Analysis of dynamical effects in the uniform electron liquids with the self-consistent method of moments complemented by the Shannon information entropy and the path-integral Monte-Carlo simulations

TL;DR

This paper introduces a novel non-perturbative approach combining the method of moments, Shannon entropy maximization, and path-integral Monte Carlo simulations to analyze the dynamical properties of uniform electron liquids across various densities and temperatures.

Contribution

The study develops a self-consistent method of moments complemented by Shannon entropy and PIMC simulations, providing new insights into the dynamical structure factor of electron liquids.

Findings

Revealed bi-modal excitation spectrum at strong coupling

Identified roton-like features in the excitation spectrum

Validated the method against existing ab initio approaches

Abstract

Dynamical properties of uniform electron fluids (jellium model) are studied within a novel non-perturbative approach consisting in the combination of the self-consistent version of the method of moments (SCMM) involving up to nine sum rules and other exact relations, the two-parameter Shannon information entropy maximization procedure, and the ab initio path integral Monte Carlo (PIMC) simulations of the imaginary-time intermediate scattering function. The explicit dependence of the electronic dynamic structure factor (DSF) on temperature and density is studied in a broad realm of variation of the dimensionless parameters ($2\leq r_s\leq 36$ and $1\leq \theta \leq 8$). When the coupling is strong ($r_s\geq 16$) we clearly observe a bi-modal structure of the excitation spectrum with a lower-energy mode possessing a well pronounced roton-like feature ($\theta \leq 2$) and an additional high-energy branch within the roton region which evolves into the strongly overdamped high-frequency shoulder when the coupling decreases ($r_s\leq 10$). We are not aware of any reconstruction of the DSF at these conditions with the effects of dynamical correlations, included here via the intermediate scattering and the dynamical Nevanlinna parameter functions. The standard static-local-field approach fails to reproduce this effect. The reliability of our method is confirmed by a detailed comparison with the recent ab initio dynamic-local-field approach by Dornheim et al. [Phys.Rev.Lett. 121, 255001 (2018)] available for high/moderate densities ($r_s\leq 10$). Moreover, within the SCMM we are able to construct the modes dispersion equation in a closed analytical form and find the decrements (lifetimes) of the quasiparticle excitations explicitly. The physical nature of the revealed modes is discussed. Mathematical details of the method are complemented in the Supplementary Material.