Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks
Abstract
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.
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[1];
[1];
[2];
[1];
[1]
- Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1865044
- Alternate Identifier(s):
- OSTI ID: 1866208
- Grant/Contract Number:
- SC0004752; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 21; Journal Issue: 18; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; metal–organic framework; plasmonic nanoparticle array; conformal coating; surface lattice resonance; ultrafast spectroscopy; polaritons; quantum mechanics; energy; lattices; metal−organic framework, plasmonic nanoparticle array, conformal coating, surface lattice resonance, ultrafast spectroscopy
Citation Formats
Sample, Alexander D., Guan, Jun, Hu, Jingtian, Reese, Thaddeus, Cherqui, Charles R., Park, Jeong-Eun, Freire-Fernández, Francisco, Schaller, Richard D., Schatz, George C., and Odom, Teri W. Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks. United States: N. p., 2021.
Web. doi:10.1021/acs.nanolett.1c02740.
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. Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks. United States. https://doi.org/10.1021/acs.nanolett.1c02740
Sample, Alexander D., Guan, Jun, Hu, Jingtian, Reese, Thaddeus, Cherqui, Charles R., Park, Jeong-Eun, Freire-Fernández, Francisco, Schaller, Richard D., Schatz, George C., and Odom, Teri W. Tue .
"Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks". United States. https://doi.org/10.1021/acs.nanolett.1c02740. https://www.osti.gov/servlets/purl/1865044.
@article{osti_1865044,
title = {Strong Coupling Between Plasmons and Molecular Excitons in Metal–Organic Frameworks},
author = {Sample, Alexander D. and Guan, Jun and Hu, Jingtian and Reese, Thaddeus and Cherqui, Charles R. and Park, Jeong-Eun and Freire-Fernández, Francisco and Schaller, Richard D. and Schatz, George C. and Odom, Teri W.},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.1c02740},
journal = {Nano Letters},
number = 18,
volume = 21,
place = {United States},
year = {Tue Sep 07 00:00:00 EDT 2021},
month = {Tue Sep 07 00:00:00 EDT 2021}
}
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