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Single-molecule phosphorescence and intersystem crossing in a coupled exciton-plasmon system

2025/02/14 by Abhishek Grewal, Grewal, Abhishek, Hiroshi Imada +15 · 1 voice · 2 citations
Biochemistry, Genetics and Molecular Biology · Engineering · Physics and Astronomy · #Advanced Fluorescence Microscopy Techniques #Molecular Junctions and Nanostructures #Photonic and Optical Devices #cond-mat.mes-hall

paper · pdf · doi:10.48550/arxiv.2502.10150

arxiv published 2025/02/14 · arxiv updated 2025/06/13

Abstract

Scanning the sharp metal tip of a scanning tunneling microscope (STM) over a molecule allows tuning the coupling between the tip plasmon and a molecular fluorescence emitter. This allows access to local variations of fluorescence field enhancement and wavelength shifts, which are central parameters for characterizing the plasmon-exciton coupling. Performing the same for phosphorescence with molecular scale resolution remains a significant challenge. In this study, we present the investigation of phosphorescence from isolated Pt-Phthalocyanine molecules by analyzing tip-enhanced emission spectra in both current-induced and laser-induced phosphorescence. The latter directly monitors singlet-to-triplet state intersystem crossing of a molecule below the tip. The study contributes to a detailed understanding of triplet excitation pathways and their potential control at sub-molecular length scales. Additionally, the coupling of organic phosphors to plasmonic structures is a promising route for improving light-emitting diodes.

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