Related papers: Accurate Frozen Core Approximation for All-Electro…
Highly accurate experimental structure factors of silicon are available in the literature, and these provide the ideal test for any \emph{ab initio} method for the construction of the all-electron charge density. In a recent paper [J. R.…
Using the Wentzel-Kramers-Brillouin method, we derive a modified form of the Thomas-Fermi approximation to electron density. This new result enables us to calculate the details of the self-consistent ion cores, as well as the ionization…
The basic idea of Frozen-Density Embedding Theory (FDET) is the constrained minimisation of the Hohenberg-Kohn density functional $E^{HK}[\rho]$ performed using the auxiliary functional $E_{v_{AB}}^{FDET}[\Psi_A,\rho_B]$, where $\Psi_A$ is…
Understanding the applicability and limitations of electronic-structure methods needs careful and efficient comparison with accurate reference data. Knowledge of the quality and errors of electronic-structure calculations is crucial to…
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…
We present an implementation of all-electron density-functional theory for massively parallel GPGPU-based platforms, using localized atom-centered basis functions and real-space integration grids. Special attention is paid to domain…
We have developed a reduced-cost non-Dyson third-order algebraic diagrammatic construction theory for the electron-attachment problem based on state-specific frozen natural orbitals. Density fitting and truncated natural auxiliary functions…
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…
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,…
A general procedure for the optimization of atomic density-fitting basis functions is designed with the balance between accuracy and numerical stability in mind. Given one-electron wavefunctions and energies, weights are assigned to the…
All-electron calculations play an important role in density functional theory, in which improving computational efficiency is one of the most needed and challenging tasks. In the model formulations, both nonlinear eigenvalue problem and…
Quantum computers have the potential to advance material design and drug discovery by performing costly electronic structure calculations. A critical aspect of this application requires optimizing the limited resources of the quantum…
The pair-coupled-cluster doubles (pCCD) method has emerged as a viable approach for quantum-chemical studies of strongly correlated systems. Despite its lower formal scaling (O(N$^4$)) compared to other versions of coupled cluster (CC)…
Hybrid density functional approximations (DFAs) offer compelling accuracy for ab initio electronic-structure simulations of molecules, nanosystems, and bulk materials, addressing some deficiencies of computationally cheaper, frequently used…
Quantum computing has shown great potential in various quantum chemical applications such as drug discovery, material design, and catalyst optimization. Although significant progress has been made in quantum simulation of simple molecules,…
In density functional theory, charge density is the core attribute of atomic systems from which all chemical properties can be derived. Machine learning methods are promising in significantly accelerating charge density prediction, yet…
A proper theoretical description of electronic structure of the 3d orbitals in the metal centers of functional metalorganics is a challenging problem. In this letter, we apply density functional theory and an exact diagonalization method in…
The Frozen Density Embedding scheme represents an embedding method in which environmental effects onto a given subsystem are included by representing the other subsystems making up the surroundings quantum mechanically, by means of their…
The electron density of a molecule or material has recently received major attention as a target quantity of machine-learning models. A natural choice to construct a model that yields transferable and linear-scaling predictions is to…
We present a real-space formulation for coarse-graining Kohn-Sham Density Functional Theory that significantly speeds up the analysis of material defects without appreciable loss of accuracy. The approximation scheme consists of two steps.…