Related papers: Automatic Generation of Accurate and Cost-efficien…
Density fitting (DF), also known as the resolution of the identity (RI), is a widely used technique in quantum chemical calculations with various types of atomic basis sets - Gaussian-type orbitals, Slater-type orbitals, as well as…
In this study, we present a general workflow that enables the automatic generation of auxiliary density basis sets for all elements of the periodic table (from H to Og) to facilitate the general applicability of relativistic Dirac-Kohn-Sham…
We present model-assisted density fitting (MADF) basis set generator, an algorithm for generating primitive atomic Gaussian density fitting (DF) basis sets (DFBSs) from a contracted Gaussian orbital basis set (OBS). The MADF algorithm…
Molecule-optimized basis sets, based on approximate natural orbitals, are developed for accelerating the convergence of quantum calculations with strongly correlated (multi-referenced) electrons. We use a low-cost approximate solution of…
Explicitly correlated calculations, aside from the orbital basis set, typically require three auxiliary basis sets: JK (Coulomb-exchange fitting), RI-MP2 (resolution of the identity MP2), and CABS (complementary auxiliary basis set). If…
Large atomic-orbital (AO) basis sets of at least triple and preferably quadruple-zeta (QZ) size are required to adequately converge Kohn-Sham density functional theory (DFT) calculations towards the complete basis set limit. However,…
Efficient implementations of electronic structure methods are essential for first-principles modeling of molecules and solids. We here present a particularly efficient common framework for methods beyond semilocal density-functional theory,…
Sequence generation and prediction form a cornerstone of modern machine learning, with applications spanning natural language processing, program synthesis, and time-series forecasting. These tasks are typically modeled in an autoregressive…
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…
We present a new adaptive method for electronic structure calculations based on novel fast algorithms for reduction of multivariate mixtures. In our calculations, spatial orbitals are maintained as Gaussian mixtures whose terms are selected…
In high magnetic field calculations, anisotropic Gaussian type orbital (AGTO) basis functions are capable of reconciling the competing demands of the spherically symmetric Coulombic interaction and cylindrical magnetic ($B$ field)…
We propose a unique scheme to construct fully optimized atomic basis sets for density-functional calculations. The shapes of the radial functions are optimized by minimizing the {\it spillage} of the wave functions between the atomic…
Electronic structure calculations, such as in the Hartree-Fock or Kohn-Sham density functional approach, require an initial guess for the molecular orbitals. The quality of the initial guess has a significant impact on the speed of…
Accurate absolute binding free energy (ABFE) calculations can reduce the time and cost of identifying drug candidates from a diverse pool of molecules that may have been overlooked experimentally. These calculations typically employ…
We introduce a method for solving a self consistent electronic calculation within localized atomic orbitals, that allows us to converge to the complete basis set (CBS) limit in a stable, controlled, and systematic way. We compare our…
With the widespread use of self-consistent field methods, including Hartree-Fock and Density Functional Theory, the implications of accelerating these methods are immense. To this end, we develop a tensor hypercontraction construction with…
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…
Differentiable programming has facilitated numerous methodological advances in scientific computing. Physics engines supporting automatic differentiation have simpler code, accelerating the development process and reducing the maintenance…
We explore the impact of optimizations of the single-particle basis on the convergence behavior and robustness of ab initio no-core shell model calculations. Our focus is on novel basis sets defined by the natural orbitals of a correlated…
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…