Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates
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Author(s)
Xiao, Jun
Liu, Xiaoze
Liu, Yongmin
Zhang, Xiang
Hu, Qing
Jin, Dafei
Nam, Sang Hoon
Fang, Xuanlai
Date Issued
September 2017
Journal
Proceedings of the National Academy of Sciences
Publisher
National Academy of Sciences (U.S.)
Citation
Hu, Qing et al. “Ultrafast Fluorescent Decay Induced by Metal-Mediated Dipole–dipole Interaction in Two-Dimensional Molecular Aggregates.” Proceedings of the National Academy of Sciences 114, 38 (September 2017): 10017–10022 © 2017 National Academy of Sciences
Version
Final published version
Abstract
Two-dimensional molecular aggregate (2DMA), a thin sheet of strongly interacting dipole molecules self-assembled at close distance on an ordered lattice, is a fascinating fluorescent material. It is distinctively different from the conventional (single or colloidal) dye molecules and quantum dots. In this paper, we verify that when a 2DMA is placed at a nanometric distance from a metallic substrate, the strong and coherent interaction between the dipoles inside the 2DMA dominates its fluorescent decay at a picosecond timescale. Our streak-camera lifetime measurement and interacting lattice–dipole calculation reveal that the metal-mediated dipole–dipole interaction shortens the fluorescent lifetime to about one-half and increases the energy dissipation rate by 10 times that expected from the noninteracting single-dipole picture. Our finding can enrich our understanding of nanoscale energy transfer in molecular excitonic systems and may designate a unique direction for developing fast and efficient optoelectronic devices. Keywords: molecular aggregate; fluorescence; nonradiative decay; dipole–dipole interaction; surface plasmon
MIT Department
Massachusetts Institute of Technology. Department of Mechanical Engineering
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1073/PNAS.1703000114
