Elucidating Molecule–Plasmon Interactions in Nanocavities with 2 nm Spatial Resolution and at the Single‐Molecule Level. Issue 35 (2nd August 2019)

• Record Type: Journal Article
• Authors: Zhang, Fan‐Li; Yi, Jun; Peng, Wei; Radjenovic, Petar M.; Zhang, Hua; Tian, Zhong‐Qun; Li, Jian‐Feng
• Is Part Of: Angewandte Chemie international edition. Volume 58:Issue 35(2019)
• Page Start: 12133
• Page End: 12137
• Publication Date: 2019-08-02
• Subjects: fluorescence -- Raman spectroscopy -- plasmonic nanocavities -- single-molecule studies -- surface plasmon resonance; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201906517
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: The fundamental understanding of the subtle interactions between molecules and plasmons is of great significance for the development of plasmon‐enhanced spectroscopy (PES) techniques with ultrahigh sensitivity. However, this information has been elusive due to the complex mechanisms and difficulty in reliably constructing and precisely controlling interactions in well‐defined plasmonic systems. Herein, the interactions in plasmonic nanocavities of film‐coupled metallic nanocubes (NCs) are investigated. Through engineering the spacer layer, molecule–plasmon interactions were precisely controlled and resolved within 2 nm. Efficient energy exchange interactions between the NCs and the surface within the 1–2 nm range are demonstrated. Additionally, optical dressed molecular excited states with a huge Lamb shift of ≈7 meV at the single‐molecule (SM) level were observed. This work provides a basis for understanding the underlying molecule–plasmon interaction, paving the way for fully manipulating light–matter interactions at the nanoscale. Abstract : Plasmonic nanocavities confine light in a small volume and strengthen the interaction of matter with light. The single‐molecule emission of probes at set positions within a nanocavity cavity was measured to provide a better understanding of the molecule–plasmon interaction.