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. 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. 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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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
Band gap states in nanocrystalline WO 3 thin films studied by soft x-ray spectroscopy and optical spectrophotometry
journal, September 2016
- Johansson, M. B.; Kristiansen, P. T.; Duda, L.
- Journal of Physics: Condensed Matter, Vol. 28, Issue 47
Optical properties of tungsten trioxide from first-principles calculations
journal, April 2013
- Ping, Yuan; Rocca, Dario; Galli, Giulia
- Physical Review B, Vol. 87, Issue 16
The W5+ polaron in crystalline low temperature WO3 ESR and optical absorption
journal, January 1980
- Schirmer, O. F.; Salje, E.
- Solid State Communications, Vol. 33, Issue 3
Effect of a Cobalt-Based Oxygen Evolution Catalyst on the Stability and the Selectivity of Photo-Oxidation Reactions of a WO 3 Photoanode
journal, March 2011
- Seabold, Jason A.; Choi, Kyoung-Shin
- Chemistry of Materials, Vol. 23, Issue 5
Solvation effects on the band edge positions of photocatalysts from first principles
journal, January 2015
- Ping, Yuan; Sundararaman, Ravishankar; Goddard III, William A.
- Physical Chemistry Chemical Physics, Vol. 17, Issue 45
Architecture of Qbox: A scalable first-principles molecular dynamics code
journal, January 2008
- Gygi, F.
- IBM Journal of Research and Development, Vol. 52, Issue 1.2
Electrochemical deposition and photoelectrochemistry of CuWO4, a promising photoanode for water oxidation
journal, January 2011
- Yourey, Joseph E.; Bartlett, Bart M.
- Journal of Materials Chemistry, Vol. 21, Issue 21
DFT Study of Hydrogen Adsorption On the Monoclinic WO 3 (001) Surface
journal, May 2012
- Wang, Fenggong; Di Valentin, Cristiana; Pacchioni, Gianfranco
- The Journal of Physical Chemistry C, Vol. 116, Issue 19
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
Nanostructured hematite: synthesis, characterization, charge carrier dynamics, and photoelectrochemical properties
journal, January 2012
- Wheeler, Damon A.; Wang, Gongming; Ling, Yichuan
- Energy & Environmental Science, Vol. 5, Issue 5
A mechanism for the hole-mediated water photooxidation on TiO 2 (1 0 1) surfaces
journal, January 2016
- Di Valentin, Cristiana
- Journal of Physics: Condensed Matter, Vol. 28, Issue 7
Facet-dependent trapping and dynamics of excess electrons at anatase TiO2 surfaces and aqueous interfaces
journal, June 2016
- Selcuk, Sencer; Selloni, Annabella
- Nature Materials, Vol. 15, Issue 10
Platinized WO 3 as an Environmental Photocatalyst that Generates OH Radicals under Visible Light
journal, September 2010
- Kim, Jungwon; Lee, Chul Wee; Choi, Wonyong
- Environmental Science & Technology, Vol. 44, Issue 17
Anisotropic Effects of Oxygen Vacancies on Electrochromic Properties and Conductivity of γ-Monoclinic WO 3
journal, May 2016
- Gerosa, Matteo; Di Valentin, Cristiana; Onida, Giovanni
- The Journal of Physical Chemistry C, Vol. 120, Issue 21
Dissolution kinetics of WO3 in acidic solutions
journal, February 2006
- Anik, Mustafa; Cansizoglu, Tuba
- Journal of Applied Electrochemistry, Vol. 36, Issue 5
Materials for solar fuels and chemicals
journal, December 2016
- Montoya, Joseph H.; Seitz, Linsey C.; Chakthranont, Pongkarn
- Nature Materials, Vol. 16, Issue 1
Ab initio study of oxygen point defects on tungsten trioxide surface
journal, January 2012
- Lambert-Mauriat, Caroline; Oison, Vincent; Saadi, Lama
- Surface Science, Vol. 606, Issue 1-2
Optimized norm-conserving Vanderbilt pseudopotentials
journal, August 2013
- Hamann, D. R.
- Physical Review B, Vol. 88, Issue 8
Heterojunction BiVO4/WO3 electrodes for enhanced photoactivity of water oxidation
journal, January 2011
- Hong, Suk Joon; Lee, Seungok; Jang, Jum Suk
- Energy & Environmental Science, Vol. 4, Issue 5
Interfacial Effects on the Band Edges of Functionalized Si Surfaces in Liquid Water
journal, November 2014
- Pham, Tuan Anh; Lee, Donghwa; Schwegler, Eric
- Journal of the American Chemical Society, Vol. 136, Issue 49
Improving O2 production of WO3 photoanodes with IrO2 in acidic aqueous electrolyte
journal, January 2014
- Spurgeon, Joshua M.; Velazquez, Jesus M.; McDowell, Matthew T.
- Physical Chemistry Chemical Physics, Vol. 16, Issue 8
Hydroxide Ions at the Water/Anatase TiO 2 (101) Interface: Structure and Electronic States from First Principles Molecular Dynamics
journal, July 2010
- Cheng, Hongzhi; Selloni, Annabella
- Langmuir, Vol. 26, Issue 13
Ab initio DFT computation of SnO2 and WO3 slabs and gas–surface interactions
journal, September 2007
- Levy, M.; Pagnier, T.
- Sensors and Actuators B: Chemical, Vol. 126, Issue 1
Alignment of Redox Levels at Semiconductor–Water Interfaces
journal, December 2017
- Guo, Zhendong; Ambrosio, Francesco; Chen, Wei
- Chemistry of Materials, Vol. 30, Issue 1
First-Principles Approach to Calculating Energy Level Alignment at Aqueous Semiconductor Interfaces
journal, October 2014
- Kharche, Neerav; Muckerman, James T.; Hybertsen, Mark S.
- Physical Review Letters, Vol. 113, Issue 17
Thermally Stable N 2 -Intercalated WO 3 Photoanodes for Water Oxidation
journal, October 2012
- Mi, Qixi; Ping, Yuan; Li, Yan
- Journal of the American Chemical Society, Vol. 134, Issue 44
Sputtered WO3 films for water splitting applications
journal, February 2016
- Valerini, D.; Hernández, S.; Di Benedetto, F.
- Materials Science in Semiconductor Processing, Vol. 42
Dipole correction for surface supercell calculations
journal, May 1999
- Bengtsson, Lennart
- Physical Review B, Vol. 59, Issue 19
First principles scheme to evaluate band edge positions in potential transition metal oxide photocatalysts and photoelectrodes
journal, January 2011
- Toroker, Maytal Caspary; Kanan, Dalal K.; Alidoust, Nima
- Physical Chemistry Chemical Physics, Vol. 13, Issue 37, p. 16644-16654
Quantitative characterization of hydroxyl radicals produced by various photocatalysts
journal, May 2011
- Xiang, Quanjun; Yu, Jiaguo; Wong, Po Keung
- Journal of Colloid and Interface Science, Vol. 357, Issue 1
Electronic and optical properties of nanocrystalline WO 3 thin films studied by optical spectroscopy and density functional calculations
journal, April 2013
- Johansson, Malin B.; Baldissera, Gustavo; Valyukh, Iryna
- Journal of Physics: Condensed Matter, Vol. 25, Issue 20
Water Oxidation on Pure and Doped Hematite (0001) Surfaces: Prediction of Co and Ni as Effective Dopants for Electrocatalysis
journal, August 2012
- Liao, Peilin; Keith, John A.; Carter, Emily A.
- Journal of the American Chemical Society, Vol. 134, Issue 32
X-ray photon correlation spectroscopy
journal, August 2014
- Shpyrko, Oleg G.
- Journal of Synchrotron Radiation, Vol. 21, Issue 5
Self-consistent hybrid functional for condensed systems
journal, May 2014
- Skone, Jonathan H.; Govoni, Marco; Galli, Giulia
- Physical Review B, Vol. 89, Issue 19
Canonical sampling through velocity rescaling
journal, January 2007
- Bussi, Giovanni; Donadio, Davide; Parrinello, Michele
- The Journal of Chemical Physics, Vol. 126, Issue 1
Charge generation layers comprising transition metal-oxide/organic interfaces: Electronic structure and charge generation mechanism
journal, May 2010
- Meyer, J.; Kröger, M.; Hamwi, S.
- Applied Physics Letters, Vol. 96, Issue 19
Modelling heterogeneous interfaces for solar water splitting
journal, January 2017
- Pham, Tuan Anh; Ping, Yuan; Galli, Giulia
- Nature Materials, Vol. 16, Issue 4
Role of oxygen vacancies in crystalline WO 3
journal, January 2016
- Wang, Wennie; Janotti, Anderson; Van de Walle, Chris G.
- Journal of Materials Chemistry C, Vol. 4, Issue 27
Will Solar-Driven Water-Splitting Devices See the Light of Day?
journal, September 2013
- McKone, James R.; Lewis, Nathan S.; Gray, Harry B.
- Chemistry of Materials, Vol. 26, Issue 1
Structural and electronic properties of tungsten trioxides: from cluster to solid surface
journal, July 2011
- Jin, Hua; Zhu, Jia; Hu, Jianming
- Theoretical Chemistry Accounts, Vol. 130, Issue 1
Semiconducting materials for photoelectrochemical energy conversion
journal, January 2016
- Sivula, Kevin; van de Krol, Roel
- Nature Reviews Materials, Vol. 1, Issue 2
Energetics and Solvation Effects at the Photoanode/Catalyst Interface: Ohmic Contact versus Schottky Barrier
journal, April 2015
- Ping, Yuan; Goddard, William A.; Galli, Giulia A.
- Journal of the American Chemical Society, Vol. 137, Issue 16
Oxidation and Photo-Oxidation of Water on TiO 2 Surface
journal, June 2008
- Valdés, Á.; Qu, Z. -W.; Kroes, G. -J.
- The Journal of Physical Chemistry C, Vol. 112, Issue 26
Role of the deep-lying electronic states of MoO3 in the enhancement of hole-injection in organic thin films
journal, September 2009
- Kröger, M.; Hamwi, S.; Meyer, J.
- Applied Physics Letters, Vol. 95, Issue 12
Recent Progress in Photoelectrochemical Water Splitting Activity of WO3 Photoanodes
journal, April 2018
- Kalanur, Shankara S.; Duy, Le Thai; Seo, Hyungtak
- Topics in Catalysis, Vol. 61, Issue 9-11
Electronic structure and phase stability of oxide semiconductors: Performance of dielectric-dependent hybrid functional DFT, benchmarked against band structure calculations and experiments
journal, April 2015
- Gerosa, Matteo; Bottani, Carlo Enrico; Caramella, Lucia
- Physical Review B, Vol. 91, Issue 15
Efficient Computation of Hartree–Fock Exchange Using Recursive Subspace Bisection
journal, December 2012
- Gygi, François; Duchemin, Ivan
- Journal of Chemical Theory and Computation, Vol. 9, Issue 1
Two-Dimensional Polaronic Behavior in the Binary Oxides and
journal, March 2012
- McKenna, Keith P.; Wolf, Matthew J.; Shluger, Alexander L.
- Physical Review Letters, Vol. 108, Issue 11
Optimizing the Band Edges of Tungsten Trioxide for Water Oxidation: A First-Principles Study
journal, March 2014
- Ping, Yuan; Galli, Giulia
- The Journal of Physical Chemistry C, Vol. 118, Issue 12
H 2 O Adsorption on WO 3 and WO 3– x (001) Surfaces
journal, June 2017
- Albanese, Elisa; Di Valentin, Cristiana; Pacchioni, Gianfranco
- ACS Applied Materials & Interfaces, Vol. 9, Issue 27
Assessing capability of semiconductors to split water using ionization potentials and electron affinities only
journal, January 2014
- Stevanović, Vladan; Lany, Stephan; Ginley, David S.
- Physical Chemistry Chemical Physics, Vol. 16, Issue 8
Optimization algorithm for the generation of ONCV pseudopotentials
journal, November 2015
- Schlipf, Martin; Gygi, François
- Computer Physics Communications, Vol. 196
Electronic Structure of Defect States in Hydroxylated and Reduced Rutile Surfaces
journal, October 2006
- Di Valentin, Cristiana; Pacchioni, Gianfranco; Selloni, Annabella
- Physical Review Letters, Vol. 97, Issue 16
Efficient iterative method for calculations of dielectric matrices
journal, September 2008
- Wilson, Hugh F.; Gygi, François; Galli, Giulia
- Physical Review B, Vol. 78, Issue 11
Alignment of electronic energy levels at electrochemical interfaces
journal, January 2012
- Cheng, Jun; Sprik, Michiel
- Physical Chemistry Chemical Physics, Vol. 14, Issue 32
Large Scale GW Calculations
journal, May 2015
- Govoni, Marco; Galli, Giulia
- Journal of Chemical Theory and Computation, Vol. 11, Issue 6
An STM study of surface structures on WO3(001)
journal, July 1996
- Jones, F. H.; Rawlings, K.; Foord, J. S.
- Surface Science, Vol. 359, Issue 1-3
Observation of a two-dimensional liquid of Fröhlich polarons at the bare SrTiO3 surface
journal, October 2015
- Chen, Chaoyu; Avila, José; Frantzeskakis, Emmanouil
- Nature Communications, Vol. 6, Issue 1
Works referencing / citing this record:
Dielectric-dependent hybrid functionals for heterogeneous materials
journal, July 2019
- Zheng, Huihuo; Govoni, Marco; Galli, Giulia
- Physical Review Materials, Vol. 3, Issue 7
The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy
journal, July 2019
- Golze, Dorothea; Dvorak, Marc; Rinke, Patrick
- Frontiers in Chemistry, Vol. 7
Dielectric-dependent hybrid functionals for heterogeneous materials
journal, July 2019
- Zheng, Huihuo; Govoni, Marco; Galli, Giulia
- Physical Review Materials, Vol. 3, Issue 7
The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy
journal, July 2019
- Golze, Dorothea; Dvorak, Marc; Rinke, Patrick
- Frontiers in Chemistry, Vol. 7
Surface depletion field in 2D perovskite microplates: Structural phase transition, quantum confinement and Stark effect
journal, October 2019
- Li, Wancai; Fang, Chen; Wang, Haizhen
- Nano Research, Vol. 12, Issue 11
The dual-defective SnS 2 monolayers: promising 2D photocatalysts for overall water splitting
journal, January 2019
- Sainbileg, Batjargal; Lai, Ying-Ren; Chen, Li-Chyong
- Physical Chemistry Chemical Physics, Vol. 21, Issue 48
Nanostructured tungsten oxide thin film devices: from optoelectronics and ionics to iontronics
journal, January 2019
- Hai, Zhenyin; Wei, Zihan; Xue, Chenyang
- Journal of Materials Chemistry C, Vol. 7, Issue 42
Quasi-degenerate states and their dynamics in oxygen deficient reducible metal oxides
journal, February 2020
- Daelman, Nathan; Hegner, Franziska Simone; Rellán-Piñeiro, Marcos
- The Journal of Chemical Physics, Vol. 152, Issue 5
Optical absorption induced by small polaron formation in transition metal oxides: The case of
journal, October 2019
- Smart, Tyler J.; Pham, Tuan Anh; Ping, Yuan
- Physical Review Materials, Vol. 3, Issue 10