Dynamical structure factors of Warm Dense Matter from Time-Dependent Orbital-Free and Mixed-Stochastic-Deterministic Density Functional Theory

TL;DR

This paper compares two computational methods, TD-OF-DFT and mixed TD-KS-DFT, for calculating the dynamical structure factor of warm dense matter, highlighting their accuracy and efficiency trade-offs in interpreting X-ray scattering data.

Contribution

It introduces and evaluates the first application of TD-OF-DFT and mixed TD-KS-DFT to WDM, demonstrating their respective strengths and limitations compared to traditional methods.

Findings

TD-OF-DFT requires a dynamic kinetic energy potential to capture plasmon response.

Mixed TD-KS-DFT aligns well with experimental data for bound and free electrons.

TD-OF-DFT is faster but less accurate; mixed TD-KS-DFT is more accurate but computationally intensive.

Abstract

We present the first calculations of the inelastic part of the dynamical structure factor (DSF) for warm dense matter (WDM) using Time-Dependent Orbital-Free Density Functional Theory (TD-OF-DFT) and Mixed-Stochastic-Deterministic (mixed) Kohn Sham TD-DFT (KS TD-DFT). WDM is an intermediate phase of matter found in planetary cores and laser-driven experiments, where the accurate calculation of the DSF is critical for interpreting X-ray Thomson scattering (XRTS) measurements. Traditional TD-DFT methods, while highly accurate, are computationally expensive, motivating the exploration of TD-OF-DFT and mixed TD-KS-DFT as more efficient alternatives. We applied these methods to experimentally measured WDM systems, including solid-density aluminum and beryllium, compressed beryllium, and carbon-hydrogen mixtures. Our results show that TD-OF-DFT requires a dynamical kinetic energy potential in order to qualitatively capture the plasmon response. Additionally, it struggles with capturing bound electron contributions and accurately modeling plasmon dynamics without the inclusion of a dynamic kinetic energy potential. In contrast, mixed TD-KS-DFT offers greater accuracy in distinguishing bound and free electron effects, aligning well with experimental data, though at a higher computational cost. This study highlights the trade-offs between computational efficiency and accuracy, demonstrating that TD-OF-DFT remains a valuable tool for rapid scans of parameter space, while mixed TD-KS-DFT should be preferred for high-fidelity simulations. Our findings provide insight into the future development of DFT methods for WDM and suggest potential improvements for TD-OF-DFT.