eQE 2.0: Subsystem DFT Beyond GGA Functionals

Abstract

By adopting a divide-and-conquer strategy, subsystem-DFT (sDFT) can dramatically reduce the computational cost of large-scale electronic structure calculations. The key ingredients of sDFT are the nonadditive kinetic energy and exchange-correlation functionals which dominate it's accuracy. Even though, semilocal nonadditive functionals find a broad range of applications, their accuracy is somewhat limited especially for those systems where achieving balance between exchange-correlation interactions on one side and nonadditive kinetic energy on the other is crucial. In eQE 2.0, we improve dramatically the accuracy of sDFT simulations by (1) implementing nonlocal nonadditive kinetic energy functionals based on the LMGP family of functionals; (2) adapting Quantum ESPRESSO's implementation of rVV10 and vdW-DF nonlocal exchange-correlation functionals to be employed in sDFT simulations; (3) implementing "deorbitalized" meta GGA functionals (e.g., SCAN-L). We carefully assess the performance of the newly implemented tools on the S22-5 test set. eQE 2.0 delivers excellent interaction energies compared to conventional Kohn-Sham DFT and CCSD(T). The improved performance does not come at a loss of computational efficiency. We show that eQE 2.0 with nonlocal nonadditive functionals retains the same linear scaling behavior achieved in eQE 1.0 with semilocal nonadditive functionals.

References in corpus (27)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Climbing the Density Functional Ladder: Non-Empirical Meta-Generalized Gradient Approximation Designed for Molecules and Solids
• Van der Waals Density Functional for General Geometries
• A Higher-Accuracy van der Waals Density Functional
• Quantum ESPRESSO toward the exascale
• Efficient implementation of a van der Waals density functional: Application to double-wall carbon nanotubes
• Nonlocal van der Waals density functional: The simpler the better
• Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory
• Libxc: a library of exchange and correlation functionals for density functional theory
• SCAN+rVV10: A promising van der Waals density functional
• O(N) methods in electronic structure calculations
• r2SCAN-D4: Dispersion corrected meta-generalized gradient approximation for general chemical applications
• Laplacian-level density functionals for the kinetic energy density and exchange-correlation energy
• Issues and Challenges in Orbital-free Density Functional Calculations
• A Simple Generalized Gradient Approximation for the Non-interacting Kinetic Energy Density Functional
• Deorbitalized meta-GGA Exchange-Correlation Functionals in Solids
• Deorbitalization strategies for meta-GGA exchange-correlation functionals
• Meta-GGA Performance in Solids at Almost GGA Cost
• Laplacian-level kinetic energy approximations based on the fourth-order gradient expansion: Global assessment and application to the subsystem formulation of density functional theory
• Subsystem Density-Functional Theory as an Effective Tool for Modeling Ground and Excited States, their Dynamics, and Many-Body Interactions
• ATLAS: A Real-Space Finite-Difference Implementation of Orbital-Free Density Functional Theory
• Orbital-Free DFT Correctly Models Quantum Dots When Asymptotics, Nonlocality and Nonhomogeneity Are Accounted For
• Laplacian-dependent models of the kinetic energy density: Applications in subsystem density functional theory with meta-generalized gradient approximation functionals
• Orbital-Free Density Functional Theory: Kinetic Potentials and Ab-Initio Local Pseudopotentials
• Periodic Subsystem Density-Functional Theory
• Nonlocal Subsystem Density Functional Theory

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