title: Quantum Monte Carlo with variable spins.
abstract: We investigate the inclusion of variable spins in electronic structure quantum Monte Carlo, with a focus on diffusion Monte Carlo with Hamiltonians that include spin-orbit interactions. Following our previous introduction of fixed-phase spin-orbit diffusion Monte Carlo, we thoroughly discuss the details of the method and elaborate upon its technicalities. We present a proof for an upper-bound property for complex nonlocal operators, which allows for the implementation of T-moves to ensure the variational property. We discuss the time step biases associated with our particular choice of spin representation. Applications of the method are also presented for atomic and molecular systems. We calculate the binding energies and geometry of the PbH and Sn2 molecules, as well as the electron affinities of the 6p row elements in close agreement with experiments.
authors.affiliation: Department of Physics, North Carolina State University, Raleigh, North Carolina 27695-8202, USA.
authors.forename: Cody A
authors.initials: CA
authors.lastname: Melton
authors.affiliation: Department of Physics, North Carolina State University, Raleigh, North Carolina 27695-8202, USA.
authors.forename: M Chandler
authors.initials: MC
authors.lastname: Bennett
authors.affiliation: Department of Physics, North Carolina State University, Raleigh, North Carolina 27695-8202, USA.
authors.forename: Lubos
authors.initials: L
authors.lastname: Mitas