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Title: The interplay of shape and crystalline anisotropies in plasmonic semiconductor nanocrystals

Doped semiconductor nanocrystals are an emerging class of materials hosting localized surface plasmon resonance (LSPR) over a wide optical range. Studies so far have focused on tuning LSPR frequency by controlling the dopant and carrier concentrations in diverse semiconductor materials. However, the influence of anisotropic nanocrystal shape and of intrinsic crystal structure on LSPR remain poorly explored. Here, we illustrate how these two factors collaborate to determine LSPR characteristics in hexagonal cesium-doped tungsten oxide nanocrystals. The effect of shape anisotropy is systematically analyzed via synthetic control of nanocrystal aspect ratio (AR), from disks to nanorods. We demonstrate the dominant influence of crystalline anisotropy, which uniquely causes strong LSPR band-splitting into two distinct peaks with comparable intensities. Modeling typically used to rationalize particle shape effects is refined by taking into account the anisotropic dielectric function due to crystalline anisotropy, thus fully accounting for the AR-dependent evolution of multiband LSPR spectra. Furthermore, this new insight into LSPR of semiconductor nanocrystals provides a novel strategy for an exquisite tuning of LSPR line shape.
Authors:
 [1] ;  [1] ;  [2] ;  [3] ;  [1]
  1. Univ. of Texas at Austin, Austin, TX (United States)
  2. Univ. of Texas at Austin, Austin, TX (United States); ETH Zurich, Zurich (Switzerland); Empa-Swiss Federal Lab. for Materials Science and Technology, Dubendorf (Switzerland)
  3. Univ. of Texas at Austin, Austin, TX (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Grant/Contract Number:
AR0000489
Type:
Published Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 16; Journal Issue: 6; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Univ. of Texas at Austin, Austin, TX (United States)
Sponsoring Org:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Contributing Orgs:
SIBR
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; doped semiconductor; tungsten bronze; nanorod; platelet; metal oxide
OSTI Identifier:
1253218
Alternate Identifier(s):
OSTI ID: 1258027