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.

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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
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• Generalized density functional theory framework for the non-linear density response of quantum many-body systems