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Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/5.0166188· OSTI ID:2422069

We develop an accurate and numerically efficient non-adiabatic path-integral approach to simulate the non-linear spectroscopy of exciton–polariton systems. This approach is based on the partial linearized density matrix approach to model the exciton dynamics with explicit propagation of the phonon bath environment, combined with a stochastic Lindblad dynamics approach to model the cavity loss dynamics. Through simulating both linear and polariton two-dimensional electronic spectra, we systematically investigate how light–matter coupling strength and cavity loss rate influence the optical response signal. Our results confirm the polaron decoupling effect, which is the reduced exciton–phonon coupling among polariton states due to the strong light–matter interactions. We further demonstrate that the polariton coherence time can be significantly prolonged compared to the electronic coherence outside the cavity.

Research Organization:
Univ. of Rochester, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
SC0022171
OSTI ID:
2422069
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 159; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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