Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons

被引:15
|
作者
Mondal, M. Elious [1 ]
Koessler, Eric R. [1 ]
Provazza, Justin [2 ]
Vamivakas, A. Nickolas [3 ,4 ]
Cundiff, Steven T. [5 ]
Krauss, Todd D. [1 ,3 ]
Huo, Pengfei [1 ,3 ]
机构
[1] Univ Rochester, Dept Chem, Rochester, NY 14627 USA
[2] Quantum Simulat Technol Inc, Boston, MA 02135 USA
[3] Univ Rochester, Inst Opt, Hajim Sch Engn, Rochester, NY 14627 USA
[4] Univ Rochester, Dept Phys & Astron, Rochester, NY 14627 USA
[5] Univ Michigan, Dept Phys, Ann Arbor, MI 48109 USA
来源
JOURNAL OF CHEMICAL PHYSICS | 2023年 / 159卷 / 09期
关键词
PHOTOSYNTHETIC ENERGY-TRANSFER; SEMICLASSICAL DESCRIPTION; CAVITIES; EQUATION; BATH;
D O I
10.1063/5.0166188
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
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页数:16
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