potential applications for HEs lie in the fields of photo-catalysis and optoelectronics, and their study constitutes a very active interdisciplinary research direction that involves chemistry, physics and device engineering. Here we focus on some particular developments enabling the use of hot carriers for these applications. Particularly, we discuss the approaches and structures required to create hot carriers, the temporal dynamics of hot carrier formation and relaxation, and relevant theoretical methods used to compute the HE dynamics. The observations presented here support the conclusion that the shape of the nanostructure matters. Although metastructures with infrared gap plasmons can exhibit spatially extended hot spots and anomalously large numbers of non-thermalized HEs, most excited carriers in a plasmonic nanostructure typically have small excitation energies. Here in this paper, we discuss ways to strongly increase the numbermore » of high-energy electrons, highlighting the role of hot spots, system size, geometry and resonant frequencies. To generate HEs efficiently, we can take advantage of special geometries with hot spots, such as metamaterial absorbers with ultra-narrow gaps or nanostars. Furthermore, we discuss the applications in ultrafast electronics based on plasmon-enhanced photoemission and tunneling in the nonlinear regime. Considering the longer timescale phenomena, we also present studies on the coherent dynamics in a nanostructure after electron thermalization, showing acoustic breathing modes. In this paper, we review some key developments in the field of ultra-fast plasmonic dynamics and provide a perspective for its possible next steps.« less

Authors:
 [1];  [2];  [2];  [3];  [4];  [5];  [6]
+ Show Author Affiliations
  1. University of Electronic Science and Technology of China, Chengdu (China); Institute National de la Recherche Scientifique, Varennes (Canada)
  2. University of Electronic Science and Technology of China, Chengdu (China)
  3. Technical University of Munich, Garching (Germany)
  4. University of Notre Dame, IN (United States)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States)
  6. University of Electronic Science and Technology of China, Chengdu (China); Ohio University, Athens, OH (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NSFC); German Research Foundation (DFG); National Science Foundation (NSF); USDOE Office of Science (SC); University of Electronic Science and Technology of China (UESTC); National Basic Research Program of China
OSTI Identifier:
1557589
Alternate Identifier(s):
OSTI ID: 1779576
Grant/Contract Number:  
AC02-06CH11357; CHE-1502848; 2017M622992; EXC 2089/1 – 390776260
Resource Type:
Accepted Manuscript
Journal Name:
Nano Today
Additional Journal Information:
Journal Volume: 27; Journal ID: ISSN 1748-0132
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; plasmonic; hot electrons; photocatalysis; theory; quantum two-temperature model; time-resolved spectroscopy; photoemission; nanoparticles; metamaterials; metamaterial absorber; breathing modes; vibrational modes; acoustic modes

Citation Formats

Besteiro, Lucas V., Yu, Peng, Wang, Zhiming, Holleitner, Alexander W., Hartland, Gregory V., Wiederrecht, Gary P., and Govorov, Alexander O. The fast and the furious: Ultrafast hot electrons in plasmonic metastructures. Size and structure matter. United States: N. p., 2019. Web. doi:10.1016/j.nantod.2019.05.006.
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Besteiro, Lucas V., Yu, Peng, Wang, Zhiming, Holleitner, Alexander W., Hartland, Gregory V., Wiederrecht, Gary P., & Govorov, Alexander O. The fast and the furious: Ultrafast hot electrons in plasmonic metastructures. Size and structure matter. United States. https://doi.org/10.1016/j.nantod.2019.05.006
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Besteiro, Lucas V., Yu, Peng, Wang, Zhiming, Holleitner, Alexander W., Hartland, Gregory V., Wiederrecht, Gary P., and Govorov, Alexander O. Thu . "The fast and the furious: Ultrafast hot electrons in plasmonic metastructures. Size and structure matter". United States. https://doi.org/10.1016/j.nantod.2019.05.006. https://www.osti.gov/servlets/purl/1557589.
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@article{osti_1557589,
title = {The fast and the furious: Ultrafast hot electrons in plasmonic metastructures. Size and structure matter},
author = {Besteiro, Lucas V. and Yu, Peng and Wang, Zhiming and Holleitner, Alexander W. and Hartland, Gregory V. and Wiederrecht, Gary P. and Govorov, Alexander O.},
abstractNote = {This review focuses on the generation of energetic (hot) electrons in plasmonic metastructures and nanomaterials, and their characterization through time-resolved spectroscopy. Excitation of hot electrons under illumination occurs in any metal or conductor, but their number will vary for each type of nanostructure. While plasmonic resonances are well described classically, the excitation of hot electrons (HEs) is a quantum process and its description requires further elaboration. Some potential applications for HEs lie in the fields of photo-catalysis and optoelectronics, and their study constitutes a very active interdisciplinary research direction that involves chemistry, physics and device engineering. Here we focus on some particular developments enabling the use of hot carriers for these applications. Particularly, we discuss the approaches and structures required to create hot carriers, the temporal dynamics of hot carrier formation and relaxation, and relevant theoretical methods used to compute the HE dynamics. The observations presented here support the conclusion that the shape of the nanostructure matters. Although metastructures with infrared gap plasmons can exhibit spatially extended hot spots and anomalously large numbers of non-thermalized HEs, most excited carriers in a plasmonic nanostructure typically have small excitation energies. Here in this paper, we discuss ways to strongly increase the number of high-energy electrons, highlighting the role of hot spots, system size, geometry and resonant frequencies. To generate HEs efficiently, we can take advantage of special geometries with hot spots, such as metamaterial absorbers with ultra-narrow gaps or nanostars. Furthermore, we discuss the applications in ultrafast electronics based on plasmon-enhanced photoemission and tunneling in the nonlinear regime. Considering the longer timescale phenomena, we also present studies on the coherent dynamics in a nanostructure after electron thermalization, showing acoustic breathing modes. In this paper, we review some key developments in the field of ultra-fast plasmonic dynamics and provide a perspective for its possible next steps.},
doi = {10.1016/j.nantod.2019.05.006},
journal = {Nano Today},
number = ,
volume = 27,
place = {United States},
year = {Thu Jul 18 00:00:00 EDT 2019},
month = {Thu Jul 18 00:00:00 EDT 2019}
}
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