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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 photo excitation by an actinic pump, the measurement uses a pair of broadband entangled photons, one (signal) interacts with the molecule together with a third narrowband pulse induces the Raman process. The other (idler) photon provides a reference for the coincidence measurement. This interferometric photon-coincidence counting detection allows to separately measure 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.
Multidimensional optical signals are commonly recorded by varying the delays between time ordered pulses. These control the evolution of the density matrix and are described by ladder diagrams. We propose a new non-time-ordered protocol based on foll
Stimulated Raman spectroscopy has become a powerful tool to study the spatiodynamics of molecular bonds with high sensitivity, resolution and speed. However, sensitivity and speed of state-of-the-art stimulated Raman spectroscopy are currently limite
We have calculated the resonant and nonresonant contributions to attosecond impulsive stimulated electronic Raman scattering (SERS) in regions of autoionizing transitions. Comparison with Multiconfiguration Time-Dependent Hartree-Fock (MCTDHF) calcul
Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is generally restr
Correlated photons inspire abundance of metrology-related platforms, which benefit from quantum (anti-) correlations and outperform their classical-light counterparts. While such demonstrations mainly focus on entanglement, the role of photon exchang