Related papers: Large-scale relativistic complete active space sel…

Despite the great success Kohn-Sham density functional theory (KS-DFT) has achieved, the delocalization error remains a major challenge for commonly used density functional approximations (DFAs), resulting in systematic errors in ionization…

Recent advances in selected CI, including the adaptive sampling configuration interaction (ASCI) algorithm and its heat bath extension, have made the ASCI approach competitive with the most accurate techniques available, and hence an…

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient…

We introduce a mixed density fitting scheme that uses both a Gaussian and a plane-wave fitting basis to accurately evaluate electron repulsion integrals in crystalline systems. We use this scheme to enable efficient all-electron Gaussian…

The multi-configurational self-consistent field theory is considered the standard starting point for almost all multireference approaches required for strongly-correlated molecular problems. The limitation of the approach is generally given…

Repeated computations on the same molecular system, but with different geometries, are often performed in quantum chemistry, for instance, in ab-initio molecular dynamics simulations or geometry optimizations. While many efficient…

A self-consistent calculation scheme for correlated electron systems is created based on the density-functional theory (DFT). Our scheme is a multi-reference DFT (MR-DFT) calculation in which the electron charge density is reproduced by an…

We formulate a set of equations that facilitate an exact numerical solution of the Kohn-Sham potential for a finite Hubbard chain with nearest neighbour hopping and arbitrary site potentials. The approach relies on a mapping of the…

We have performed self-consistent calculations for first and second row atoms using a variant of density-functional theory, the optimized effective potential method, with an approximation due to Krieger, Li and Iafrate and a…

We present an iterative method to reconstruct the linear-theory initial conditions from the late-time cosmological matter density field, with the intent of improving the recovery of the cosmic distance scale from the baryon acoustic…

In a Hilbert space setting, for convex optimization, we analyze the convergence rate of a class of first-order algorithms involving inertial features. They can be interpreted as discrete time versions of inertial dynamics involving both…

Density functional theory (DFT) and beyond-DFT methods are often used in combination with photoelectron spectroscopy to obtain physical insights into the electronic structure of molecules and solids. The Kohn-Sham eigenvalues are not…

We propose a new self-consistent field (SCF) algorithm based on an iterative, partially stochastic \textit{``Divide \& Conquer''}-type approach. This new SCF algorithm is a simple variant of the usual SCF procedure and can be easily…

Recently several methods were proposed for sparse optimization which make careful use of second-order information [10, 28, 16, 3] to improve local convergence rates. These methods construct a composite quadratic approximation using Hessian…

Ab initio calculations are fundamentally bottlenecked for large systems by the steep computational scaling of solving self-consistent field (SCF) equations. While machine learning offers potential accelerations, existing methods often…

We present a fully variational locally scaled self-interaction corrected (SIC) energy functional using complex optimal orbitals. This represents an important milestone for fully variational SIC energy functionals, which have been shown to…

We here adapt an extended version of the adaptive cubic regularisation method with dynamic inexact Hessian information for nonconvex optimisation in [3] to the stochastic optimisation setting. While exact function evaluations are still…

We investigate fully self-consistent multiscale quantum-classical algorithms on current generation superconducting quantum computers, in a unified approach to tackle the correlated electronic structure of large systems in both quantum…

Separating the Coulomb potential into short-range and long-range components enables the use of different electron repulsion integral algorithms for each component. The short-range part can be efficiently computed using the analytical…

In this paper we propose a unified two-phase scheme for convex optimization to accelerate: (1) the adaptive cubic regularization methods with exact/inexact Hessian matrices, and (2) the adaptive gradient method, without any knowledge of the…