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Article Dans Une Revue Journal of Chemical Physics Année : 2022

Stochastic Multi Configuration Time-Dependent Hartree for Dissipative Quantum Dynamics with Strong Intramolecular Coupling

Résumé

In this article, we explore the dissipation dynamics of a strongly coupled multidimensional system in contact with a Markovian bath following a system-bath approach. We use in this endeavour the recently developed stochastic Multi-Configuration Time-Dependent Hartree approach within the Monte Carlo wave packet formalism [J. Chem. Phys. 156, 094109 (2022)]. The method proved to yield thermalized ensembles of wave packets when intramolecular coupling is weak. To treat strongly coupled systems, new Lindblad dissipative operators are constructed as linear combinations of the system coordinates and associated momenta. These are obtained by an unitary transformation to a normal mode representation, which reduces intermode coupling up to second order. Additionally, we use combinations of generalized raising/lowering operators to enforce the Boltzmann distribution in the dissipation operators, which yield perfect thermalization in the harmonic limit. The two ansatz are tested using a model two-dimensional hamiltonian parameterized to disentangle the effects of intramolecular potential coupling, of strong mode mixing observed in Fermi resonances, and of anharmonicity.
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Dates et versions

hal-03774088 , version 1 (09-09-2022)

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Souvik Mandal, Fabien Gatti, Oussama Bindech, Roberto Marquardt, Jean Christophe Tremblay. Stochastic Multi Configuration Time-Dependent Hartree for Dissipative Quantum Dynamics with Strong Intramolecular Coupling. Journal of Chemical Physics, 2022, 157 (14), pp.144105. ⟨10.1063/5.0105308⟩. ⟨hal-03774088⟩
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