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

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

doi:10.1021/acs.jpclett.5c03719

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

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

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

1 Citation (Scopus)

Abstract

Quantum entanglement offers an incredible resource for quantum-enhanced sensing, imaging, and spectroscopy. Here we evaluate the enhancement of stimulated Raman scattering (SRS) signal by 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.

© 2026 American Chemical Society

Original language	English
Pages (from-to)	4100–4108
Number of pages	9
Journal	Journal of Physical Chemistry Letters
Volume	17
Issue number	14
Online published	6 Mar 2026
DOIs	https://doi.org/10.1021/acs.jpclett.5c03719
Publication status	Published - 9 Apr 2026

Funding

Z. D. Z. and M. Z. gratefully thank the support of the Excellent Young Scientists Fund by National Science Foundation of China (No. 9240172), the General Fund by National Science Foundation of China (No. 12474364), and the National Science Foundation of China/RGC Collaborative Research Scheme (No. 9054901). F. S. acknowledges support from the Cluster of Excellence “Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG) - EXC 2056 - project ID 390715994, and the research unit “FOR5750: OPTIMAL” - project ID 531215165.

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@article{b9b757bd224247ba9b2349126e377920,

title = "Theory for Entangled-Photons Stimulated Raman Scattering versus Nonlinear Absorption for Polyatomic Molecules",

abstract = "Quantum entanglement offers an incredible resource for quantum-enhanced sensing, imaging, and spectroscopy. Here we evaluate the enhancement of stimulated Raman scattering (SRS) signal by 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. {\textcopyright} 2026 American Chemical Society",

author = "Mingran Zhang and Fan, \{Jiahao Joel\} and Frank Schlawin and Zhedong Zhang",

year = "2026",

month = apr,

day = "9",

doi = "10.1021/acs.jpclett.5c03719",

language = "English",

volume = "17",

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journal = "Journal of Physical Chemistry Letters",

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TY - JOUR

T1 - Theory for Entangled-Photons Stimulated Raman Scattering versus Nonlinear Absorption for Polyatomic Molecules

AU - Zhang, Mingran

AU - Fan, Jiahao Joel

AU - Schlawin, Frank

AU - Zhang, Zhedong

PY - 2026/4/9

Y1 - 2026/4/9

N2 - Quantum entanglement offers an incredible resource for quantum-enhanced sensing, imaging, and spectroscopy. Here we evaluate the enhancement of stimulated Raman scattering (SRS) signal by 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. © 2026 American Chemical Society

AB - Quantum entanglement offers an incredible resource for quantum-enhanced sensing, imaging, and spectroscopy. Here we evaluate the enhancement of stimulated Raman scattering (SRS) signal by 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. © 2026 American Chemical Society

UR - https://www.webofscience.com/wos/woscc/full-record/WOS:001708757000001

U2 - 10.1021/acs.jpclett.5c03719

DO - 10.1021/acs.jpclett.5c03719

M3 - RGC 21 - Publication in refereed journal

SN - 1948-7185

VL - 17

SP - 4100

EP - 4108

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 14

ER -

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

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NSFC-CRS-ExtU-Lead: Superradiant Time-crystal Maser and Applications in Quantum Metrology

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

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NSFC-CRS-ExtU-Lead: Superradiant Time-crystal Maser and Applications in Quantum Metrology

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