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

Sample, Alexander D.; Guan, Jun; Hu, Jingtian; Reese, Thaddeus; Cherqui, Charles R.; Park, Jeong-Eun; Freire-Fernández, Francisco; Schaller, Richard D.; Schatz, George C.; Odom, Teri W.

doi:10.1021/acs.nanolett.1c02740

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

Journal Article · Tue Sep 07 00:00:00 EDT 2021 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.1c02740· OSTI ID:1865044

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Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

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. Furthermore, this hybrid system demonstrates how MOFs can function as an accessible excitonic material for polariton chemistry.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0004752; AC02-06CH11357

OSTI ID:: 1865044

Alternate ID(s):: OSTI ID: 1866208

Journal Information:: Nano Letters, Vol. 21, Issue 18; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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

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