Highly accurate ab-initio thermochemistry via real-space quantum Monte Carlo: Benzene

Abstract

Real-space quantum Monte Carlo is used to calculate the total atomization energy of benzene. In contrast to orbital-space methods common in quantum chemistry, real-space methods allow results at near the complete-basis-set limit to be immediately obtained, all at a computational cost that scales with the fourth power of system size. We demonstrate this utility using the moderately sized benzene molecule, obtaining energies that agree with experiment and previous results from highly accurate composite methods including HEAT and W2. Due to the low scaling of these algorithms, it opens up the possibility of addressing systems out of reach of quantum chemical methods.

References in corpus (15)

• Recent developments in the PySCF program package
• Generalized Lanczos Algorithm for Variational Quantum Monte Carlo
• Projected Hartree-Fock Theory
• Beyond the locality approximation in the standard diffusion Monte Carlo method
• Correlated geminal wave function for molecules: an efficient resonating valence bond approach
• Full optimization of Jastrow-Slater wave functions with application to the first-row atoms and homonuclear diatomic molecules
• Geminal wavefunctions with Jastrow correlation: a first application to atoms
• Size-consistent variational approaches to non-local pseudopotentials: standard and lattice regularized diffusion Monte Carlo methods revisited
• Optimizing large parameter sets in variational quantum Monte Carlo
• Diffusion Monte Carlo with lattice regularization
• Ground state properties of the one dimensional Coulomb gas
• Fully ab initio atomization energy of benzene via W2 theory
• Spin-Orbit Interactions in Electronic Structure Quantum Monte Carlo
• Symmetry projected Jastrow mean field wavefunction in variational Monte Carlo
• Speeding up the ab initio diffusion Monte Carlo by a smart lattice regularization