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arXiv:2601.13646

Theory for Entangled-Photons Stimulated Raman Scattering versus Nonlinear Absorption for Polyatomic Molecules

Mingran Zhang, Jiahao Joel Fan, Frank Schlawin, Zhedong Zhang

quant-phphysics.chem-phSubmitted Jan 20, 2026• Announced Jan 21, 2026• 0 citations
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Abstract

Quantum entanglement offers an incredible resource for enhancing the sensing and spectroscopic probes. Here we develop a microscopic theory for the stimulated Raman scattering (SRS) using entangled photons. We demonstrate that the time-energy correlation of the photon pairs can optimize the signal for polyatomic molecules. Our results show that the spectral-line intensity of the entangled-photon SRS (ESRS) is of the same order of magnitude as the one for the entangled two-photon absorption (ETPA); the parameter window is thus identified to do so. Moreover, the vibrational coherence is found to play an important role for enhancing the ESRS against the ETPA intensity. Our work paves a firm road for extending the schemes of molecular spectroscopy with quantum light, based on the observation of the ETPA in experiments.

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26 pages, 6 figures

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Abstract Quantum entanglement has emerged as a great resource for studying the interactions between molecules and radiation. We propose a new scheme of stimulated Raman scattering with entangled photons. A quantum ultrafast Raman spectroscopy is developed for condensed-phase molecules, to monitor the exciton populations and coherences. Analytic results are obtained, showing an entanglement-enabled time-frequency scale not attainable by classical light. The Raman signal presents an unprecedented selectivity of molecular correlation functions, as a result of the Hong-Ou-Mandel interference. Our work suggests a new paradigm of using an unconventional interferometer as part of spectroscopy, with the potential to unveil advanced information about complex materials.
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