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Title: Combinatorial Discovery of Lanthanum–Tantalum Oxynitride Solar Light Absorbers with Dilute Nitrogen for Solar Fuel Applications

Abstract

Oxynitrides with the photoelectrochemical stability of oxides and desirable band energetics of nitrides comprise a promising class of materials for solar photochemistry. Challenges in synthesizing a wide variety of oxynitride materials has limited exploration of this class of functional materials, which we address using a reactive cosputtering combined with rapid thermal processing method to synthesize multi-cation–multi-anion libraries. We demonstrate the synthesis of a LaxTa1–xOyNz thin film composition spread library and its characterization by both traditional thin film materials characterization and custom combinatorial optical spectroscopy and X-ray absorption near edge spectroscopy (XANES) techniques, ultimately establishing structure-chemistry-property relationships. We observe that over a substantial La–Ta composition range the thin films crystallize in the same perovskite LaTaON2 structure with significant variation of anion chemistry. The relative invariance in optical band gap demonstrates a remarkable decoupling of composition and band energetics so that the composition can be optimized while retaining the desirable 2 eV band gap energy. We also demonstrate the intercalation of diatomic nitrogen into the La3TaO7 structure, which gives rise to a direct-allowed optical transition at 2.2 eV, less than half the value of the oxide’s band gap. These findings motivate further exploration of the visible light response of this material thatmore » is predicted to be stable over a wide range of electrochemical potential.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [3]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); Toyota Research Inst., Mountain View, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
  3. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis (JCAP) and Molecular Biophysics and Integrated Bioimaging Division
Publication Date:
Research Org.:
California Institute of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1468652
Alternate Identifier(s):
OSTI ID: 1468651
Grant/Contract Number:  
SC0004993; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Combinatorial Science
Additional Journal Information:
Journal Volume: 20; Journal Issue: 1; Journal ID: ISSN 2156-8952
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
10 SYNTHETIC FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; combinatorial materials science; light absorber; oxynitride; solar fuel; x-ray absorption spectroscopy

Citation Formats

Suram, Santosh K., Fackler, Sean W., Zhou, Lan, N’Diaye, Alpha T., Drisdell, Walter S., Yano, Junko, and Gregoire, John M. Combinatorial Discovery of Lanthanum–Tantalum Oxynitride Solar Light Absorbers with Dilute Nitrogen for Solar Fuel Applications. United States: N. p., 2017. Web. doi:10.1021/acscombsci.7b00143.
Suram, Santosh K., Fackler, Sean W., Zhou, Lan, N’Diaye, Alpha T., Drisdell, Walter S., Yano, Junko, & Gregoire, John M. Combinatorial Discovery of Lanthanum–Tantalum Oxynitride Solar Light Absorbers with Dilute Nitrogen for Solar Fuel Applications. United States. https://doi.org/10.1021/acscombsci.7b00143
Suram, Santosh K., Fackler, Sean W., Zhou, Lan, N’Diaye, Alpha T., Drisdell, Walter S., Yano, Junko, and Gregoire, John M. Mon . "Combinatorial Discovery of Lanthanum–Tantalum Oxynitride Solar Light Absorbers with Dilute Nitrogen for Solar Fuel Applications". United States. https://doi.org/10.1021/acscombsci.7b00143. https://www.osti.gov/servlets/purl/1468652.
@article{osti_1468652,
title = {Combinatorial Discovery of Lanthanum–Tantalum Oxynitride Solar Light Absorbers with Dilute Nitrogen for Solar Fuel Applications},
author = {Suram, Santosh K. and Fackler, Sean W. and Zhou, Lan and N’Diaye, Alpha T. and Drisdell, Walter S. and Yano, Junko and Gregoire, John M.},
abstractNote = {Oxynitrides with the photoelectrochemical stability of oxides and desirable band energetics of nitrides comprise a promising class of materials for solar photochemistry. Challenges in synthesizing a wide variety of oxynitride materials has limited exploration of this class of functional materials, which we address using a reactive cosputtering combined with rapid thermal processing method to synthesize multi-cation–multi-anion libraries. We demonstrate the synthesis of a LaxTa1–xOyNz thin film composition spread library and its characterization by both traditional thin film materials characterization and custom combinatorial optical spectroscopy and X-ray absorption near edge spectroscopy (XANES) techniques, ultimately establishing structure-chemistry-property relationships. We observe that over a substantial La–Ta composition range the thin films crystallize in the same perovskite LaTaON2 structure with significant variation of anion chemistry. The relative invariance in optical band gap demonstrates a remarkable decoupling of composition and band energetics so that the composition can be optimized while retaining the desirable 2 eV band gap energy. We also demonstrate the intercalation of diatomic nitrogen into the La3TaO7 structure, which gives rise to a direct-allowed optical transition at 2.2 eV, less than half the value of the oxide’s band gap. These findings motivate further exploration of the visible light response of this material that is predicted to be stable over a wide range of electrochemical potential.},
doi = {10.1021/acscombsci.7b00143},
journal = {ACS Combinatorial Science},
number = 1,
volume = 20,
place = {United States},
year = {2017},
month = {11}
}

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