4.7 Article

Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 159, Issue 9, Pages -

Publisher

AIP Publishing
DOI: 10.1063/5.0166188

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We have developed an accurate and numerically efficient method for simulating the non-linear spectroscopy of exciton-polariton systems. By investigating the influence of light-matter coupling strength and cavity loss rate on the optical response, we have confirmed the polaron decoupling effect and demonstrated the prolongation of polariton coherence time.
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.

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