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Title: Direct observation of narrow mid-infrared plasmon linewidths of single metal oxide nanocrystals

Infrared-responsive doped metal oxide nanocrystals are an emerging class of plasmonic materials whose localized surface plasmon resonances (LSPR) can be resonant with molecular vibrations. This presents a distinctive opportunity to manipulate light-matter interactions to redirect chemical or spectroscopic outcomes through the strong local electric fields they generate. Here we report a technique for measuring single nanocrystal absorption spectra of doped metal oxide nanocrystals, revealing significant spectral inhomogeneity in their mid-infrared LSPRs. Our analysis suggests dopant incorporation is heterogeneous beyond expectation based on a statistical distribution of dopants. The broad ensemble linewidths typically observed in these materials result primarily from sam ple heterogeneity and not from strong electronic damping associated with lossy plasmonic materials. In fact, single nanocrystal spectra reveal linewidths as narrow as 600 cm -1 in aluminium-doped zinc oxide, a value less than half the ensemble linewidth and markedly less than homogeneous linewidths of gold nanospheres.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [4]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  3. Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  4. Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
  5. Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering; Univ. of California, Berkeley, CA (United States). Graduate Program in Applied Science and Technology
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; nanoscale materials; optical physics
OSTI Identifier:
1379340

Johns, Robert W., Bechtel, Hans A., Runnerstrom, Evan L., Agrawal, Ankit, Lounis, Sebastien D., and Milliron, Delia J.. Direct observation of narrow mid-infrared plasmon linewidths of single metal oxide nanocrystals. United States: N. p., Web. doi:10.1038/ncomms11583.
Johns, Robert W., Bechtel, Hans A., Runnerstrom, Evan L., Agrawal, Ankit, Lounis, Sebastien D., & Milliron, Delia J.. Direct observation of narrow mid-infrared plasmon linewidths of single metal oxide nanocrystals. United States. doi:10.1038/ncomms11583.
Johns, Robert W., Bechtel, Hans A., Runnerstrom, Evan L., Agrawal, Ankit, Lounis, Sebastien D., and Milliron, Delia J.. 2016. "Direct observation of narrow mid-infrared plasmon linewidths of single metal oxide nanocrystals". United States. doi:10.1038/ncomms11583. https://www.osti.gov/servlets/purl/1379340.
@article{osti_1379340,
title = {Direct observation of narrow mid-infrared plasmon linewidths of single metal oxide nanocrystals},
author = {Johns, Robert W. and Bechtel, Hans A. and Runnerstrom, Evan L. and Agrawal, Ankit and Lounis, Sebastien D. and Milliron, Delia J.},
abstractNote = {Infrared-responsive doped metal oxide nanocrystals are an emerging class of plasmonic materials whose localized surface plasmon resonances (LSPR) can be resonant with molecular vibrations. This presents a distinctive opportunity to manipulate light-matter interactions to redirect chemical or spectroscopic outcomes through the strong local electric fields they generate. Here we report a technique for measuring single nanocrystal absorption spectra of doped metal oxide nanocrystals, revealing significant spectral inhomogeneity in their mid-infrared LSPRs. Our analysis suggests dopant incorporation is heterogeneous beyond expectation based on a statistical distribution of dopants. The broad ensemble linewidths typically observed in these materials result primarily from sam ple heterogeneity and not from strong electronic damping associated with lossy plasmonic materials. In fact, single nanocrystal spectra reveal linewidths as narrow as 600 cm -1 in aluminium-doped zinc oxide, a value less than half the ensemble linewidth and markedly less than homogeneous linewidths of gold nanospheres.},
doi = {10.1038/ncomms11583},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {5}
}

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