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Multiple Rabi Splittings under Ultra-Strong Vibrational Coupling
Authors:
Jino George,
Thibault Chervy,
Atef Shalabney,
Eloïse Devaux,
Hidefumi Hiura,
Cyriaque Genet,
Thomas W. Ebbesen
Abstract:
From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultra-strongly coupled to multiple IR cavity modes, with Rabi splittings reaching $24\%$ of the vibration frequencies. As a proof of the ultra-strong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the anti-r…
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From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultra-strongly coupled to multiple IR cavity modes, with Rabi splittings reaching $24\%$ of the vibration frequencies. As a proof of the ultra-strong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the anti-resonant terms in the interaction energy and from the dipolar self-energy of the molecular vibrations themselves. In particular, we measure the opening of a genuine vibrational polaritonic bandgap of ca. $60$ meV. We also demonstrate that the multimode splitting effect defines a whole vibrational ladder of heavy polaritonic states perfectly resolved. These findings reveal the broad possibilities in the vibrational ultra-strong coupling regime which impact both the optical and the molecular properties of such coupled systems, in particular in the context of mode-selective chemistry.
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Submitted 6 September, 2016;
originally announced September 2016.
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Coherent Coupling of WS_2 Monolayers with Metallic Photonic Nanostructures at Room Temperature
Authors:
S. Wang,
S. Li,
T. Chervy,
A. Shalabney,
S. Azzini,
E. Orgiu,
J. A. Hutchison,
C. Genet,
P. Samori,
T. W. Ebbesen
Abstract:
Room temperature strong coupling of WS_2 monolayer exciton transitions to metallic Fabry-Perot and plasmonic optical cavities is demonstrated. A Rabi splitting of 101 meV is observed for the Fabry-Perot cavity, more than double those reported to date in other 2D materials. The enhanced magnitude and visibility of WS_2 monolayer strong coupling is attributed to the larger absorption coefficient, th…
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Room temperature strong coupling of WS_2 monolayer exciton transitions to metallic Fabry-Perot and plasmonic optical cavities is demonstrated. A Rabi splitting of 101 meV is observed for the Fabry-Perot cavity, more than double those reported to date in other 2D materials. The enhanced magnitude and visibility of WS_2 monolayer strong coupling is attributed to the larger absorption coefficient, the narrower linewidth of the A exciton transition, and greater spin-orbit coupling. For WS_2 coupled to plasmonic arrays, the Rabi splitting still reaches 60 meV despite the less favorable coupling conditions, and displays interesting photoluminescence features. The unambiguous signature of WS_2 monolayer strong coupling in easily fabricated metallic resonators at room temperature suggests many possibilities for combining light-matter hybridization with spin and valleytronics.
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Submitted 22 April, 2016;
originally announced April 2016.
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Coherent coupling of molecular resonators with a micro-cavity mode
Authors:
Atef Shalabney,
Jino George,
James A. Hutchison,
Guido Pupillo,
Cyriaque Genet,
Thomas W. Ebbesen
Abstract:
The optical hybridization of the electronic states in strongly coupled molecule-cavity systems have revealed unique properties such as lasing, room temperature polariton condensation, and the modification of excited electronic landscapes involved in molecular isomerization. Here we show that molecular vibrational modes of the electronic ground state can also be coherently coupled with a micro-cavi…
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The optical hybridization of the electronic states in strongly coupled molecule-cavity systems have revealed unique properties such as lasing, room temperature polariton condensation, and the modification of excited electronic landscapes involved in molecular isomerization. Here we show that molecular vibrational modes of the electronic ground state can also be coherently coupled with a micro-cavity mode at room temperature, given the low vibrational thermal occupation factors associated with molecular vibrations, and the collective coupling of a large ensemble of molecules immersed within the cavity mode volume. This enables the enhancement of the collective Rabi-exchange rate with respect to the single oscillator coupling strength. The possibility of inducing large shifts in the vibrational frequency of selected molecular bonds should have immediate consequences for chemistry.
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Submitted 3 February, 2015; v1 submitted 5 March, 2014;
originally announced March 2014.