Fast and Universal Kohn Sham Density Functional Theory Algorithm for Warm Dense Matter to Hot Dense Plasma

Abstract

Understanding many processes, e.g. fusion experiments, planetary interiors and dwarf stars, depends strongly on microscopic physics modeling of warm dense matter (WDM) and hot dense plasma. This complex state of matter consists of a transient mixture of degenerate and nearly-free electrons, molecules, and ions. This regime challenges both experiment and analytical modeling, necessitating predictive \emph{ab initio} atomistic computation, typically based on quantum mechanical Kohn-Sham Density Functional Theory (KS-DFT). However, cubic computational scaling with temperature and system size prohibits the use of DFT through much of the WDM regime. A recently-developed stochastic approach to KS-DFT can be used at high temperatures, with the exact same accuracy as the deterministic approach, but the stochastic error can converge slowly and it remains expensive for intermediate temperatures (<50 eV). We have developed a universal mixed stochastic-deterministic algorithm for DFT at any temperature. This approach leverages the physics of KS-DFT to seamlessly integrate the best aspects of these different approaches. We demonstrate that this method significantly accelerated self-consistent field calculations for temperatures from 3 to 50 eV, while producing stable molecular dynamics and accurate diffusion coefficients.

References in corpus (21)

• Relativistic separable dual-space Gaussian Pseudopotentials from H to Rn
• Thermal and electrical conductivity of iron at Earth's core conditions
• The Interiors of Giant Planets: Models and Outstanding Questions
• Nightside condensation of iron in an ultra-hot giant exoplanet
• Local Spin-density Approximation Exchange-correlation Free-energy Functional
• Large scale ab initio calculations based on three levels of parallelization
• A multiphase equation of state for carbon addressing high pressures and temperatures
• The importance of finite-temperature exchange-correlation for warm dense matter calculations
• Ab initio thermodynamic results for the degenerate electron gas at finite temperature
• All-Electron Path Integral Monte Carlo Simulations of Warm Dense Matter: Application to Water and Carbon Plasmas
• The Fermion Sign Problem in Path Integral Monte Carlo Simulations: Quantum Dots, Ultracold Atoms, and Warm Dense Matter
• Self-averaging stochastic Kohn-Sham density functional theory
• Calculation of a Deuterium Double Shock Hugoniot from Ab initio Simulations
• Extended First-Principles Molecular Dynamics Method From Cold Materials to Hot Dense Plasmas
• Embedded fragment stochastic density functional theory
• Stochastic Density Functional Theory at Finite Temperatures
• Influence of finite temperature Exchange-Correlation effects in Hydrogen
• Stochastic density functional theory
• Parallel eigensolvers in plane-wave Density Functional Theory
• Overlapped Embedded Fragment Stochastic Density Functional Theory for Covalently Bonded Materials
• Stochastic embedding DFT: theory and application to p-nitroaniline

Cited by in corpus (17)

• First principles simulations of dense hydrogen
• Requirements for very high temperature Kohn-Sham density functional simulations and how to bypass them
• Abinit 2025: New Capabilities for the Predictive Modeling of Solids and Nanomaterials
• Properties of carbon up to 10 million kelvin from Kohn-Sham density functional theory molecular dynamics
• A Kinetic Model for Electron-Ion Transport in Warm Dense Matter
• Mixed Stochastic-Deterministic Time-Dependent Density Functional Theory: Application to Stopping Power of Warm Dense Carbon
• First-principles derivation and properties of density-functional average-atom models
• Combining stochastic density functional theory with deep potential molecular dynamics to study warm dense matter
• Bypassing the energy functional in density functional theory: Direct calculation of electronic energies from conditional probability densities
• Stochastic and Mixed Density Functional Theory within the projector augmented wave formalism for the simulation of warm dense matter
• Plane-Wave-Based Stochastic-Deterministic Density Functional Theory for Extended Systems
• A Time-Dependent Random State Approach for Large-scale Density Functional Calculations
• Real-space density kernel method for Kohn-Sham density functional theory calculations at high temperature
• Effect of Ionic Disorder on the Principal Shock Hugoniot
• Nonlocal free-energy density functional for warm dense matter
• Group Conductivity and Nonadiabatic Born Effective Charges of Disordered Metals, Warm Dense Matter, and Hot Dense Plasma
• eminus -- Pythonic electronic structure theory