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Title: Mapping Photoemission and Hot-Electron Emission from Plasmonic Nanoantennas

Abstract

Understanding plasmon-mediated electron emission and energy transfer on the nanometer length scale is critical to controlling light–matter interactions at nanoscale dimensions. In a high-resolution lithographic material, electron emission and energy transfer lead to chemical transformations. Here, we employ such chemical transformations in two different high-resolution electron-beam lithography resists, poly(methyl methacrylate) (PMMA) and hydrogen silsesquioxane (HSQ), to map local electron emission and energy transfer with nanometer resolution from plasmonic nanoantennas excited by femtosecond laser pulses. We observe exposure of the electron-beam resists (both PMMA and HSQ) in regions on the surface of nanoantennas where the local field is significantly enhanced. Exposure in these regions is consistent with previously reported optical-field-controlled electron emission from plasmonic hotspots as well as earlier work on low-electron-energy scanning probe lithography. For HSQ, in addition to exposure in hotspots, we observe resist exposure at the centers of rod-shaped nanoantennas in addition to exposure in plasmonic hotspots. Optical field enhancement is minimized at the center of nanorods suggesting that exposure in these regions involves a different mechanism to that in plasmonic hotspots. Our simulations suggest that exposure at the center of nanorods results from the emission of hot electrons produced via plasmon decay in the nanorods. Our resultsmore » provide a means to map both optical-field-controlled electron emission and hot-electron transfer from nanoparticles via chemical transformations produced locally in lithographic materials.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [4]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics; Trinity College, Dublin (Ireland). Centre for Research on Adapative Nanostructures and Nanodevices (CRANN), Advanced Materials Bio-Engineering Resarch Center (AMBER)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics; Univ. of Hamburg (Germany). Dept. of Physics, Center for Ultrafast Imaging; Northrop Grumman, Redondo Beach, CA (United States)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics; Univ. of Hamburg (Germany). Dept. of Physics, Center for Ultrafast Imaging; Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1395006
Grant/Contract Number:  
SC0001088
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; charge transfer; hot electrons; Nanoantennas; photoemission; plasmon decay; plasmonics

Citation Formats

Hobbs, Richard G., Putnam, William P., Fallahi, Arya, Yang, Yujia, Kärtner, Franz X., and Berggren, Karl K. Mapping Photoemission and Hot-Electron Emission from Plasmonic Nanoantennas. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b02495.
Hobbs, Richard G., Putnam, William P., Fallahi, Arya, Yang, Yujia, Kärtner, Franz X., & Berggren, Karl K. Mapping Photoemission and Hot-Electron Emission from Plasmonic Nanoantennas. United States. https://doi.org/10.1021/acs.nanolett.7b02495
Hobbs, Richard G., Putnam, William P., Fallahi, Arya, Yang, Yujia, Kärtner, Franz X., and Berggren, Karl K. 2017. "Mapping Photoemission and Hot-Electron Emission from Plasmonic Nanoantennas". United States. https://doi.org/10.1021/acs.nanolett.7b02495. https://www.osti.gov/servlets/purl/1395006.
@article{osti_1395006,
title = {Mapping Photoemission and Hot-Electron Emission from Plasmonic Nanoantennas},
author = {Hobbs, Richard G. and Putnam, William P. and Fallahi, Arya and Yang, Yujia and Kärtner, Franz X. and Berggren, Karl K.},
abstractNote = {Understanding plasmon-mediated electron emission and energy transfer on the nanometer length scale is critical to controlling light–matter interactions at nanoscale dimensions. In a high-resolution lithographic material, electron emission and energy transfer lead to chemical transformations. Here, we employ such chemical transformations in two different high-resolution electron-beam lithography resists, poly(methyl methacrylate) (PMMA) and hydrogen silsesquioxane (HSQ), to map local electron emission and energy transfer with nanometer resolution from plasmonic nanoantennas excited by femtosecond laser pulses. We observe exposure of the electron-beam resists (both PMMA and HSQ) in regions on the surface of nanoantennas where the local field is significantly enhanced. Exposure in these regions is consistent with previously reported optical-field-controlled electron emission from plasmonic hotspots as well as earlier work on low-electron-energy scanning probe lithography. For HSQ, in addition to exposure in hotspots, we observe resist exposure at the centers of rod-shaped nanoantennas in addition to exposure in plasmonic hotspots. Optical field enhancement is minimized at the center of nanorods suggesting that exposure in these regions involves a different mechanism to that in plasmonic hotspots. Our simulations suggest that exposure at the center of nanorods results from the emission of hot electrons produced via plasmon decay in the nanorods. Our results provide a means to map both optical-field-controlled electron emission and hot-electron transfer from nanoparticles via chemical transformations produced locally in lithographic materials.},
doi = {10.1021/acs.nanolett.7b02495},
url = {https://www.osti.gov/biblio/1395006}, journal = {Nano Letters},
issn = {1530-6984},
number = ,
volume = 17,
place = {United States},
year = {Tue Sep 19 00:00:00 EDT 2017},
month = {Tue Sep 19 00:00:00 EDT 2017}
}

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Cited by: 47 works
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Figures / Tables:

Figure 1 Figure 1: Nanoantennas and experimental approach. (a, b) Top-down SEM micrographs of an array of Au nanorod (a) and nanotriangle (b) antennas fabricated by electron-beam lithography. (c) Schematic representation of experimental setup. The 10 fs pulses of linearly polarized light with a central wavelength of 1.2 $$μ$$m and a bandwidthmore » of 400 nm were focused to a 1/e2 diameter of 5.2 $$μ$$m on the nanoantenna arrays, which were fabricated on an ITO-coated (blue regions) sapphire substrate (gray regions). A 5 $$μ$$m gap was etched in the ITO layer as shown to allow a bias to be applied between the nanoantenna emitter array (the emitter electrode: blue region on the right; $$V$$E = 0) and the collector electrode (blue region on the left; $$V$$C = $$V$$BIAS). (d) Schematic showing a nanoantenna coated with a 20-nm-thick layer of PMMA or HSQ (semitransparent green region), which acted as an imaging layer for emitted electrons.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.