Stimulated Raman Spectroscopy with Entangled Light: Enhanced Resolution and Pathway Selection

[Image: see text] We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photoexcitation by an actinic pump, the measurement uses a pair of broad-band entangled photons; one (signal) interacts with the molecule and together with a third narrow-band pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon coincidence counting detection allows one to separately measure the Raman gain and loss signals, which is not possible with conventional probe transmission detection. Entangled photons further provide a unique temporal and spectral detection window that can better resolve fast excited-state dynamics compared to classical and correlated disentangled states of light.