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Unveiling and controlling the coherent evolution of low energy states is akey to attain light driven new functionalities of materials. Here weinvestigate the coherent evolution of non-equilibrium photon-phonon Ramaninteractions in the low photon number regime via femtosecond time-resolvedmultimode heterodyne detection. The time dependence of the weak probe spectralcomponents is revealed by interferential amplification with shaped phase-lockedreference fields that allow for a frequency selective amplification. We reportmeasurements on $\alpha$-quartz that show that both amplitude and phase of theprobe spectral components are modulated at the phonon frequency, but encodequalitatively different responses which are representative respectively of thetime dependent position and momentum of the atoms. We stress that thesensitivity achieved here (1-10 photons per pulse) may be of relevance for bothquantum information technologies and time domain studies on photosensitivematerials.

Time-resolved multimode heterodyne detection for dissecting coherent states of matter