Alchemical perturbation density functional theory (APDFT)

Abstract

We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density functional estimates of properties of new molecules can be systematically surpassed---at negligible cost. The associated energy functional is an approximation to the integrated energy derivative, requiring only perturbed reference electron densities: No self-consistent field equations are necessary to estimate energies and electron densities. Electronic ground state properties considered include covalent bonding potentials, atomic forces, as well as dipole and quadropole moments.

References in corpus (7)

• Nonlocal van der Waals density functional: The simpler the better
• By-passing the Kohn-Sham equations with machine learning
• Fast and accurate predictions of covalent bonds in chemical space
• Exploring water adsorption on isoelectronically doped graphene using alchemical derivatives
• Dramatic changes in electronic structure revealed by fractionally charged nuclei
• The Chemical Space of B, N-substituted Polycyclic Aromatic Hydrocarbons: Combinatorial Enumeration and High-Throughput First-Principles Modeling
• Al${}_x$Ga${}_{1-x}$As crystals with direct 2 eV band gaps from computational alchemy