Ab initio Static Exchange-Correlation Kernel across Jacob's Ladder without functional derivatives

Abstract

The electronic exchange-correlation (XC) kernel constitutes a fundamental input for the estimation of a gamut of material properties such as the dielectric characteristics, the thermal and electrical conductivity, or the response to an external perturbation. In practice, no reliable method has been known that allows to compute the kernel of real materials with arbitrary XC functionals. In this work, we overcome this long-standing limitation by introducing a new, formally exact methodology for the computation of the material specific static XC kernel exclusively within the framework of density functional theory (DFT) and without employing functional derivatives -- no external input apart from the usual XC-functional is required. We compare our new results with exact quantum Monte Carlo (QMC) data for the archetypical uniform electron gas model at both ambient and warm dense matter conditions. This gives us unprecedented insights into the performance of different XC-functionals, and has important implications for the development of new functionals that are designed for the application at extreme temperatures. In addition, we obtain new DFT results for the XC kernel of warm dense hydrogen as it occurs in fusion applications and astrophysical objects. The observed excellent agreement to the QMC reference data demonstrates that our framework is capable to capture nontrivial effects such as XC-induced isotropy breaking in the density response of hydrogen at large wave numbers.

References in corpus (12)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Observation of the Wigner-Huntington Transition to Solid Metallic Hydrogen
• {\em Ab initio} Quantum Monte Carlo simulation of the warm dense electron gas in the thermodynamic limit
• Ab initio equations of state for hydrogen (H-REOS.3) and helium (He-REOS.3) and their implications for the interior of Brown Dwarfs
• Nonlinear Electronic Density Response in Warm Dense Matter
• Dynamic properties of the warm dense electron gas: an ab initio path integral Monte Carlo approach
• Dynamical structure factor of strongly coupled ions in a dense quantum plasma
• The Relevance of Electronic Perturbations in the Warm Dense Electron Gas
• Integral equation theory based dielectric scheme for strongly coupled electron liquids
• Nonlinear Density Response and Higher Order Correlation Functions in Warm Dense Matter
• Density-Functional-Theory Perspective on the Non-Linear Response of Correlated Electrons Across Temperature Regimes

Cited by in corpus (17)

• Electronic Density Response of Warm Dense Matter
• First principles simulations of dense hydrogen
• X-ray Thomson scattering spectra from DFT-MD simulations based on a modified Chihara formula
• Linear-response time-dependent density functional theory approach to warm dense matter with adiabatic exchange--correlation kernels
• Non-empirical mixing coefficient for hybrid XC functionals from analysis of the XC kernel
• Assessing the accuracy of hybrid exchange-correlation functionals for the density response of warm dense electrons
• From Density Response to Energy Functionals and Back: An ab initio perspective on Matter Under Extreme Conditions
• Model-free Rayleigh weight from x-ray Thomson scattering measurements
• Averaging over atom snapshots in linear-response TDDFT of disordered systems: A case study of warm dense hydrogen
• Imposing Correct Jellium Response Is Key to Predict the Density Response by Orbital-Free DFT
• Revisiting the Vashishta-Singwi dielectric scheme for the warm dense uniform electron fluid
• Virial coefficients of the Uniform Electron Gas from Path Integral Monte Carlo Simulations
• Nonlocal vs Local Pseudopotentials Affect Kinetic Energy Kernels in Orbital-Free DFT
• Excitation signatures of isochorically heated electrons in solids at finite wavenumber explored from first principles
• Ultrafast Heating Induced Suppression of $d$-band Dominance in the Electronic Excitation Spectrum of Cuprum
• Ab initio density functional theory approach to warm dense hydrogen: from density response to electronic correlations
• Generalized density functional theory framework for the non-linear density response of quantum many-body systems