Cavity-mediated superthermal phonon correlations in the ultrastrong coupling regime

Abstract: Phonons, or vibrational quanta, are behind some of the most fundamental physical phenomena in solids, including superconductivity, Raman processes, and broken-symmetry phases. It is therefore of fundamental importance to find ways to harness phonons for controlling these phenomena and developing novel quantum technologies. However, the majority of current phonon control techniques rely on the use of intense external driving fields or strong anharmonicities, which restricts their range of applications. Here, we present a scheme for controlling the intensity fluctuations in phonon emission at room temperature based on multimode ultrastrong light--matter coupling. The multimode ultrastrong coupling regime is achieved by coupling two optical phonon modes in lead halide perovskites to an array of nanoslots, which operates as a single-mode cavity. The extremely small mode volume of the nanoslots enables unprecedented coupling strengths in a cavity phonon-polariton system. In the far-detuned, low-cavity-frequency regime, we demonstrate that the nanoslot resonator mediates an effective coupling between the phonon modes, resulting in superthermal phonon bunching in thermal equilibrium, both within the same mode and between different modes. Experimental results are in good agreement with a multimode Hopfield model. Our work paves the way for the tailoring of phonons to modify charge and energy transport in perovskite materials, with potential applications in light-collecting or emitting devices.