Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 106, Taiwan.
Department of Chemistry, National Taiwan University, Taipei 106, Taiwan.
J Phys Chem Lett. 2023 Mar 9;14(9):2395-2401. doi: 10.1021/acs.jpclett.3c00065. Epub 2023 Mar 1.
The Huang-Rhys (HR) factor, a dimensionless factor that characterizes electron-phonon (vibronic) coupling, has been extensively employed to investigate a variety of material properties. In the same spirit, we propose a quantity called the polaritonic HR factor to quantitatively describe the effects of (i) light-matter coupling induced by permanent dipoles and (ii) dipole self-energy. The former leads to polaritonic displacements, while the latter is associated with the electronic coupling shift named reorganization dipole self-coupling. In the framework of macroscopic quantum electrodynamics, our theory can evaluate the polaritonic HR factor, reorganization dipole self-coupling, and modified light-matter coupling strength in an arbitrary dielectric environment without free parameters, whose magnitudes are in good agreement with the previous experimental results. We believe that this study provides a useful perspective on understanding and quantifying light-matter interactions in media.
Huang-Rhys（HR）因子是一个无量纲因子，用于描述电子-声子（振子）耦合，被广泛用于研究各种材料性质。本着同样的精神，我们提出了一个称为极化子 HR 因子的量，用于定量描述以下两个方面的影响：（i）由永久偶极子引起的光物质耦合，以及（ii）偶极子自能。前者导致极化子位移，后者与电子耦合移位有关，称为重新组织偶极子自耦合。在宏观量子电动力学的框架内，我们的理论可以在没有自由参数的情况下评估任意介电环境中的极化子 HR 因子、重新组织偶极子自耦合和修正的光物质耦合强度，其大小与以前的实验结果非常吻合。我们相信，这项研究为理解和量化介质中的光物质相互作用提供了一个有用的视角。
