Plane-Wave-Based Stochastic-Deterministic Density Functional Theory for Extended Systems
arXiv:2204.05662 · doi:10.1103/PhysRevB.106.125132
Abstract
Traditional finite-temperature Kohn-Sham density functional theory (KSDFT) has an unfavorable scaling with respect to the electron number or at high temperatures. The evaluation of the ground-state density in KSDFT can be replaced by the Chebyshev trace (CT) method. In addition, the use of stochastic orbitals within the CT method leads to the stochastic density functional theory [Phys. Rev. Lett. 111, 106402 (2013)] (SDFT) and its improved theory, mixed stochastic-deterministic density functional theory [Phys. Rev. Lett. 125, 055002 (2020)] (MDFT). We have implemented the above four methods within the first-principles package ABACUS. All of the four methods are based on the plane-wave basis set with the use of norm-conserving pseudopotentials and the periodic boundary conditions with the use of -point sampling in the Brillouin zone. By using the KSDFT calculation results as benchmarks, we systematically evaluate the accuracy and efficiency of the CT, SDFT, and MDFT methods via examining a series of physical properties, which include the electron density, the free energy, the atomic forces, stress, and density of states for a few condensed phase systems. The results suggest that our implementations of CT, SDFT, and MDFT not only reproduce the KSDFT results with a high accuracy, but also exhibit several advantages over the tradition KSDFT method. We expect these methods can be of great help in studying high-temperature and large-size extended systems such as warm dense matter and dense plasma.
References in corpus (26)
- Selfconsistent order-N density-functional calculations for very large systems
- Nearsightedness of Electronic Matter
- Local Spin-density Approximation Exchange-correlation Free-energy Functional
- Breaking the theoretical scaling limit for predicting quasi-particle energies: The stochastic GW approach
- The importance of finite-temperature exchange-correlation for warm dense matter calculations
- Systematically improvable optimized atomic basis sets for {\it ab inito} calculations
- Self-averaging stochastic Kohn-Sham density functional theory
- First-Principles Equation of State Database for Warm Dense Matter Computation
- 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
- Swift beyond electrons using fractured stochastic orbitals
- Fast and accurate quantum molecular dynamics of dense plasmas across temperature regimes
- Fast and Universal Kohn Sham Density Functional Theory Algorithm for Warm Dense Matter to Hot Dense Plasma
- First-principles Equation of State and Shock Compression Predictions of Warm Dense Hydrocarbons
- Stochastic Optimally-Tuned Ranged-Separated Hybrid Density Functional Theory
- Towards accurate orbital-free simulations: a generalized gradient approximation for the non-interacting free energy density functional
- Stochastic density functional theory
- Thermophysical properties for shock compressed polystyrene
- Requirements for very high temperature Kohn-Sham density functional simulations and how to bypass them
- Overlapped Embedded Fragment Stochastic Density Functional Theory for Covalently Bonded Materials
- Link between K-absorption edges and thermodynamic properties of warm-dense plasmas established by improved first-principles method
- Equilibrium configurations of large nanostructures using the embedded saturated-fragments stochastic density functional theory
- Thermal Transport by Electrons and Ions in Warm Dense Aluminum: A Combined Density Functional Theory and Deep Potential Study
- Transition to metallization in warm dense helium-hydrogen mixtures using stochastic density functional theory within the Kubo-Greenwood formalism
- Stochastic embedding DFT: theory and application to p-nitroaniline