Electronic structure by quantum Monte Carlo: atoms, molecules and solids

Abstract

An overview of the development, implementation and application of quantum Monte Carlo (QMC) to electronic structure calculations of real systems such as atoms, molecules and solids is presented. The relation of QMC to traditional approaches is discussed and the basic notions of variational and diffusion Monte Carlo methods are introduced. The QMC applications are illustrated on calculations of excited states of transition metal atoms, energy ordering of Si and C clusters, and cohesive energies and excitations in insulating solids. Comparisons with other methods indicate the QMC advantages in accuracy, scaling in the number of electrons and scalability on parallel architectures. The variety of treated systems demonstrates the usefulness and wide applicability of this approach. The presented results show that QMC is providing a new alternative and is becoming a powerful tool for ab initio electronic structure calculations.