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

doi:10.1038/s41563-018-0192-4

This content will become publicly available on October 29, 2019

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:

^[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)

Publication Date:: 2018-10-29

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.

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                    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.

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                    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.

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@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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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
DOI: 10.1103/PhysRevLett.77.3865

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
DOI: 10.1088/0953-8984/21/39/395502

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Similar Records

This content will become publicly available on October 29, 2019

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

Abstract

Citation Formats

Generalized Gradient Approximation Made Simple journal, October 1996

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

Generalized Gradient Approximation Made Simple
journal, October 1996

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009