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Title: Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities

Abstract

Localized surface plasmon resonances (LSPR) of nanostructures can be tuned by controlling their morphology, local dielectric environment, and free carrier concentration. We report the colloidal synthesis of an ~3 tungsten–oxygen (W-O) layer thick (~1 nm), two-dimensional (2D) WO3-x nanoplatelets (NPLs) (x ≈ 0.55–1.03), which display tunable near-infrared LSPR properties and additionally high free electron density (Ne) that arises predominantly from the large shape factor of 2D NPLs. Importantly, the W to O composition ratios inferred from their LSPR measurements show much higher percentage of oxygen vacancies than those determined by X-ray diffraction analysis, suggesting that the aspect ratio of ultrathin WO3-x NPLs is the key to producing an unprecedentedly large Ne, although synthesis temperature is also an independent factor. We find that NPL formation is kinetically controlled, whereas thermodynamic parameter manipulation leads to Ne values as high as 4.13 × 1022 cm–3, which is close to that of plasmonic noble metals, and thus our oxide-based nanostructures can be considered as quasi-metallic. The unique structural properties of 2D nanomaterials along with the high Ne of WO3-x NPLs provide an attractive alternative to plasmonic noble metal nanostructures for various plasmon-driven energy conversions and design of photochromic nanodevices.

Authors:
 [1];  [1];  [2];  [1]; ORCiD logo [3]
+ Show Author Affiliations
  1. Purdue Univ., West Lafayette, IN (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Purdue Univ., West Lafayette, IN (United States); Indiana Univ., Bloomington, IN (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)
OSTI Identifier:
1774248
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 142; Journal Issue: 13; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Nanostructures; Oxides; Metals; Plasmonics; Surface plasmon resonance

Citation Formats

Prusty, Gyanaranjan, Lee, Jacob T., Seifert, Soenke, Muhoberac, Barry B., and Sardar, Rajesh. Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities. United States: N. p., 2020. Web. doi:10.1021/jacs.9b13909.
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Prusty, Gyanaranjan, Lee, Jacob T., Seifert, Soenke, Muhoberac, Barry B., & Sardar, Rajesh. Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities. United States. https://doi.org/10.1021/jacs.9b13909
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Prusty, Gyanaranjan, Lee, Jacob T., Seifert, Soenke, Muhoberac, Barry B., and Sardar, Rajesh. Mon . "Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities". United States. https://doi.org/10.1021/jacs.9b13909. https://www.osti.gov/servlets/purl/1774248.
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@article{osti_1774248,
title = {Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities},
author = {Prusty, Gyanaranjan and Lee, Jacob T. and Seifert, Soenke and Muhoberac, Barry B. and Sardar, Rajesh},
abstractNote = {Localized surface plasmon resonances (LSPR) of nanostructures can be tuned by controlling their morphology, local dielectric environment, and free carrier concentration. We report the colloidal synthesis of an ~3 tungsten–oxygen (W-O) layer thick (~1 nm), two-dimensional (2D) WO3-x nanoplatelets (NPLs) (x ≈ 0.55–1.03), which display tunable near-infrared LSPR properties and additionally high free electron density (Ne) that arises predominantly from the large shape factor of 2D NPLs. Importantly, the W to O composition ratios inferred from their LSPR measurements show much higher percentage of oxygen vacancies than those determined by X-ray diffraction analysis, suggesting that the aspect ratio of ultrathin WO3-x NPLs is the key to producing an unprecedentedly large Ne, although synthesis temperature is also an independent factor. We find that NPL formation is kinetically controlled, whereas thermodynamic parameter manipulation leads to Ne values as high as 4.13 × 1022 cm–3, which is close to that of plasmonic noble metals, and thus our oxide-based nanostructures can be considered as quasi-metallic. The unique structural properties of 2D nanomaterials along with the high Ne of WO3-x NPLs provide an attractive alternative to plasmonic noble metal nanostructures for various plasmon-driven energy conversions and design of photochromic nanodevices.},
doi = {10.1021/jacs.9b13909},
journal = {Journal of the American Chemical Society},
number = 13,
volume = 142,
place = {United States},
year = {Mon Mar 16 00:00:00 EDT 2020},
month = {Mon Mar 16 00:00:00 EDT 2020}
}
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https://doi.org/10.1021/jacs.9b13909
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