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Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks

Cite this: Nano Lett. 2021, 21, 18, 7775–7780
Publication Date (Web):September 7, 2021
https://doi.org/10.1021/acs.nanolett.1c02740
Copyright © 2021 American Chemical Society

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    Abstract

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    This Letter describes strong coupling of densely packed molecular emitters in metal–organic frameworks (MOFs) and plasmonic nanoparticle (NP) lattices. Porphyrin-derived ligands with small transition dipole moments in an ordered MOF film were grown on Ag NP arrays. Angle-resolved optical measurements of the MOF-NP lattice system showed the formation of a polariton that is lower in energy and does not cross the uncoupled MOF Q1 band. Modeling predicted the upper polariton energy and a calculated Rabi splitting of 110 meV. The coupling strength was systematically controlled by detuning the plasmon energy by changing the refractive index of the solvents infiltrating the MOF pores. Through transient absorption spectroscopy, we found that the lower polariton decays quickly at shorter time scales (<500 ps) and slowly at longer times because of energy transfer from the upper polariton. This hybrid system demonstrates how MOFs can function as an accessible excitonic material for polariton chemistry.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.1c02740.

    • Materials, fabrication and measurement information, X-ray diffraction data, modeling details, additional transient absorption and angle-resolved measurements, transient absorption decay fitting (PDF)

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