Related papers: Smart local orbitals for efficient calculations wi…

Atomic orbitals underpin our understanding of electronic structure, providing intuitive descriptions of bonding, charge transfer, magnetism, and correlation effects. Despite their utility, an atomic basis that is adaptable, strictly…

We introduce surrogate functionals: machine-learned energy functionals for orbital-free density functional theory (OF-DFT) which are defined not by universal fidelity to a physical reference, but merely by the requirement that density…

Quantum mechanical methods based on the density functional theory (DFT) offer a realistic possibility of first-principles design of organic donor-acceptor systems and engineered band-gap materials. This promise is contingent upon the…

Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…

Diabatic states and the couplings between them are important for quantifying, elucidating, and predicting the rates and mechanisms of many chemical and biochemical processes. Here, we propose and investigate approaches to accurately compute…

Selecting excitations in localized orbitals to calculate long-range correlation contributions to range-separated density-functional theory can reduce the overall computational effort significantly. Beyond simple selection schemes of excited…

The importance of the Lieb-Simon proof of the relative exactness of Thomas-Fermi theory in the large-Z limit to modern density functional theory (DFT) is explored. The principle, that there is a specific semiclassical limit in which…

In contrast to the original Kohn-Sham (KS) formalism, we propose a density functional theory (DFT) with fractional orbital occupations for the study of ground states of many-electron systems, wherein strong static correlation is shown to be…

We present a simple and general method for construction of localized orbitals to describe electronic structure of extended periodic metals and insulators as well as confined systems. Spatial decay of these orbitals is found to exhibit…

Density functional theory offers accurate structure prediction at acceptable computational cost, but commonly used approximations suffer from delocalization error; this results in inaccurate predictions of quantities such as energy band…

We present a method to make highly accurate pseudopotentials for use with orbital-free density functional theory (OF-DFT) with given exchange-correlation and kinetic energy functionals, which avoids the compounding of errors of Kohn-Sham…

We use projector operators to correct the Kohn-Sham Hamiltonian of density functional theory (KS-DFT) so that the resulting mean-field scheme yields, in finite systems, virtual orbitals and energy gaps in better agreement with those…

Reconstructing a quantum system's Hamiltonian from limited yet experimentally observable information is interesting both as a practical task and from a fundamental standpoint. We pose and investigate the inverse problem of reconstructing a…

An efficient O($N$) divide-conquer (DC) method based on localized natural orbitals (LNOs) is presented for large-scale density functional theories (DFT) calculations of gapped and metallic systems. The LNOs are non-iteratively calculated by…

In a recent paper we presented a linear scaling Kohn-Sham density functional theory (DFT) code based on Daubechies wavelets, where a minimal set of localized support functions is optimized in situ and therefore adapted to the chemical…

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

We present a detailed study of the use of localized spherical-wave basis sets, first introduced in the context of linear-scaling, in first-principles density-functional calculations. Several parameters that control the completeness of this…

We present in full detail a newly developed formalism enabling density functional perturbation theory (DFPT) calculations from a DFT+$U$ ground state. The implementation includes ultrasoft pseudopotentials and is valid for both insulating…

We developed a general framework for hybrid quantum-classical computing of molecular and periodic embedding approaches based on an orbital space separation of the fragment and environment degrees of freedom. We demonstrate its potential by…

In the present work, we investigate the computational efficiency afforded by higher-order finite-element discretization of the saddle-point formulation of orbital-free density functional theory. We first investigate the robustness of viable…