Structural Stability and Defect Energetics of ZnO from Diffusion Quantum Monte Carlo

Abstract

We have applied the many-body ab-initio diffusion quantum Monte Carlo (DMC) method to study Zn and ZnO crystals under pressure, and the energetics of the oxygen vacancy, zinc interstitial and hydrogen impurities in ZnO. We show that DMC is an accurate and practical method that can be used to characterize multiple properties of materials that are challenging for density functional theory approximations. DMC agrees with experimental measurements to within 0.3 eV, including the band-gap of ZnO, the ionization potential of O and Zn, and the atomization energy of O${}_2$, ZnO dimer, and wurtzite ZnO. DMC predicts the oxygen vacancy as a deep donor with a formation energy of 5.0(2) eV under O-rich conditions and thermodynamic transition levels located between 1.8 and 2.5 eV from the valence band maximum. Our DMC results indicate that the concentration of zinc interstitial and hydrogen impurities in ZnO should be low under n-type, and Zn- and H-rich conditions because these defects have formation energies above 1.4 eV under these conditions. Comparison of DMC and hybrid functionals shows that these DFT approximations can be parameterized to yield a general correct qualitative description of ZnO. However, the formation energy of defects in ZnO evaluated with DMC and hybrid functionals can differ by more than 0.5 eV.

43 pages, 10 figures

References in corpus (34)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Anion vacancies as a source of persistent photoconductivity in II-VI and chalcopyrite semiconductors
• Continuum variational and diffusion quantum Monte Carlo calculations
• Twist-averaged Boundary Conditions in Continuum Quantum Monte Carlo
• Optimization of quantum Monte Carlo wave functions by energy minimization
• Rich variety of defects in ZnO via an attractive interaction between O-vacancies and Zn-interstitials
• The Finite Size Error in Many-body Simulations with long-Ranged Interactions
• Finite-size errors in continuum quantum Monte Carlo calculations
• Beyond the locality approximation in the standard diffusion Monte Carlo method
• Correlated geminal wave function for molecules: an efficient resonating valence bond approach
• Applications of quantum Monte Carlo methods in condensed systems
• Geminal wavefunctions with Jastrow correlation: a first application to atoms
• Manybody GW calculation of the oxygen vacancy in ZnO
• Insulator-to-Metal Transition in Selenium-Hyperdoped Silicon: Observation and Origin
• Size-consistent variational approaches to non-local pseudopotentials: standard and lattice regularized diffusion Monte Carlo methods revisited
• Finite-size correction in many-body electronic structure calculations
• Finite size errors in quantum many-body simulations of extended systems
• Transferable relativistic Dirac-Slater pseudopotentials
• Structural properties and enthalpy of formation of magnesium hydride from quantum Monte Carlo calculations
• Quantum Monte Carlo applied to solids
• Ab initio quantum Monte Carlo calculations of spin superexchange in cuprates: the benchmarking case of Ca${}_2$CuO${}_3$
• The Schottky defect formation energy in MgO calculated by diffusion Monte Carlo
• The effect of electron correlation on the electronic structure and spin-lattice coupling of the high-T${}_c$ cuprates: quantum Monte Carlo calculations
• Computing the energy of a water molecule using MultiDeterminants: A simple, efficient algorithm
• Quantum Monte Carlo calculations of structural properties of FeO under pressure
• Point-Defect Optical Transitions and Thermal Ionization Energies from Quantum Monte Carlo Methods: Application to F-center Defect in MgO
• Structural Stability and Defect Energetics of ZnO from Diffusion Quantum Monte Carlo
• Excited state calculations in solids by auxiliary-field quantum Monte Carlo
• Diffusion quantum Monte Carlo study of the equation of state and point defects in aluminum
• Fundamental high pressure calibration from all-electron quantum Monte Carlo calculations
• Accuracy of Quantum Monte Carlo Methods for Point Defects in Solids
• Self-healing diffusion quantum Monte Carlo algorithms: methods for direct reduction of the fermion sign error in electronic structure calculations
• Equations of state and stability of MgSiO${}_3$ perovskite and post-perovskite phases from quantum Monte Carlo simulations
• Oxygen vacancy and EC - 1 eV electron trap in ZnO

Cited by in corpus (23)

• QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids
• Phase Stability of TiO${}_2$ Polymorphs from Diffusion Quantum Monte Carlo
• Discovering correlated fermions using quantum Monte Carlo
• Structural Stability and Defect Energetics of ZnO from Diffusion Quantum Monte Carlo
• A first-principles Quantum Monte Carlo study of two-dimensional (2D) GaSe
• Towards a systematic assessment of errors in diffusion Monte Carlo calculations of semiconductors: case study of zinc selenide and zinc oxide
• Cohesive energy and structural parameters of binary oxides of groups IIA and IIIB from diffusion quantum Monte Carlo
• Diffusion quantum Monte Carlo calculations of SrFeO${}_3$ and LaFeO${}_3$
• Charge density and redox potential of LiNiO2 using ab initio diffusion quantum Monte Carlo
• Systematic DFT+U and Quantum Monte Carlo benchmark of magnetic two-dimensional (2D) CrX${}_3$ (X = I, Br, Cl, F)
• Quantum Monte Carlo analysis of a charge ordered insulating antiferromagnet: the Ti${}_4$O${}_7$ Magnéli phase
• On the accuracy of the HSE hybrid functional to describe many-electron interactions and charge localization in semiconductors
• Magnitude of pseudopotential localization errors in fixed node diffusion quantum Monte Carlo
• Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory
• The intrinsic ferromagnetism of two-dimensional (2D) MnO${}_2$ revisited: A many-body Quantum Monte Carlo and DFT+U study
• Structural, Electronic and Magnetic Properties of Bulk and Epitaxial LaCoO${}_3$ through Diffusion Monte Carlo
• Error Cancellation in Diffusion Monte Carlo Calculations of Surface Chemistry
• A pathway towards high throughput Quantum Monte Carlo simulations for alloys: A case study of two-dimensional (2D) $Ga{S}_{x}S{e}_{1-x}$
• Locality Error Free Effective Core Potentials for 3d Transition Metal Elements Developed for the Diffusion Monte Carlo Method
• Optimization and parallelization of B-spline based orbital evaluations in QMC on multi/many-core shared memory processors
• Prediction for the singlet-triplet excitation energy for the spinel MgTi${}_2$O${}_4$ using first-principles diffusion Monte Carlo
• Defect energetics of cubic hafnia from quantum Monte Carlo simulations
• General embedded cluster protocol for accurate modeling of oxygen vacancies in metal-oxides