Extracting Kinetic Information from Short-Time Trajectories: Relaxation and Disorder of Lossy Cavity Polaritons
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, we have demonstrated significant potential in the use of the TTM towards 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.
- Manipulating matter by strong coupling to vacuum fields. Science, 373:6551, 2021.
- Wei Xiong. Molecular vibrational polariton dynamics: What can polaritons do? Acc. Chem. Res., 56(7):776–786, 2023.
- From a quantum-electrodynamical light-matter description to novel spectroscopies. Nat. Rev. Chem., 2:0118, 2018.
- Relevance of the quadratic diamagnetic and self-polarization terms in cavity quantum electrodynamics. ACS Photonics, 7:975, 2020.
- F. Herrera and F. C. Spano. Theory of nanoscale organic cavities: The essential role of vibration-photon dressed states. ACS Photonics, 5:65–79, 2018.
- Polariton chemistry: Controlling molecular dynamics with optical cavities. Chem. Sci., 9:6325, 2018.
- Swinging between shine and shadow: Theoretical advances on thermally-activated vibropolaritonic chemistry (a perspective). J. Chem. Phys., 158:230901, 2023.
- Tensor network simulation of non-Markovian dynamics in organic polaritons. Phys. Rev. Lett., 121:227401, 2018.
- G. Groenhof and J. J. Toppari. Coherent light harvesting through strong coupling to confined light. J. Phys. Chem. Lett., 9:4848–4851, 2018.
- Tracking polariton relaxation with multiscale molecular dynamics simulations. J. Phys. Chem. Lett., 10:5476–5483, 2019.
- B. Cui and A. Nitzan. Collective response in light-matter interactions: The interplay between strong coupling and local dynamics. J. Chem. Phys., 129:173001, 2022.
- Quantum simulations of vibrational strong coupling via path integrals. J. Phys. Chem. Lett., 13(17):3890–3825, 2022.
- Quantum effects in chemical reactions under polaritonic vibrational strong coupling. J. Phys. Chem. Lett., 12:9531–9538, 2021.
- Suppression and enhancement of thermal chemical rates in a cavity. JPCL, 13(20):4441–4446, 2022.
- Theory of vibrational polariton chemistry in the collective coupling regime. J. of Chem. Phys., 156:014101, 2022.
- J. Cao. Generalized resonance energy transfer theory: Applications to vibrational energy flow in optical cavities. J. Phys. Chem. Lett., 13:10943–10951, 2022.
- Non-markovian dynamical maps: Numerical processing of open quantum trajectories. Physical Review Letters, 112(11), Mar 2014.
- Prescription for experimental determination of the dynamics of a quantum black box. Journal of Modern Optics, 44(11-12):2455–2467, 1997.
- Tomographically reconstructed master equations for any open quantum dynamics. Quantum, 2:76, July 2018.
- Efficient simulation of non-Markovian system-environment interaction. New Journal of Physics, 18(2):023035, 2016.
- Effective-mode representation of non-Markovian dynamics: A hierarchical approximation of the spectral density. i. Application to single surface dynamics. The Journal of Chemical Physics, 131(2):024109, 2009.
- Zero-temperature localization in a sub-ohmic spin-boson model investigated by an extended hierarchy equation of motion. Physical Review B, 95(21):214308, 2017.
- A unified stochastic formulation of dissipative quantum dynamics. I. Generalized hierarchical equations. J. Chem. Phys. 148(1), 014103/1-14, 2018.
- Open Quantum System Dynamics from Infinite Tensor Network Contraction. arXiv preprint, arXiv:2307.01802, 2023.
- Sublinear scaling in non-Markovian open quantum systems simulations. arXiv preprint, arXiv:2304.05291, 2023.
- Nancy Makri Small Matrix Path Integral with Extended Memory. J. Chem. Theory Comput., 17(1):1–6, 2021.
- Nancy Makri Small Matrix Path Integral for Driven Dissipative Dynamics. J. Phys. Chem. A, 125(48):10500–10506, 2021.
- Introduction to the Dicke model: From equilibrium to nonequilibrium, and vice versa. Advanced Quantum Technologies, 2(1-2):1800043, 2019.
- Quantum chaos triggered by precursors of a quantum phase transition: The Dicke model. Physical Review Letters, 90(4), jan 2003.
- R. H. Dicke. Coherence in spontaneous radiation processes. Phys. Rev., 93:99–110, Jan 1954.
- Exact solution for an n𝑛nitalic_n-molecule—radiation-field hamiltonian. Phys. Rev., 170:379–384, Jun 1968.
- E. A. Power and S. Zienau. Coulomb gauge in non-relativistic quantum electro-dynamics and the shape of spectral lines. Phil. Trans. R. Soc. Lond. A, 251:427, 1959.
- Initial system-environment correlations via the transfer-tensor method. Physical Review A, 96(6):062122, 2017.
- Sadao Nakajima. On Quantum Theory of Transport Phenomena: Steady Diffusion. Progress of Theoretical Physics, 20(6):948–959, 12 1958.
- Robert Zwanzig. Ensemble method in the theory of irreversibility. The Journal of Chemical Physics, 33(5):1338–1341, 1960.
- Accurate long-time mixed quantum-classical Liouville dynamics via the transfer tensor method. J. Phys. Chem. Lett., 7:4809–4814, 2016.
- Applicability of transfer tensor method for open quantum system dynamics. The Journal of Chemical Physics, 147(23):234108, 2017.
- Qutip: An open-source python framework for the dynamics of open quantum systems. Computer Physics Communications, 183(8):1760–1772, 2012.
- Spectral analysis of electron transfer kinetics. I. Symmetric reactions. The Journal of Chemical Physics, 112(10), 4716-4722, 2000.
- Electronic coherence in mixed-valence systems: Spectral analysis. The Journal of Physical Chemistry A, 103(47):9460–9468, 1999.
- G. Engelhardt and J. Cao. Unusual dynamical properties of disordered polaritons in microcavities. Phys. Rev. B, 105:064205/1–19, 2022.
- Polarition localization and spectroscopic properties of disordered quantum emitters in spatially-extended microcavities. Phys. Rev. Lett., pages 213602/1–7, 2023.
- Correlative dark-field and photoluminescence spectroscopy of individual plasmon-molecule hybrid nanostructures in a strong coupling regime. ACS Photonics, 6(10):2570–2576, 2019.
- Cavity Born-Oppenheimer Hartree-Fock ansatz: Light-matter properties of strongly coupled molecular ensembles. J. Phys. Chem. Lett., 14(36):8024-8033, 2023.
- Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling. arXiv preprint, arXiv:2306.06004, 2023.
- Understanding polaritonic chemistry from ab initio quantum electrodynamics. Chem. Rev., 123(19):11191-11229, 2023.
- Polariton mediated electron transfer via cavity quantum electrodynamics. J. Phys. Chem. B, 124:6321, 2020.
- J. Cao and E. Pollak. Cavity-induced quantum interference and collective interactions in Van der Waals systems. arXiv:2310.12881, 2023.
Paper Prompts
Sign up for free to create and run prompts on this paper using GPT-5.
Top Community Prompts
Collections
Sign up for free to add this paper to one or more collections.