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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.
Pairs of photons entangled in their time-frequency degree of freedom are of great interest in quantum optics research and applications, due to their relative ease of generation and their high capacity for encoding information. Here we analyze, both t
Time-bin entangled photons are ideal for long-distance quantum communication via optical fibers. Here we present a source where, even at high creation rates, each excitation pulse generates at most one time-bin entangled pair. This is important for t
Long distance quantum communication is one of the prime goals in the field of quantum information science. With information encoded in the quantum state of photons, existing telecommunication fiber networks can be effectively used as a transport medi
A theory of correlations between N photons of given frequencies and detected at given time delays is presented. These correlation functions are usually too cumbersome to be computed explicitly. We show that they are obtained exactly through intensity
Time-resolved Raman spectroscopy has been applied to probe the anharmonic coupling and electron-phonon interaction of optical phonons in graphite. From the decay of the transient anti-Stokes scattering of the G-mode following ultrafast excitation, we