Scheme for adding electron-nucleus cusps to Gaussian orbitals

Abstract

A simple scheme is described for introducing the correct cusps at nuclei into orbitals obtained from Gaussian basis set electronic structure calculations. The scheme is tested with all-electron variational quantum Monte Carlo (VMC) and diffusion quantum Monte Carlo (DMC) methods for the Ne atom, the H2 molecule, and 55 molecules from a standard benchmark set. It greatly reduces the variance of the local energy in all cases and slightly improves the variational energy. This scheme yields a general improvement in the efficiency of all-electron VMC and DMC calculations using Gaussian basis sets.

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• Jastrow correlation factor for atoms, molecules, and solids
• Norm-conserving Hartree-Fock pseudopotentials and their asymptotic behavior
• An efficient localized basis set for quantum Monte Carlo calculations on condensed matter
• Monte Carlo energy and variance minimization techniques for optimizing many-body wave functions

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