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Extracting Kinetic Information from Short-time Trajectories: Relaxation and Disorder of Lossy Cavity Polaritons

Overview
Journal Nanophotonics
Publisher De Gruyter
Date 2024 Dec 16
PMID 39678665
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Abstract

The emerging field of molecular cavity polaritons has stimulated a surge of experimental and theoretical activities and presents a unique opportunity to develop the many-body simulation methodology. This paper presents a numerical scheme for the extraction of key kinetic information of lossy cavity polaritons based on the transfer tensor method (TTM). Steady state, relaxation timescales, and oscillatory phenomena can all be deduced directly from a set of transfer tensors without the need for long-time simulation. Moreover, we generalize TTM to disordered systems by sampling dynamical maps and achieve fast convergence to disordered-averaged dynamics using a small set of realizations. Together, these techniques provide a toolbox for characterizing the interplay of cavity loss, disorder, and cooperativity in polariton relaxation and allow us to predict unusual dependences on the initial excitation state, photon decay rate, strength of disorder, and the type of cavity models. Thus, using the example of cavity polaritons, we have demonstrated significant potential in the use of the TTM toward both the efficient computation of long-time polariton dynamics and the extraction of crucial kinetic information about polariton relaxation from a small set of short-time trajectories.

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References
1.
Cao J . Generalized Resonance Energy Transfer Theory: Applications to Vibrational Energy Flow in Optical Cavities. J Phys Chem Lett. 2022; 13(47):10943-10951. DOI: 10.1021/acs.jpclett.2c02707. View

2.
Gelzinis A, Rybakovas E, Valkunas L . Applicability of transfer tensor method for open quantum system dynamics. J Chem Phys. 2017; 147(23):234108. DOI: 10.1063/1.5009086. View

3.
Makri N . Small Matrix Path Integral with Extended Memory. J Chem Theory Comput. 2021; 17(1):1-6. DOI: 10.1021/acs.jctc.0c00987. View

4.
Cerrillo J, Cao J . Non-Markovian dynamical maps: numerical processing of open quantum trajectories. Phys Rev Lett. 2014; 112(11):110401. DOI: 10.1103/PhysRevLett.112.110401. View

5.
Groenhof G, Toppari J . Coherent Light Harvesting through Strong Coupling to Confined Light. J Phys Chem Lett. 2018; 9(17):4848-4851. PMC: 6129961. DOI: 10.1021/acs.jpclett.8b02032. View