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

Gerosa, Matteo; Gygi, Francois; Govoni, Marco; Galli, Giulia

doi:10.1038/s41563-018-0192-4

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

Journal Article · 28 October 2018 · Nature Materials

DOI: https://doi.org/10.1038/s41563-018-0192-4 · OSTI ID:1490163

^[1]; Gygi, Francois ^[2]; Govoni, Marco ^[3]; Galli, Giulia ^[3]

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)

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.

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

Sponsoring Organization:: National Science Foundation (NSF) - Centers for Chemical Innovation (CCI); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1490163

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 12 Vol. 17; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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