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Title: The role of defects and excess surface charges at finite temperature for optimizing oxide photoabsorbers

Abstract

Computational screening of materials for solar to fuel conversion technologies has mostly focused on bulk properties, thus neglecting the structure and chemistry of surfaces and interfaces with water. We report a finite temperature study of WO 3, a promising anode for photoelectrochemical cells, carried out using first-principles molecular dynamics simulations coupled with many-body perturbation theory. We identified three major factors determining the chemical reactivity of the material interfaced with water: the presence of surface defects, the dynamics of excess charge at the surface, and finite temperature fluctuations of the surface electronic orbitals. These general descriptors are essential for the understanding and prediction of optimal oxide photoabsorbers for water oxidation.

Authors:
ORCiD logo [1];  [2];  [3];  [3]
  1. Univ. of Chicago, IL (United States)
  2. Univ. of California, Davis, CA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF) - Centers for Chemical Innovation (CCI); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1490163
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 17; Journal Issue: 12; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Gerosa, Matteo, Gygi, Francois, Govoni, Marco, and Galli, Giulia. The role of defects and excess surface charges at finite temperature for optimizing oxide photoabsorbers. United States: N. p., 2018. Web. doi:10.1038/s41563-018-0192-4.
Gerosa, Matteo, Gygi, Francois, Govoni, Marco, & Galli, Giulia. The role of defects and excess surface charges at finite temperature for optimizing oxide photoabsorbers. United States. doi:10.1038/s41563-018-0192-4.
Gerosa, Matteo, Gygi, Francois, Govoni, Marco, and Galli, Giulia. Mon . "The role of defects and excess surface charges at finite temperature for optimizing oxide photoabsorbers". United States. doi:10.1038/s41563-018-0192-4.
@article{osti_1490163,
title = {The role of defects and excess surface charges at finite temperature for optimizing oxide photoabsorbers},
author = {Gerosa, Matteo and Gygi, Francois and Govoni, Marco and Galli, Giulia},
abstractNote = {Computational screening of materials for solar to fuel conversion technologies has mostly focused on bulk properties, thus neglecting the structure and chemistry of surfaces and interfaces with water. We report a finite temperature study of WO3, a promising anode for photoelectrochemical cells, carried out using first-principles molecular dynamics simulations coupled with many-body perturbation theory. We identified three major factors determining the chemical reactivity of the material interfaced with water: the presence of surface defects, the dynamics of excess charge at the surface, and finite temperature fluctuations of the surface electronic orbitals. These general descriptors are essential for the understanding and prediction of optimal oxide photoabsorbers for water oxidation.},
doi = {10.1038/s41563-018-0192-4},
journal = {Nature Materials},
number = 12,
volume = 17,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
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Works referenced in this record:

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