Organic charged polaritons in the ultrastrong coupling regime

Abstract

We embedded an all-hydrocarbon-based carbocation in a metallic microcavity that was tuned to resonance with an electronic transition of the carbocation. The measured Rabi splitting was 41% of the excitation energy, putting the system well into the ultrastrong coupling regime. Importantly, due to the intrinsic charge on the carbocation, the polaritons that form carry a significant charge fraction $0.55e_0$ and a large charge-to-mass ratio ($\sim 2400e_0/m_0$). Moreover, the ground state of the ultrastrongly coupled system is calculated to carry about one percent of one elementary charge, implying a potentially enhanced charge transport across the molecules. These unique properties of our system, together with its convenient preparation, provide a practical platform to study charged polaritons in the ultrastrong coupling regime.

6+4 pages, 4+3 figures

References in corpus (5)

• Beyond the Jaynes-Cummings model: circuit QED in the ultrastrong coupling regime
• Ultra-Strong Light-Matter Coupling Regime with Polariton Dots
• Charge induced coherence between intersubband plasmons in a quantum structure
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Cited by in corpus (4)

• Quantum amplification and simulation of strong and ultrastrong coupling of light and matter
• Controlling the Manifold of Polariton States Through Molecular Disorder
• The Fate of the Upper Polariton: Breakdown of the Quasiparticle Picture in the Continuum
• Release of virtual photon and phonon pairs from qubit-plasmon-phonon ultrastrong coupling system