Nonadiabatic \textit{ab initio} Quantum Dynamics without Potential Energy Surfaces

Phys. Rev. Materials 3, 023803 (2019)

Nonadiabatic \textit{ab initio} Quantum Dynamics without Potential Energy Surfaces

Guillermo Albareda, Aaron Kelly, Angel Rubio

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 and for nonequilibrium dynamics in a cavity bound electron-photon system in the ultra-strong coupling regime, using two orders of magnitude fewer trajectories than the corresponding mean field calculation. This method is highly parallelizable, and constitutes a practical and efficient alternative to available quantum-classical simulation methods for systems of interacting fermions and bosons.

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Preprint - 742.94 KB
Doi 10.1103/PhysRevMaterials.3.023803
All of the authors thank Shunsuke Sato, Heiko Appel and Tarek A. Elsayed for fruitful discussions. G.A. acknowledges financial support from the European Unions Horizon 2020 research and innovation programme under the Marie Skodowska-Curie grant agreement No 752822, the Spanish Ministerio de Economa y Competitividad (CTQ2016-76423-P), and the Generalitat de Catalunya (2017 SGR 348). A.K. acknowledges funding from the National Sciences and Engineering Research Council of Canada Discovery grant program. A.R. acknowledges financial support from the European Research Council (ERC-2015-AdG-694097), and Grupos Consolidados (IT578-13).

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