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We introduce machine learning (ML) models that predict the electronic structure of materials across a wide temperature range. Our models employ neural networks and are trained on density functional theory (DFT) data. Unlike most other ML…
Within the method of spectral moments it is possible to construct the spectral function of a many-electron system from the first $2P$ spectral moments ($P=1,2,3,\dots$). The case $P=1$ corresponds to standard Kohn-Sham density functional…
We present an investigation into diffusion models for molecular generation, with the aim of better understanding how their predictions compare to the results of physics-based calculations. The investigation into these models is driven by…
Linear-scaling implementations of density functional theory (DFT) reach their intended efficiency regime only when applied to systems having a physical size larger than the range of their Kohn-Sham density matrix (DM). This causes a problem…
We present a novel theoretical approach to simulate spin, time and angular-resolved photoelectron spectroscopy (ARPES) from first principles that is applicable to surfaces, thin films, few layer systems, and low-dimensional nanostructures.…
We formulate the Kohn-Sham density functional theory (KS-DFT) as a statistical theory in which the electron density is deter-mined from an average of correlated stochastic densities in a trace formula. The key idea is that it is sufficient…
The ground state energy of a many-electron system can be approximated by an variational approach in which the total energy of the system is minimized with respect to one and two-body reduced density matrices (RDM) instead of many-electron…
We introduce 'single-particle-exact density functional theory' (1pEx-DFT), a novel density functional approach that represents all single-particle contributions to the energy with exact functionals. Here, we parameterize interaction energy…
Ab initio electronic structure methods give accurate results for small systems, but do not scale well to large systems. Chemical insight tells us that molecular functional groups will behave approximately the same way in all molecules,…
We present a numerical method for grand canonical density functional theory (DFT) tailored to solid-state systems, employing Gaussian-type orbitals as the primary basis. Our approach directly minimizes the grand canonical free energy using…
While methods based on density-functional perturbation theory have dramatically improved our understanding of electron-phonon contributions to transport in materials, methods for accurately capturing electron-electron scattering relevant to…
Various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations exist. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the…
We present the theory and implementation of a fully variational wave function -- density functional theory (DFT) hybrid model, which is applicable to many cases of strong correlation. We denote this model the multiconfigurational…
We present a second-order formulation of multi-reference algebraic diagrammatic construction theory [Sokolov, A. Yu. J. Chem. Phys. 2018, 149, 204113] for simulating photoelectron spectra of strongly correlated systems (MR-ADC(2)). The…
Recent advances in X-ray free-electron laser diagnostics have enabled direct probing of the electronic structure under extreme pressures and temperatures, such as those encountered in stellar interiors and inertial confinement fusion…
We demonstrate the accurate calculation of entropies and free energies for a variety of liquid metals using an extension of the two phase thermodynamic (2PT) model based on a decomposition of the velocity autocorrelation function into…
Structure factors obtained from diffraction experiments are one of the most important quantities for characterizing the electronic and structural properties of materials. Methods for calculating this quantity from plane-wave density…
We propose a systematic procedure for the approximation of density functionals in density functional theory that consists of two parts. First, for the efficient approximation of a general density functional, we introduce an efficient ansatz…
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…
Density functional theory (DFT) has transformed our ability to investigate and understand electronic ground states. In its original formulation, however, DFT is not suited to addressing (e.g.) degenerate ground states, mixed states with…