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 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.
- Authors:
-
[1];
- Univ. of Chicago, IL (United States)
- Univ. of California, Davis, CA (United States)
- 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)
- 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. https://doi.org/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. https://doi.org/10.1038/s41563-018-0192-4. https://www.osti.gov/servlets/purl/1490163.
@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}
}
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