Department of Chemical Sciences, University of Padova, via Marzolo 1, 35131 Padova, Italy.
Department of Chemistry, Norwegian University of Science and Technology, 7491 Trondheim, Norway.
Nano Lett. 2023 Jun 14;23(11):4938-4946. doi: 10.1021/acs.nanolett.3c00735. Epub 2023 May 23.
Strong coupling between molecules and quantized fields has emerged as an effective methodology to engineer molecular properties. New hybrid states are formed when molecules interact with quantized fields. Since the properties of these states can be modulated by fine-tuning the field features, an exciting and new side of chemistry can be explored. In particular, significant modifications of the molecular properties can be achieved in plasmonic nanocavities, where the field quantization volume is reduced to subnanometric volumes, thus leading to intriguing applications such as single-molecule imaging and high-resolution spectroscopy. In this work, we focus on phenomena where the simultaneous effects of multiple plasmonic modes are critical. We propose a theoretical methodology to account for many plasmonic modes simultaneously while retaining computational feasibility. Our approach is conceptually simple and allows us to accurately account for the multimode effects and rationalize the nature of the interaction between multiple plasmonic excitations and molecules.
分子与量子场的强耦合已成为工程化分子性质的有效方法。当分子与量子场相互作用时，会形成新的混合态。由于这些态的性质可以通过微调场特征来调制，因此可以探索化学的一个令人兴奋和新颖的方面。特别是，在等离子体纳米腔中可以实现分子性质的显著修饰，其中场量子化体积减小到亚纳米体积，从而导致单分子成像和高分辨率光谱学等有趣的应用。在这项工作中，我们关注的是多个等离子体模式的同时效应至关重要的现象。我们提出了一种理论方法，可以同时考虑多个等离子体模式，同时保持计算可行性。我们的方法概念简单，可以准确地考虑多模效应，并合理化多个等离子体激发与分子之间相互作用的性质。
