Thibault Chervy

Coherent Coupling of WS2 Monolayers with Metallic Photonic Nanostructures at Room Temperature.

Room temperature strong coupling of WS2 monolayer exciton transitions to metallic Fabry-Pérot and plasmonic optical cavities is demonstrated. A Rabi splitting of 101 meV is observed for the Fabry-Pérot cavity. The enhanced magnitude and visibility of WS2 monolayer strong coupling is attributed to the larger absorption coefficient, the narrower line width of the A exciton transition, and greater spin-orbit coupling. For WS2 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 WS2 monolayer strong coupling in easily fabricated metallic resonators at room temperature suggests many possibilities for combining light-matter hybridization with spin and valleytronics.

Ground-State Chemical Reactivity under Vibrational Coupling to the Vacuum Electromagnetic Field.

Abstract The ground‐state deprotection of a simple alkynylsilane is studied under vibrational strong coupling to the zero‐point fluctuations, or vacuum electromagnetic field, of a resonant IR microfluidic cavity. The reaction rate decreased by a factor of up to 5.5 when the Si−C vibrational stretching modes of the reactant were strongly coupled. The relative change in the reaction rate under strong coupling depends on the Rabi splitting energy. Product analysis by GC‐MS confirmed the kinetic results. Temperature dependence shows that the activation enthalpy and entropy change significantly, suggesting that the transition state is modified from an associative to a dissociative type. These findings show that vibrational strong coupling provides a powerful approach for modifying and controlling chemical landscapes and for understanding reaction mechanisms.

Quantum Yield of Polariton Emission from Hybrid Light-Matter States.

The efficiency of light-matter strong coupling is tuned by precisely varying the spatial position of a thin layer of cyanine dye J-aggregates in Fabry-Perot microcavities, and their photophysical properties are determined. Placing the layer at the cavity field maximum affords an interaction energy (Rabi splitting) of 503 meV, a 62% increase over that observed if the aggregates are simply spread evenly through the cavity, placing the system in the ultrastrong coupling regime. The fluorescence quantum yield of the lowest polaritonic state P- integrated over k-space is found to be ∼10(-2). The same value can be deduced from the 1.4 ps lifetime of P- measured by femtosecond transient absorption spectroscopy and the calculated radiative decay rate constant. Thus, the polariton decay is dominated by nonradiative processes, in contrast with what might be expected from the small effective mass of the polaritons. These findings provide a deeper understanding of hybrid light-molecule states and have implications for the modification of molecular and material properties by strong coupling.

Non-Radiative Energy Transfer Mediated by Hybrid Light-Matter States

We present direct evidence of enhanced non-radiative energy transfer between two J-aggregated cyanine dyes strongly coupled to the vacuum field of a cavity. Excitation spectroscopy and femtosecond pump-probe measurements show that the energy transfer is highly efficient when both the donor and acceptor form light-matter hybrid states with the vacuum field. The rate of energy transfer is increased by a factor of seven under those conditions as compared to the normal situation outside the cavity, with a corresponding effect on the energy transfer efficiency. The delocalized hybrid states connect the donor and acceptor molecules and clearly play the role of a bridge to enhance the rate of energy transfer. This finding has fundamental implications for coherent energy transport and light-energy harvesting.

Energy Transfer between Spatially Separated Entangled Molecules

Abstract Light–matter strong coupling allows for the possibility of entangling the wave functions of different molecules through the light field. We hereby present direct evidence of non‐radiative energy transfer well beyond the Förster limit for spatially separated donor and acceptor cyanine dyes strongly coupled to a cavity. The transient dynamics and the static spectra show an energy transfer efficiency approaching 37 % for donor–acceptor distances ≥100 nm. In such systems, the energy transfer process becomes independent of distance as long as the coupling strength is maintained. This is consistent with the entangled and delocalized nature of the polaritonic states.

Quantum Strong Coupling with Protein Vibrational Modes

In quantum electrodynamics, matter can be hybridized to confined optical fields by a process known as light-matter strong coupling. This gives rise to new hybrid light-matter states and energy levels in the coupled material, leading to modified physical and chemical properties. Here, we report for the first time the strong coupling of vibrational modes of proteins with the vacuum field of a Fabry-Perot mid-infrared cavity. For two model systems, poly(l-glutamic acid) and bovine serum albumin, strong coupling is confirmed by the anticrossing in the dispersion curve, the square root dependence on the concentration, and a vacuum Rabi splitting that is larger than the cavity and vibration line widths. These results demonstrate that strong coupling can be applied to the study of proteins with many possible applications including the elucidation of the role of vibrational dynamics in enzyme catalysis and in H/D exchange experiments.

Tracking surface plasmon pulses using ultrafast leakage imaging

We introduce a new method for performing ultrafast imaging and tracking of surface plasmon wave packets that propagate on metal films. We demonstrate the efficiency of leakage radiation microscopy implemented in the time domain for measuring both group and phase velocities of near-field pulses with a high level of precision. The versatility of our far-field imaging method is particularly appealing in the context of ultrafast near-field optics.