Ultrafast Coherence Delocalization in Real Space Simulated by Polaritons

Abstract

We investigated coherence delocalization on a coupled-cavity molecular polariton platform in time, frequency, and spatial domains, enabled by ultrafast two-dimensional infrared hyperspectral imaging. Unidirectional coherence delocalization (coherence prepared in one cavity transfer to another cavity) was observed in frequency and real spaces. This directionality was enabled by dissipation of delocalized photon from high-energy to low-energy modes, described by Lindblad dynamics. Further experiments showed that when coherences were directly prepared across cavities (superpositions between polaritons from different cavities), only energetically nearby polaritons could form coherences that survived the long-range environmental fluctuation. Together with the Lindblad dynamics, this result implied that coherences delocalized through a one-step mechanism where photons transferred from one cavity to another, shedding lights to coherence evolution in natural and artificial quantum systems. This work also demonstrated a way of combining photon and molecular modes to simulate coherence dynamics.