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Title: Resolution of the Band Gap Prediction Problem for Materials Design

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [1];  [1]
  1. Materials and Process Simulation Center, MC139-74, California Institute of Technology, Pasadena, California 91125, United States
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An important property with any new material is the band gap. Standard density functional theory methods grossly underestimate band gaps. This is known as the band gap problem. Here in this paper, we show that the hybrid B3PW91 density functional returns band gaps with a mean absolute deviation (MAD) from experiment of 0.22 eV over 64 insulators with gaps spanning a factor of 500 from 0.014 to 7 eV. The MAD is 0.28 eV over 70 compounds with gaps up to 14.2 eV, with a mean error of -0.03 eV. To benchmark the quality of the hybrid method, we compared the hybrid method to the rigorous GW many-body perturbation theory method. Surprisingly, the MAD for B3PW91 is about 1.5 times smaller than the MAD for GW. Furthermore, B3PW91 is 3-4 orders of magnitude faster computationally. Hence, B3PW91 is a practical tool for predicting band gaps of materials before they are synthesized and represents a solution to the band gap prediction problem.

Research Organization:
California Institute of Technology (CalTech), Pasadena, CA (United States)
Sponsoring Organization:
USDOE; National Science Foundation (NSF)
Grant/Contract Number:
SC0004993
OSTI ID:
1328820
Alternate ID(s):
OSTI ID: 1436091
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Vol. 7 Journal Issue: 7; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 182 works
Citation information provided by
Web of Science

References (36)

Generalized Gradient Approximation Made Simple journal October 1996
Density‐functional thermochemistry. III. The role of exact exchange journal April 1993
Improved semiconductor lattice parameters and band gaps from a middle-range screened hybrid exchange functional journal March 2012
Efficient implementation of the G W approximation within the all-electron FLAPW method journal March 2010
Systematically convergent basis sets with relativistic pseudopotentials. II. Small-core pseudopotentials and correlation consistent basis sets for the post- d group 16–18 elements journal December 2003
Electronic phase transitions of bismuth under strain from relativistic self-consistent G W calculations journal March 2015
Density-functional exchange-energy approximation with correct asymptotic behavior journal September 1988
Influence of the exchange screening parameter on the performance of screened hybrid functionals journal December 2006
Energy band gaps and lattice parameters evaluated with the Heyd-Scuseria-Ernzerhof screened hybrid functional journal November 2005
Antiferromagnetic band structure of La 2 CuO 4 :  Becke-3–Lee-Yang-Parr calculations journal March 2001
Density-based mixing parameter for hybrid functionals journal January 2011
On the prediction of band gaps from hybrid functional theory journal July 2001
Localization and Delocalization Errors in Density Functional Theory and Implications for Band-Gap Prediction journal April 2008
Band-edge positions in G W : Effects of starting point and self-consistency journal October 2014
Relativistic energy-consistent pseudopotentials?Recent developments journal April 2002
Quasiparticle band structure of thirteen semiconductors and insulators journal June 1991
Accurate Ab Initio Quantum Mechanics Simulations of Bi 2 Se 3 and Bi 2 Te 3 Topological Insulator Surfaces journal September 2015
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies journal October 1986
Accurate Band Gaps for Semiconductors from Density Functional Theory journal January 2011
Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation journal September 1992
Band-edge levels in semiconductors and insulators: Hybrid density functional theory versus many-body perturbation theory journal July 2012
Predicted roles of defects on band offsets and energetics at CIGS (Cu(In,Ga)Se 2 /CdS) solar cell interfaces and implications for improving performance journal September 2014
Core polarization in solids: Formulation and application to semiconductors journal September 1997
Quasiparticle energies in GaAs and AlAs journal March 1987
Self-interaction correction to density-functional approximations for many-electron systems journal May 1981
All-Electron Self-Consistent G W Approximation: Application to Si, MnO, and NiO journal September 2004
Ab Initio Prediction of Conduction Band Spin Splitting in Zinc Blende Semiconductors journal March 2006
Accurate Quasiparticle Spectra from Self-Consistent GW Calculations with Vertex Corrections journal December 2007
Definitive Band Gaps for Single-Wall Carbon Nanotubes journal September 2010
Photoemission from Rare-Gas Solids: Electron Energy Distributions from the Valence Bands journal March 1975
Analysis of the Heyd-Scuseria-Ernzerhof density functional parameter space journal May 2012
Quasiparticle band structures of the antiferromagnetic transition-metal oxides MnO, FeO, CoO, and NiO journal June 2009
Correspondence of defect energy levels in hybrid density functional theory and many-body perturbation theory journal September 2013
Spin-orbit splittings and energy band gaps calculated with the Heyd-Scuseria-Ernzerhof screened hybrid functional journal August 2006
Semiconductors: Data Handbook book January 2004
Physical Content of the Exact Kohn-Sham Orbital Energies: Band Gaps and Derivative Discontinuities journal November 1983

Figures / Tables (3)

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Figure 2(p. 3)figure Figure 2
Figure 3(p. 4)figure Figure 3

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36 MATERIALS SCIENCE