Nonlocal Pseudopotential Energy Density Functional for Orbital-Free Density Functional Theory

Abstract

Orbital-free density functional theory (OF-DFT) runs at low computational cost that scales linearly with the number of simulated atoms, making it suitable for large-scale material simulations. It is generally considered that OF-DFT strictly requires the use of local pseudopotentials, rather than orbital-dependent nonlocal pseudopotentials, for the calculation of electron-ion interaction energies, as no orbitals are available. This is unfortunate situation since the nonlocal pseudopotentials are known to give much better transferability and calculation accuracy than local ones. We report here the development of a theoretical scheme that allows the direct use of nonlocal pseudopotentials in OF-DFT. In this scheme, a nonlocal pseudopotential energy density functional is derived by the projection of nonlocal pseudopotential onto the non-interacting density matrix (instead of 'orbitals') that can be approximated explicitly as a functional of electron density. Our development defies the belief that nonlocal pseudopotentials are not applicable to OF-DFT, leading to the creation of an alternate theoretical framework of OF-DFT that works superior to the traditional one.

arXiv comment8 pages, 4 figures

References in corpus (16)

• CALYPSO: a method for crystal structure prediction
• Crystal Structure Prediction via Particle Swarm Optimization
• Ab initio pseudopotentials for electronic structure calculations of poly-atomic systems using density-functional theory
• Non-empirical Generalized Gradient Approximation Free Energy Functional for Orbital-free Simulations
• A Simple Generalized Gradient Approximation for the Non-interacting Kinetic Energy Density Functional
• Orbital-Free Density Functional Theory Implementation with the Projector Augmented-Wave Method
• Semilocal Pauli-Gaussian Kinetic Functionals for Orbital-Free Density Functional Theory Calculations of Solids
• Nonlocal Kinetic Energy Functionals By Functional Integration
• ATLAS: A Real-Space Finite-Difference Implementation of Orbital-Free Density Functional Theory
• Kinetic Energy Density Study of Some Representative Semilocal Kinetic Energy Functionals
• Orbital-Free DFT Correctly Models Quantum Dots When Asymptotics, Nonlocality and Nonhomogeneity Are Accounted For
• Non-local kinetic energy functional from the Jellium-with-gap model: applications to Orbital-Free Density Functional Theory
• Towards accurate orbital-free simulations: a generalized gradient approximation for the non-interacting free energy density functional
• Jellium-with-gap model applied to semilocal kinetic functionals
• Kinetic energy density functionals from the Airy gas, with an application to the atomization kinetic energies of molecules
• Nonlocal Kinetic Energy Density Functionals for Isolated Systems via Local Density Approximation Kernels

Cited by in corpus (8)

• Nonlocal Machine-Learned Exchange Functional for Molecules and Solids
• Machine learning of kinetic energy densities with target and feature averaging: better results with fewer training data
• A machine-learned kinetic energy model for light weight metals and compounds of group III-V elements
• Nonlocal vs Local Pseudopotentials Affect Kinetic Energy Kernels in Orbital-Free DFT
• Assessing the source of error in the Thomas-Fermi-von Weizsäcker density functional
• Nonlocal free-energy density functional for warm dense matter
• Machine learning-guided construction of an analytic kinetic energy functional for orbital free density functional theory
• Unlocking the Power of Orbital-Free Density Functional Theory to Explore the Electronic Structure Under Extreme Conditions