Nonadiabatic quantum dynamics without potential energy surfaces

  title={Nonadiabatic quantum dynamics without potential energy surfaces},
  author={Guillermo Albareda and Aaron Kelly and {\'A}ngel Rubio},
  journal={Physical Review Materials},
We present an efficient \textit{ab initio} algorithm for quantum dynamics simulations of interacting systems that is based on the conditional decomposition of the many-body wavefunction [Phys. Rev. Lett. 113, 083003 (2014)]. Starting with this formally exact approach, we develop a stochastic wavefunction ansatz using a set of interacting conditional wavefunctions as a basis. We show that this technique achieves quantitative accuracy for a photo-excited proton-coupled electron transfer problem… 

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  • W. Miller
  • Physics
    The journal of physical chemistry. A
  • 2009
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It was recently shown [G. Albareda, et al., Phys. Rev. Lett. 113, 083003 (2014)] that within the conditional decomposition approach to the coupled electron-nuclear dynamics, the electron-nuclear wave

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The molecular Schrödinger equation is rewritten in terms of nonunitary equations of motion for the nuclei that depend parametrically on the configuration of an ensemble of generally defined electronic trajectories to circumvent the calculation of the computationally demanding Born-Oppenheimer potential-energy surfaces and nonadiabatic coupling elements.