Related papers: Correlation-consistent Gaussian basis sets for sol…

Diffuse atomic orbital basis sets have proven to be essential to obtain accurate interaction energies, especially in regard to non-covalent interactions. However, they also have a detrimental impact on the sparsity of the one-particle…

We develop an innovative numerical technique to describe few-body systems. Correlated Gaussian basis functions are used to expand the channel functions in the hyperspherical representation. The method is proven to be robust and efficient…

Gausslets are one of the few basis constructions for electronic structure that combine locality, orthonormality, variable resolution, and an accurate diagonal approximation for the electron-electron interaction, but the original…

Basis sets are a crucial but often largely overlooked choice when setting up quantum chemistry calculations. The choice of basis set can be critical in determining the accuracy and calculation time of your quantum chemistry calculations.…

Multicomponent methods are a conceptually simple way to include nuclear quantum effects into quantum chemistry calculations. In multicomponent methods, the electronic molecular orbitals are described using the linear combination of atomic…

We reexamine the recently introduced basis-set correction theory based on density-functional theory consisting in correcting the basis-set incompleteness error of wave-function methods using a density functional. We use a one-dimensional…

Calculations of the hyperpolarizability are typically much more difficult to converge with basis set size than the linear polarizability. In order to understand these convergence issues and hence obtain accurate ab initio values, we compare…

We introduce a family of all-electron Gaussian basis sets, augmented MOLOPT, optimized for excited-state calculations on large molecules. We generate these basis sets by augmenting existing STO-3G, STO-6G, and MOLOPT basis sets optimized…

Basis set convergence of the Hartree-Fock and the correlation energy is examined for the hydrogen bonded infinite bent chains (HF)_infinity and (HCl)_infinity. We employ series of correlation consistent basis sets up to quintuple zeta…

We propose a streamlined combination scheme of the transcorrelation (TC) and coupled cluster (CC) theory, which not only increases the convergence rate with respect to the basis set, but also extends the applicability of the lowest order CC…

A challenge in modeling time-dependent strong-field processes such as high-harmonic generation for many-body systems, is how to effectively represent the electronic continuum. We apply Rothe's method to the time-dependent Hartree-Fock…

How can we train a statistical mixture model on a massive data set? In this work we show how to construct coresets for mixtures of Gaussians. A coreset is a weighted subset of the data, which guarantees that models fitting the coreset also…

We describe a method for imposing the correct electron-nucleus (e-n) cusp in molecular orbitals expanded as a linear combination of (cuspless) Gaussian basis functions. Enforcing the e-n cusp in trial wave functions is an important asset in…

Atomic Compton profiles (CPs) are a very important property which provide us information about the momentum distribution of atomic electrons. Therefore, for CPs of heavy atoms, relativistic effects are expected to be important, warranting a…

Within the Correlated Gaussian Method the parameters of the Gaussian basis functions are often chosen stochastically using pseudo-random sequences. We show that alternative low-discrepancy sequences, also known as quasi-random sequences,…

The use of Gaussian processes (GPs) is supported by efficient sampling algorithms, a rich methodological literature, and strong theoretical grounding. However, due to their prohibitive computation and storage demands, the use of exact GPs…

In past decades the scientific community has been looking for a reliable first-principles method to predict the electronic structure of solids with high accuracy. Here we present an approach which we call the quasiparticle self-consistent…

The quantum simulation of real molecules and materials is one of the most highly anticipated applications of quantum computing. Algorithms for simulating electronic structure using a first-quantized plane wave representation are especially…

While pseudospectral (PS) methods can feature very high accuracy, they tend to be severely limited in terms of geometric flexibility. Application of global radial basis functions overcomes this, however at the expense of problematic…

We propose a general method for constructing system-dependent basis functions for correlated quantum chemical calculations. Our construction combines features from several traditional approaches: plane waves, localized basis functions, and…