Entangled Photons Enabled Time- and Frequency-Resolved Coherent Raman Spectroscopy in Condensed Phase Molecules

We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics which often shows a rapid decay within $sim$50fs. The heterodyne-detected Raman signal is further developed to capture the phases of electronic coherence and emission in real-time domain.