Nonadiabatic transition paths from quantum jump trajectories

• URL: http://arxiv.org/abs/2206.04018v2
• Date: Wed, 3 Aug 2022 23:43:02 GMT
• Title: Nonadiabatic transition paths from quantum jump trajectories
• Authors: Michelle C. Anderson, Addison J. Schile, David T. Limmer
• Abstract summary: We study rare reactive pathways in open quantum systems using Transition Path Theory and ensembles of quantum jump trajectories. We detail the dominant pathways and rates of thermally activated processes, as well as the relaxation pathways and photoyields following vertical excitation.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We present a means of studying rare reactive pathways in open quantum systems using Transition Path Theory and ensembles of quantum jump trajectories. This approach allows for elucidation of reactive paths for dissipative, nonadiabatic dynamics when the system is embedded in a Markovian environment. We detail the dominant pathways and rates of thermally activated processes, as well as the relaxation pathways and photoyields following vertical excitation in a minimal model of a conical intersection. We find that the geometry of the conical intersection affects the electronic character of the transition state, as defined through a generalization of a committor function for a thermal barrier crossing event. Similarly, the geometry changes the mechanism of relaxation following a vertical excitation. Relaxation in models resulting from small diabatic coupling proceed through pathways dominated by pure dephasing, while those with large diabatic coupling proceed through pathways limited by dissipation. The perspective introduced here for the nonadiabatic dynamics of open quantum systems generalizes classical notions of reactive paths to fundamentally quantum mechanical processes.

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