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Relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons (Conference Presentation)
Author(s): Blake S. Simpkins; Kenan P. Fears; Walter J. Dressick; Adam D. Dunkelberger; Bryan T. Spann; Jeffrey C. Owrutsky
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Paper Abstract

Coherent coupling between an optical transition and confined optical mode have been investigated for electronic-state transitions, however, only very recently have vibrational transitions been considered. Here, we demonstrate both static and dynamic results for vibrational bands strongly coupled to optical cavities. We experimentally and numerically describe strong coupling between a Fabry-Pérot cavity and carbonyl stretch (~1730 cm 1) in poly-methylmethacrylate and provide evidence that the mixed-states are immune to inhomogeneous broadening. We investigate strong and weak coupling regimes through examination of cavities loaded with varying concentrations of a urethane monomer. Rabi splittings are in excellent agreement with an analytical description using no fitting parameters. Ultrafast pump-probe measurements reveal transient absorption signals over a frequency range well-separated from the vibrational band, as well as drastically modified relaxation rates. We speculate these modified kinetics are a consequence of the energy proximity between the vibration-cavity polariton modes and excited state transitions and that polaritons offer an alternative relaxation path for vibrational excitations. Varying the polariton energies by angle-tuning yields transient results consistent with this hypothesis. Furthermore, Rabi oscillations, or quantum beats, are observed at early times and we see evidence that these coherent vibration-cavity polariton excitations impact excited state population through cavity losses. Together, these results indicate that cavity coupling may be used to influence both excitation and relaxation rates of vibrations. Opening the field of polaritonic coupling to vibrational species promises to be a rich arena amenable to a wide variety of infrared-active bonds that can be studied in steady state and dynamically.

Paper Details

Date Published: 9 November 2016
PDF: 1 pages
Proc. SPIE 9918, Metamaterials, Metadevices, and Metasystems 2016, 991811 (9 November 2016); doi: 10.1117/12.2237043
Show Author Affiliations
Blake S. Simpkins, U.S. Naval Research Lab. (United States)
Kenan P. Fears, U.S. Naval Research Lab. (United States)
Walter J. Dressick, U.S. Naval Research Lab. (United States)
Adam D. Dunkelberger, U.S. Naval Research Lab. (United States)
Bryan T. Spann, National Institute of Standards and Technology (United States)
Jeffrey C. Owrutsky, U.S. Naval Research Lab. (United States)


Published in SPIE Proceedings Vol. 9918:
Metamaterials, Metadevices, and Metasystems 2016
Nader Engheta; Mikhail A. Noginov; Nikolay I. Zheludev, Editor(s)

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Relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons (Conference Presentation)



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