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分子极化激元学的理论视角

A Theoretical Perspective on Molecular Polaritonics.

作者信息

Sánchez-Barquilla Mónica, Fernández-Domínguez Antonio I, Feist Johannes, García-Vidal Francisco J

机构信息

Departamento de Física Teórica de la Materia Condensada and Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, E-28049 Madrid, Spain.

Institute of High Performance Computing, Agency for Science, Technology, and Research (ASTAR), Connexis, Singapore, 138632 Singapore.

出版信息

ACS Photonics. 2022 Jun 15;9(6):1830-1841. doi: 10.1021/acsphotonics.2c00048. Epub 2022 Jun 3.

Abstract

In the past decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction of polaritonic phenomena emerging in this light-matter interaction regime have proven to be difficult tasks. The challenge originates from the enormous number of degrees of freedom that need to be taken into account, both in the organic molecules and in their photonic environment. On one hand, the accurate treatment of the vibrational spectrum of the former is key, and simplified quantum models are not valid in many cases. On the other hand, most photonic setups have complex geometric and material characteristics, with the result that photon fields corresponding to more than just a single electromagnetic mode contribute to the light-matter interaction in these platforms. Moreover, loss and dissipation, in the form of absorption or radiation, must also be included in the theoretical description of polaritons. Here, we review and offer our own perspective on some of the work recently done in the modeling of interacting molecular and optical states with increasing complexity.

摘要

在过去十年中,许多理论研究都集中在研究有机分子(或一般而言的量子发射器)与光模式之间的强耦合。事实证明,描述和预测在这种光与物质相互作用机制中出现的极化激元现象是一项艰巨的任务。这一挑战源于在有机分子及其光子环境中都需要考虑的大量自由度。一方面,准确处理前者的振动光谱是关键,在许多情况下简化的量子模型并不适用。另一方面,大多数光子装置具有复杂的几何和材料特性,结果是在这些平台中,对应于不止一个单一电磁模式的光子场会对光与物质的相互作用产生影响。此外,以吸收或辐射形式存在的损耗和耗散也必须纳入极化激元的理论描述中。在此,我们回顾并就最近在对日益复杂的相互作用分子和光学态进行建模方面所做的一些工作给出我们自己的观点。

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