Herrera Felipe, Owrutsky Jeffrey
Department of Physics, Universidad de Santiago de Chile, Av. Ecuador 3493, Santiago, Chile and Millennium Institute for Research in Optics MIRO, Concepción, Chile.
U.S. Naval Research Laboratory, Washington, DC 20375, USA.
J Chem Phys. 2020 Mar 14;152(10):100902. doi: 10.1063/1.5136320.
This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared cavities. Using a microscopic quantum electrodynamics formulation, we discuss the competition between the collective cooperative dipolar response of a molecular ensemble and local dynamical processes that molecules typically undergo, including chemical reactions. We highlight some of the observable consequences of this competition between local and collective effects in linear transmission spectroscopy, including the formal equivalence between quantum mechanical theory and the classical transfer matrix method, under specific conditions of molecular density and indistinguishability. We also overview recent experimental and theoretical developments on strong and ultrastrong coupling with electronic and vibrational transitions, with a special focus on cavity-modified chemistry and infrared spectroscopy under vibrational strong coupling. We finally suggest several opportunities for further studies that may lead to novel applications in chemical and electromagnetic sensing, energy conversion, optoelectronics, quantum control, and quantum technology.
这是一篇关于分子极化激元领域的教程式介绍。我们描述了嵌入紫外 - 可见光或红外腔中的分子系综中强光 - 物质耦合的基本物理原理及其后果。使用微观量子电动力学公式，我们讨论了分子系综的集体合作偶极响应与分子通常经历的局部动力学过程（包括化学反应）之间的竞争。我们强调了这种局部和集体效应之间竞争在线性透射光谱中的一些可观察到的后果，包括在分子密度和不可区分性的特定条件下量子力学理论与经典转移矩阵方法之间的形式等效性。我们还概述了与电子和振动跃迁的强耦合和超强耦合的近期实验和理论进展，特别关注振动强耦合下的腔修饰化学和红外光谱。我们最后提出了几个进一步研究的机会，这些研究可能会在化学和电磁传感、能量转换、光电子学、量子控制和量子技术中带来新的应用。
