Correlation Consistent Gaussian Basis Sets for H, B-Ne with Dirac-Fock AREP Pseudopotentials: Applications in Quantum Monte Carlo Calculations.

Abstract

In this paper, we introduce correlation consistent Gaussian-type orbital basis sets for the H and B-Ne atoms for use with the CASINO Dirac-Fock AREP pseudopotentials. These basis sets are tested in coupled cluster calculations on H2, B2, C2, N2, O2, and F2 as well as in quantum Monte Carlo calculations on the water monomer and dimer and the water-benzene complex, where they are found to give low variances in variational Monte Carlo calculations and to lead to reduced time step errors and improved convergence in diffusion Monte Carlo calculations compared to the use of nonoptimized basis sets. The use of basis sets with a large number of contracted s and p primitives is found to be especially important for the convergence of the energy in the diffusion Monte Carlo calculations.