Exciton-polaritons perform as ideal carriers of macroscopic quantum coherence, which can be potentially manipulated through precisely shaping the driving laser field. However, the connection of the coherence properties between the pumping laser and the strongly coupled light-and-matter system is studied to a lesser extent. In this paper, we visualize the femtosecond dynamics of coherence transfer from the driving laser field to the resonantly excited exciton-polariton by an interferometric measurement. The resonant polaritons can effectively preserve the coherence of the pumping laser field in femtosecond timescales. At a high excitation strength, non-resonant polaritons appear at higher energies delayed by several picoseconds, without the phase coherence from the pump, which is understood by a coupled oscillator model. Our results offer the possibility of regulating the polariton coherence by finely shaping the external pump laser fields.
Condensation of bosons causes spectacular phenomena such as superfluidity or superconductivity. Understanding the nature of the condensed particles is crucial for active control of such quantum phases. Fascinating possibilities emerge from condensates of light–matter-coupled excitations, such as exciton–polaritons, photons hybridized with hydrogen-like bound electron–hole pairs. So far, only the photon component has been resolved, while even the mere existence of excitons in the condensed regime has been challenged. Here we trace the matter component of polariton condensates by monitoring intra-excitonic terahertz transitions. We study how a reservoir of optically dark excitons forms and feeds the degenerate state. Unlike atomic gases, the atom-like transition in excitons is dramatically renormalized on macroscopic ground state population. Our results establish fundamental differences between polariton condensation and photon lasing and open possibilities for coherent control of condensates. Exciton–polaritons are bosonic quasi-particles resulting from strong coupling of excitons and photons but so far only their photon component had been resolved. Here, Menard et al. monitor the intra-excitonic transitions and study how a reservoir of optically dark excitons forms and feeds the degenerate state.
Self-hybridized exciton polaritons in layered semiconductors emerge from the hybridization of excitonic resonances with confined photonic modes in films and provide a versatile platform for controlling light--matter interactions at the nanoscale. Yet, the nature of exciton--photon interactions and the collective and synchronous strong coupling of multiple excitons to the same photonic mode remain largely unexplored. Here, we use complementary momentum-resolved photoluminescence and cathodoluminescence spectroscopy to compare self-hybridized exciton polaritons in Ruddlesden--Popper perovskite flakes under optical and electron-beam excitation. We find that cathodoluminescence exhibits remarkably larger polaritonic level repulsion than photoluminescence, revealing an enhanced effective coupling strength under electron-beam excitation. We attribute this enhancement to the collective coherent excitation of multiple excitons by fast electrons, which couple to the same photonic mode and increase the interaction strength according to a gN=g1N scaling, with an effective number of up to N≈23 coherently coupled excitonic oscillators. By reducing the electron kinetic energy, we further uncover a crossover to a partially incoherent excitation regime in which higher-order Fabry--Pérot exciton-polariton resonances disappear, leaving only the lowest polariton branches while coherent transition radiation persists. This transition arises because low-energy electrons excite excitons over extended spatial volumes, washing out the phase coherence required to sustain collective coupling and form polaritonic resonances. Our work shows that electron beams can actively modify collective light--matter coupling in layered semiconductors and establishes cathodoluminescence as a route to access excitation regimes beyond all-optical excitation schemes.