Abstract
Time-resolved Raman spectroscopy techniques offer various ways to study the dynamics of molecular vibrations in liquids or gases and optical phonons in crystals. While these techniques give access to the coherence time of the vibrational modes, they are not able to reveal the fragile quantum correlations that are spontaneously created between light and vibration during the Raman interaction. Here, we present a scheme leveraging universal properties of spontaneous Raman scattering to demonstrate Bell correlations between light and a collective molecular vibration. We measure the decay of these hybrid photon-phonon Bell correlations with sub-picosecond time resolution and find that they survive over several hundred oscillations at ambient conditions. Our method offers a universal approach to generate entanglement between light and molecular vibrations. Moreover, our results pave the way for the study of quantum correlations in more complex solid-state and molecular systems in their natural state.