Related papers: Configurational forces in electronic structure cal…
It is shown here that Kohn-Sham equations cannot be derived from Hohenberg-Kohn theory without an additional postulate. Assuming that a functional derivative with respect to total electron density exists leads in general to a theory…
Here we present a density matrix based KS inversion method formulated entirely within a Gaussian basis representation to optimize a KS potential matrix that reproduces a target electron density. Inverse Kohn-Sham (KS) density functional…
The ground state energy of a system of electrons and nuclei is proven to be a variational functional of the conditional electronic density $n_R(\mathbf{r})$, the nuclear wavefunction $\chi(R)$ and an induced vector potential $A_{\mu}(R)$…
We introduce a spectral density functional theory which can be used to compute energetics and spectra of real strongly--correlated materials using methods, algorithms and computer programs of the electronic structure theory of solids. The…
Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…
This study presents a fractional-order continuum mechanics approach that allows combining selected characteristics of nonlocal elasticity, typical of classical integral and gradient formulations, under a single frame-invariant framework.…
By partitioning the electron density into subsystem contributions, the Frozen Density Embedding (FDE) formulation of subsystem DFT has recently emerged as a powerful tool for reducing the computational scaling of Kohn--Sham DFT. To date,…
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…
Non-adiabatic effects arising from electron-phonon interactions are often neglected within the Born-Oppenheimer (BO) approximation, which assumes that electronic states adjust instantaneously to nuclear motion. The exact factorization (EF)…
Multiresolution analysis of electronic structure affords the opportunity to capture the full physics of atomic cores in a systematically improvable manner. Applying new techniques, we demonstrate for the first time that multiresolution…
Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…
We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…
In transitions between different environmental settings, a molecular system inevitably undergoes a range of detectable changes, and the ability to accurately simulate such responses, e.g., in the form of shifts to molecular energies,…
Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…
Variational excited-state density functional theory (DFT) enables the calculation of excited states at a cost comparable to ground-state calculations, but single-configuration approaches often suffer from spin contamination. We implement…
We present recent developments of the NTChem program for performing large scale hybrid Density Functional Theory calculations on the supercomputer Fugaku. We combine these developments with our recently proposed Complexity Reduction…
In this work we give a comprehensive derivation of an exact and numerically feasible method to perform ab-initio calculations of quantum particles interacting with a quantized electromagnetic field. We present a hierachy of…
Density fitting is used throughout quantum chemistry to simplify the electron-electron interaction energy (EE). A fundamental property of quantum chemistry, and DFT in particular, is that a variational principle connects the EE to a…
This article reviews the current status of lattice-dynamical calculations in crystals, using density-functional perturbation theory, with emphasis on the plane-wave pseudo-potential method. Several specialized topics are treated, including…
In exact density functional theory (DFT) the total ground-state energy is a series of linear segments between integer electron points, a condition known as "piecewise linearity". Deviation from this condition is indicative of poor…