Multiple Rabi Splittings under Ultrastrong Vibrational Coupling.

From the high vibrational dipolar strength offered by molecular liquids, we demonstrate that a molecular vibration can be ultrastrongly coupled to multiple IR cavity modes, with Rabi splittings reaching 24% of the vibration frequencies. As a proof of the ultrastrong coupling regime, our experimental data unambiguously reveal the contributions to the polaritonic dynamics coming from the antiresonant 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 band gap 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 ultrastrong coupling regime which impact both the optical and the molecular properties of such coupled systems, in particular, in the context of mode-selective chemistry.

Enhanced Raman Scattering from Vibro-Polariton Hybrid States.

Ground-state molecular vibrations can be hybridized through strong coupling with the vacuum field of a cavity optical mode in the infrared region, leading to the formation of two new coherent vibro-polariton states. The spontaneous Raman scattering from such hybridized light-matter states was studied, showing that the collective Rabi splitting occurs at the level of a single selected bond. Moreover, the coherent nature of the vibro-polariton states boosts the Raman scattering cross-section by two to three orders of magnitude, revealing a new enhancement mechanism as a result of vibrational strong coupling. This observation has fundamental consequences for the understanding of light-molecule strong coupling and for molecular science.

Enhanced logic performance with semiconducting bilayer graphene channels.

Realization of logic circuits in graphene with an energy gap (EG) remains one of the main challenges for graphene electronics. We found that large transport EGs (>100 meV) can be fulfilled in dual-gated bilayer graphene underneath a simple alumina passivation top gate stack, which directly contacts the graphene channels without an inserted buffer layer. With the presence of EGs, the electrical properties of the graphene transistors are significantly enhanced, as manifested by enhanced on/off current ratio, subthreshold slope, and current saturation. For the first time, complementary-like semiconducting logic graphene inverters are demonstrated that show a large improvement over their metallic counterparts. This result may open the way for logic applications of gap-engineered graphene.