Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities

Prusty, Gyanaranjan; Lee, Jacob T.; Seifert, Soenke; Muhoberac, Barry B.; Sardar, Rajesh

doi:10.1021/jacs.9b13909

Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities

Journal Article · Mon Mar 16 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b13909· OSTI ID:1774248

Prusty, Gyanaranjan ^[1]; Lee, Jacob T. ^[1]; Seifert, Soenke ^[2]; Muhoberac, Barry B. ^[1]; ^[3]

Purdue Univ., West Lafayette, IN (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Purdue Univ., West Lafayette, IN (United States); Indiana Univ., Bloomington, IN (United States)

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) WO_3-x nanoplatelets (NPLs) (x ≈ 0.55–1.03), which display tunable near-infrared LSPR properties and additionally high free electron density (N_e) 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 WO_3-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 N_e 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 N_e of WO_3-x NPLs provide an attractive alternative to plasmonic noble metal nanostructures for various plasmon-driven energy conversions and design of photochromic nanodevices.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1774248

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 13 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Ultrathin Plasmonic Tungsten Oxide Quantum Wells with Controllable Free Carrier Densities

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