Molecular Polaritons Generated from Strong Coupling between CdSe Nanoplatelets and a Dielectric Optical Cavity
Molecular Polaritons Generated from Strong Coupling between CdSe Nanoplatelets and a Dielectric Optical Cavity
复制标题
CdSe 纳米片与介电光腔强耦合产生的分子极化子
DOI：
10.1021/acs.jpclett.1c01104
复制
发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Krauss, Todd D.
中科院分区：
文献类型：
--
作者：
Qiu, Liangyu;Mandal, Arkajit;Morshed, Ovishek;Meidenbauer, Mahilet T.;Girten, William;Huo, Pengfei;Vamivakas, A. Nickolas;Krauss, Todd D.
我们证明了 CdSe 纳米片 (NPL) 激子极化子在分布式布拉格反射器 (DBR) 腔中的形成。分子-腔混合系统处于强耦合状态，具有 83 meV 拉比分裂，通过角度分辨反射率和光致发光测量进行表征。混合量子经典动力学模拟用于通过量子力学处理电子和光子自由度 (DOF) 以及经典核声子自由度来研究混合系统的极化子光物理。我们对角度分辨光致发光（PL）的数值模拟与实验数据非常吻合，为上下极化子分支的不对称强度分布提供了基本解释。我们的结果还提供了关于极化子态之间声子辅助非绝热跃迁重要性的机制见解，这反映在 PL 光谱的各种特征中。这项工作证明了将纳米片电子态与介电腔的光子态耦合形成混合系统的可行性，并为研究腔介导的物理和化学过程提供了新的平台。
We demonstrate the formation of CdSe nanoplatelet (NPL) exciton-polaritons in a distributed Bragg reflector (DBR) cavity. The molecule-cavity hybrid system is in the strong coupling regime with an 83 meV Rabi splitting, characterized from angle-resolved reflectance and photoluminescence measurements. Mixed quantum-classical dynamics simulations are used to investigate the polariton photophysics of the hybrid system by treating the electronic and photonic degrees of freedom (DOF) quantum mechanically and the nuclear phononic DOF classically. Our numerical simulations of the angle-resolved photoluminescence (PL) agree extremely well with the experimental data, providing a fundamental explanation of the asymmetric intensity distribution of the upper and lower polariton branches. Our results also provide mechanistic insights into the importance of phonon-assisted nonadiabatic transitions among polariton states, which are reflected in the various features of the PL spectra. This work proves the feasibility of coupling nanoplatelet electronic states with the photon states of a dielectric cavity to form a hybrid system and provides a new platform for investigating cavity-mediated physical and chemical processes.