Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Finite-size correction for slab supercell calculations of materials with spontaneous polarization

Journal Article · · npj Computational Materials
; ; ; ; ;
Abstract

The repeated slab approach has become a de facto standard to accurately describe surface properties of materials by density functional theory calculations with periodic boundary conditions. For materials exhibiting spontaneous polarization, we show that the conventional scheme of passivation with pseudo hydrogen is unable to realize a charge-neutral surface. The presence of a net surface charge induces via Gauss’s law a macroscopic electric field through the slab and results in poor size convergence with respect to the thickness of the slab. We propose a modified passivation method that accounts for the effect of spontaneous polarization, describes the correct bulk limits and boosts convergence with respect to slab thickness. The robustness, reliability, and superior convergence of energetics and electronic structure achieved by the proposed method are demonstrated using the example of polar ZnO surfaces.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0010689
OSTI ID:
1779987
Alternate ID(s):
OSTI ID: 1851420
Journal Information:
npj Computational Materials, Journal Name: npj Computational Materials Journal Issue: 1 Vol. 7; ISSN 2057-3960
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

References (59)

Elucidation of the Electrochemical Activation of Water over Pd by First Principles journal January 2006
Electrostatic interactions between charged defects in supercells journal December 2010
Polarization, piezoelectric constants, and elastic constants of ZnO, MgO, and CdO journal April 2006
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface journal January 2004
Optical control of polarization in ferroelectric heterostructures journal August 2018
Manipulating topological transformations of polar structures through real-time observation of the dynamic polarization evolution journal October 2019
Molecular catalysis at polarized interfaces created by ferroelectric BaTiO 3 journal January 2017
Spontaneous polarization field-enhanced charge separation for an iron oxide photo-catalyst journal January 2017
Hybrid functionals based on a screened Coulomb potential journal May 2003
First-principles calculations for defects and impurities: Applications to III-nitrides journal April 2004
A comprehensive review of ZnO materials and devices journal August 2005
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] journal June 2006
Exact exchange plane-wave-pseudopotential calculations for slabs journal May 2014
First-principles study of vacancy-assisted impurity diffusion in ZnO journal September 2014
Field-evaporation from first-principles journal May 2004
Generalized dipole correction for charged surfaces in the repeated-slab approach journal July 2020
Electron counting model and its application to island structures on molecular-beam epitaxy grown GaAs(001) and ZnSe(001) journal November 1989
Adsorbate-substrate and adsorbate-adsorbate interactions of Na and K adlayers on Al(111) journal December 1992
Theory of polarization of crystalline solids journal January 1993
Electric polarization as a bulk quantity and its relation to surface charge journal August 1993
Ab initio study of piezoelectricity and spontaneous polarization in ZnO journal October 1994
Projector augmented-wave method journal December 1994
Atomic and electronic structure of the GaAs/ZnSe(001) interface journal September 1994
Periodic boundary conditions in ab initio calculations journal February 1995
Lattice dynamics and hyperfine interactions in ZnO and ZnSe at high external pressures journal May 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Spontaneous polarization and piezoelectric constants of III-V nitrides journal October 1997
High-density phases of ZnO: Structural and compressive parameters journal December 1998
Valence-band ordering in ZnO journal July 1999
Polarization properties of ZnO and BeO: An ab initio study through the Berry phase and Wannier functions approaches journal December 2001
Competing stabilization mechanism for the polar ZnO(0001)-Zn surface journal December 2003
Reconstruction of charged surfaces: General trends and a case study of Pt(110) and Au(110) journal December 2003
Defect energetics in ZnO: A hybrid Hartree-Fock density functional study journal June 2008
Hydrogen adsorption on polar ZnO(0001)-Zn: Extending equilibrium surface phase diagrams to kinetically stabilized structures journal October 2010
GaN(0001) surface states: Experimental and theoretical fingerprints to identify surface reconstructions journal September 2013
First-principles Green's-function method for surface calculations: A pseudopotential localized basis set approach journal November 2017
Exact exchange potential for slabs: Asymptotic behavior of the Krieger-Li-Iafrate approximation journal February 2018
First-principles calculations for charged defects at surfaces, interfaces, and two-dimensional materials in the presence of electric fields journal May 2018
Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations journal January 2009
Temperature Stabilized Surface Reconstructions at Polar ZnO(0001) journal August 2009
First-Principles Molecular Dynamics at a Constant Electrode Potential journal December 2012
Finite-Size Supercell Correction for Charged Defects at Surfaces and Interfaces journal February 2013
Concentration of Vacancies at Metal-Oxide Surfaces: Case Study of MgO(100) journal July 2013
Selective Solvent-Induced Stabilization of Polar Oxide Surfaces in an Electrochemical Environment journal February 2018
First-Principles Approach to Model Electrochemical Reactions: Understanding the Fundamental Mechanisms behind Mg Corrosion journal June 2018
Ab initio Description of Bond Breaking in Large Electric Fields journal April 2020
External-charge-induced surface reconstruction on Ag(110) journal October 1989
Generalized Gradient Approximation Made Simple journal October 1996
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] journal February 1997
First-Principles Surface Phase Diagram for Hydrogen on GaN Surfaces journal January 2002
Novel Stabilization Mechanism on Polar Surfaces: ZnO(0001)-Zn journal January 2003
Kohn-Sham Exchange Potential for a Metallic Surface journal July 2006
Macroscopic polarization in crystalline dielectrics: the geometric phase approach journal July 1994
Orbital-dependent density functionals: Theory and applications journal January 2008
First-principles calculations for point defects in solids journal March 2014
A New Slab Model Approach for Electronic Structure Calculation of Polar Semiconductor Surface journal October 1990
Oxide Surface Science journal March 2010
Review—Visible LEDs: More than Efficient Light journal November 2019

Similar Records

Finite-size correction for slab supercell calculations of materials with spontaneous polarization
Journal Article · Thu Apr 29 00:00:00 EDT 2021 · npj Computational Materials · OSTI ID:1851420
Lifetime distribution of spontaneous emission from an assembly of atoms in a dielectric slab
Journal Article · Fri Feb 28 23:00:00 EST 2003 · Physical Review. A · OSTI ID:20633909
Spontaneous emission interference enhancement with a {mu}-negative metamaterial slab
Journal Article · Thu Sep 15 00:00:00 EDT 2011 · Physical Review. A · OSTI ID:22072199

Related Subjects