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Title: Design of Semiconducting Tetrahedral Mn 1-xZn xO Alloys and Their Application to Solar Water Splitting

Abstract

Transition metal oxides play important roles as contact and electrode materials, but their use as active layers in solar energy conversion requires achieving semiconducting properties akin to those of conventional semiconductors like Si or GaAs. In particular, efficient bipolar carrier transport is a challenge in these materials. Based on the prediction that a tetrahedral polymorph of MnO should have such desirable semiconducting properties, and the possibility to overcome thermodynamic solubility limits by nonequilibrium thin-film growth, we exploit both structure-property and composition-structure relationships to design and realize novel wurtzite-structure Mn 1₋xZn xO alloys. At Zn compositions above x≈0.3, thin films of these alloys assume the tetrahedral wurtzite structure instead of the octahedral rocksalt structure of MnO, thereby enabling semiconductor properties that are unique among transition metal oxides, i.e., a band gap within the visible spectrum, a band-transport mechanism for both electron and hole carriers, electron doping, and a band lineup suitable for solar hydrogen generation. In conclusion, a proof of principle is provided by initial photo-electrocatalytic device measurements, corroborating, in particular, the predicted favorable hole-transport properties of these alloys.

Authors:
 [1];  [1];  [1];  [1];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1182803
Alternate Identifier(s):
OSTI ID: 1220582
Report Number(s):
NREL/JA-5K00-60832
Journal ID: ISSN 2160-3308
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Published Article
Journal Name:
Physical Review. X
Additional Journal Information:
Journal Volume: 5; Journal Issue: 2; Journal ID: ISSN 2160-3308
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; materials design; semiconductor oxides; ab initio computation; non-equilibrium materials

Citation Formats

Peng, Haowei, Ndione, Paul F., Ginley, David S., Zakutayev, Andriy, and Lany, Stephan. Design of Semiconducting Tetrahedral Mn1-xZnxO Alloys and Their Application to Solar Water Splitting. United States: N. p., 2015. Web. doi:10.1103/PhysRevX.5.021016.
Peng, Haowei, Ndione, Paul F., Ginley, David S., Zakutayev, Andriy, & Lany, Stephan. Design of Semiconducting Tetrahedral Mn1-xZnxO Alloys and Their Application to Solar Water Splitting. United States. doi:10.1103/PhysRevX.5.021016.
Peng, Haowei, Ndione, Paul F., Ginley, David S., Zakutayev, Andriy, and Lany, Stephan. Wed . "Design of Semiconducting Tetrahedral Mn1-xZnxO Alloys and Their Application to Solar Water Splitting". United States. doi:10.1103/PhysRevX.5.021016.
@article{osti_1182803,
title = {Design of Semiconducting Tetrahedral Mn1-xZnxO Alloys and Their Application to Solar Water Splitting},
author = {Peng, Haowei and Ndione, Paul F. and Ginley, David S. and Zakutayev, Andriy and Lany, Stephan},
abstractNote = {Transition metal oxides play important roles as contact and electrode materials, but their use as active layers in solar energy conversion requires achieving semiconducting properties akin to those of conventional semiconductors like Si or GaAs. In particular, efficient bipolar carrier transport is a challenge in these materials. Based on the prediction that a tetrahedral polymorph of MnO should have such desirable semiconducting properties, and the possibility to overcome thermodynamic solubility limits by nonequilibrium thin-film growth, we exploit both structure-property and composition-structure relationships to design and realize novel wurtzite-structure Mn1₋xZnxO alloys. At Zn compositions above x≈0.3, thin films of these alloys assume the tetrahedral wurtzite structure instead of the octahedral rocksalt structure of MnO, thereby enabling semiconductor properties that are unique among transition metal oxides, i.e., a band gap within the visible spectrum, a band-transport mechanism for both electron and hole carriers, electron doping, and a band lineup suitable for solar hydrogen generation. In conclusion, a proof of principle is provided by initial photo-electrocatalytic device measurements, corroborating, in particular, the predicted favorable hole-transport properties of these alloys.},
doi = {10.1103/PhysRevX.5.021016},
journal = {Physical Review. X},
number = 2,
volume = 5,
place = {United States},
year = {2015},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1103/PhysRevX.5.021016

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Cited by: 24 works
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