Imposing Correct Jellium Response Is Key to Predict the Density Response by Orbital-Free DFT

Abstract

Orbital-free density functional theory (OF-DFT) constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends on the employed kinetic energy (KE) density functional, which has to be supplied as an external input. In this work we consider several nonlocal and Laplacian-level KE functionals and use an external harmonic perturbation to compute the static density response at T=0 K in the linear and beyond linear response regimes. We test for the satisfaction of exact conditions in the limit of uniform densities and for how approximate KE functionals reproduce the density response of realistic materials (e.g., Al and Si) against the Kohn-Sham DFT reference which employs the exact KE. The results illustrate that several functionals violate exact conditions in the UEG limit. We find a strong correlation between the accuracy of the KE functionals in the UEG limit and in the strongly inhomogeneous case. This empirically demonstrates the importance of imposing the limit of UEG response for uniform densities and validates the use of the Lindhard function in the formulation of kernels for nonlocal functionals. This conclusion is substantiated by additional calculations for bulk Aluminum (Al) with a face-centered cubic (fcc) lattice and Silicon (Si) with an fcc lattice, body-centered cubic (bcc) lattice, and semiconducting crystal diamond (cd) state. The analysis of fcc Al, and fcc as well as bcc Si data follows closely the conclusions drawn for the UEG, allowing us to extend our conclusions to realistic systems that are subject to density inhomogeneities induced by ions.

References in corpus (43)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• A real-space grid implementation of the Projector Augmented Wave method
• The Uniform Electron Gas at Warm Dense Matter Conditions
• Theoretical foundations of quantum hydrodynamics for plasmas
• A Simple Generalized Gradient Approximation for the Non-interacting Kinetic Energy Density Functional
• Statically screened ion potential and Bohm potential in a quantum plasma
• Electronic Density Response of Warm Dense Matter
• Semilocal Pauli-Gaussian Kinetic Functionals for Orbital-Free Density Functional Theory Calculations of Solids
• Nonlocal Kinetic Energy Functionals By Functional Integration
• Nonlinear Electronic Density Response in Warm Dense Matter
• Fast and accurate quantum molecular dynamics of dense plasmas across temperature regimes
• DFTpy: An efficient and object-oriented platform for orbital-free DFT simulations
• Orbital-Free DFT Correctly Models Quantum Dots When Asymptotics, Nonlocality and Nonhomogeneity Are Accounted For
• Density Response of the Warm Dense Electron Gas beyond Linear Response Theory: Excitation of Harmonics
• Electronic Density Response of Warm Dense Hydrogen: Ab initio Path Integral Monte Carlo Simulations
• Dynamical structure factor of strongly coupled ions in a dense quantum plasma
• Laplacian-Level Quantum Hydrodynamic Theory for Plasmonics
• Towards accurate orbital-free simulations: a generalized gradient approximation for the non-interacting free energy density functional
• Ionic and electronic transport properties in dense plasmas by orbital-free density functional theory
• Ab initio Static Exchange-Correlation Kernel across Jacob's Ladder without functional derivatives
• Scaling of Magneto-Quantum-Radiative Hydrodynamic Equations: From Laser-produced Plasmas to Astrophysics
• Jellium-with-gap model applied to semilocal kinetic functionals
• The Relevance of Electronic Perturbations in the Warm Dense Electron Gas
• Time-dependent Orbital-free Density Functional Theory: Background and Pauli kernel approximations
• Benchmarking Exchange-Correlation Functionals in the Spin-Polarized Inhomogeneous Electron Gas under Warm Dense Conditions
• Screening of a test charge in a free-electron gas at warm dense matter and dense non-ideal plasma conditions
• Ion Potential in Non-ideal Dense Quantum Plasmas
• Linear-response time-dependent density functional theory approach to warm dense matter with adiabatic exchange--correlation kernels
• Gradient correction and Bohm potential for 2D and 1D electron gases at a finite temperature
• Shock Physics in Warm Dense Matter--a quantum hydrodynamics perspective
• Non-empirical mixing coefficient for hybrid XC functionals from analysis of the XC kernel
• Accelerating Equilibration in First-Principles Molecular Dynamics with Orbital-Free Density Functional Theory
• Assessing the accuracy of hybrid exchange-correlation functionals for the density response of warm dense electrons
• Properties of carbon up to 10 million kelvin from Kohn-Sham density functional theory molecular dynamics
• An \textit{ab initio} study of shock-compressed copper
• An Efficient DFT Solver for Nanoscale Simulations and Beyond
• Nonlinear electromagnetic response of a uniform electron gas
• Towards a Quantum Fluid Theory of Correlated Many-Fermion Systems from First Principles
• Unravelling the nonlinear ideal density response of many-body systems
• Averaging over atom snapshots in linear-response TDDFT of disordered systems: A case study of warm dense hydrogen
• Nonlocal and nonadiabatic Pauli potential for time-dependent orbital-free density functional theory
• Coupled Maxwell and Time-Dependent Orbital Free Density Functional Calculations

Cited by in corpus (7)

• First principles simulations of dense hydrogen
• From Density Response to Energy Functionals and Back: An ab initio perspective on Matter Under Extreme Conditions
• Averaging over atom snapshots in linear-response TDDFT of disordered systems: A case study of warm dense hydrogen
• Nonlocal vs Local Pseudopotentials Affect Kinetic Energy Kernels in Orbital-Free DFT
• Nonlocal free-energy density functional for warm dense matter
• Generalized density functional theory framework for the non-linear density response of quantum many-body systems
• Unlocking the Power of Orbital-Free Density Functional Theory to Explore the Electronic Structure Under Extreme Conditions