Mondal M Elious, Koessler Eric R, Provazza Justin, Vamivakas A Nickolas, Cundiff Steven T, Krauss Todd D, Huo Pengfei
Department of Chemistry, University of Rochester, Rochester, New York 14627, USA.
Quantum Simulation Technologies, Inc., Boston, Massachusetts 02135, USA.
J Chem Phys. 2023 Sep 7;159(9). doi: 10.1063/5.0166188.
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.
我们开发了一种精确且数值高效的非绝热路径积分方法,用于模拟激子 - 极化激元系统的非线性光谱。该方法基于部分线性化密度矩阵方法,通过声子浴环境的显式传播来模拟激子动力学,并结合随机林德布拉德动力学方法来模拟腔损耗动力学。通过模拟线性和极化激元二维电子光谱,我们系统地研究了光 - 物质耦合强度和腔损耗率如何影响光学响应信号。我们的结果证实了极化子解耦效应,即由于强光 - 物质相互作用,极化激元态之间的激子 - 声子耦合减弱。我们进一步证明了与腔外的电子相干相比,极化激元的相干时间可以显著延长。