The Experts below are selected from a list of 4065 Experts worldwide ranked by ideXlab platform

Shiwei Zhang - One of the best experts on this subject based on the ideXlab platform.

  • communication calculation of interatomic forces and optimization of molecular geometry with auxiliary field quantum monte carlo
    Journal of Chemical Physics, 2018
    Co-Authors: Mario Motta, Shiwei Zhang
    Abstract:

    We propose an algorithm for accurate, systematic, and scalable computation of interatomic forces within the auxiliary-field quantum Monte Carlo (AFQMC) method. The algorithm relies on the Hellmann-Feynman Theorem and incorporates Pulay corrections in the presence of atomic orbital basis sets. We benchmark the method for small molecules by comparing the computed forces with the derivatives of the AFQMC potential energy surface and by direct comparison with other quantum chemistry methods. We then perform geometry optimizations using the steepest descent algorithm in larger molecules. With realistic basis sets, we obtain equilibrium geometries in agreement, within statistical error bars, with experimental values. The increase in computational cost for computing forces in this approach is only a small prefactor over that of calculating the total energy. This paves the way for a general and efficient approach for geometry optimization and molecular dynamics within AFQMC.

Francisco M Fernandez - One of the best experts on this subject based on the ideXlab platform.

Mario Motta - One of the best experts on this subject based on the ideXlab platform.

  • communication calculation of interatomic forces and optimization of molecular geometry with auxiliary field quantum monte carlo
    Journal of Chemical Physics, 2018
    Co-Authors: Mario Motta, Shiwei Zhang
    Abstract:

    We propose an algorithm for accurate, systematic, and scalable computation of interatomic forces within the auxiliary-field quantum Monte Carlo (AFQMC) method. The algorithm relies on the Hellmann-Feynman Theorem and incorporates Pulay corrections in the presence of atomic orbital basis sets. We benchmark the method for small molecules by comparing the computed forces with the derivatives of the AFQMC potential energy surface and by direct comparison with other quantum chemistry methods. We then perform geometry optimizations using the steepest descent algorithm in larger molecules. With realistic basis sets, we obtain equilibrium geometries in agreement, within statistical error bars, with experimental values. The increase in computational cost for computing forces in this approach is only a small prefactor over that of calculating the total energy. This paves the way for a general and efficient approach for geometry optimization and molecular dynamics within AFQMC.

Sokrates T Pantelides - One of the best experts on this subject based on the ideXlab platform.

  • hellmann feynman Theorem and the definition of forces in quantum time dependent and transport problems
    Physical Review B, 2000
    Co-Authors: Massimiliano Di Ventra, Sokrates T Pantelides
    Abstract:

    The conventional Hellmann-Feynman Theorem for the definition of forces on nuclei is not directly applicable to quantum time-dependent and transport problems. We present a rigorous derivation of a general Hellmann-Feynman-like Theorem that applies to all quantum mechanical systems and reduces to well-known results for ground-state problems. It provides a rigorous definition of forces in time-dependent and transport problems. Explicit forms of Pulay-like forces are derived and the conditions for them to be zero are identified. A practical scheme for ab initio calculations of current-induced forces is described and the study of the transfer of a Si atom between two electrodes is presented as an example.

Piotr Bala - One of the best experts on this subject based on the ideXlab platform.

  • extended hellmann feynman Theorem for non stationary states and its application in quantum classical molecular dynamics simulations
    Chemical Physics Letters, 1994
    Co-Authors: Piotr Bala, Bogdan Lesyng, J A Mccammon
    Abstract:

    Abstract An extended Hellmann-Feynman Theorem for non-stationary states is presented. For systems in which some particles are described quantum-mechanically and others classically, the extended Theorem allows one to determine more precisely the forces exerted by quantum particles on classical particles. The forces are used in quantum-classical molecular dynamics (QCMD) simulations, where the extended Theorem allows an increase in the integration time-step and a reduction in the energy drift. The QCMD model also accounts for a dynamical vibronic coupling between quantum and classical subsystems, which further improves the quality of the simulation results.