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Abstract Quantum entanglement has emerged as a great resource for spectroscopy and its importance in two-photon spectrum and microscopy has been demonstrated. Current studies focus on the two-photon absorption, whereas the Raman spectroscopy with quantum entanglement still remains elusive, with outstanding issues of temporal and spectral resolutions. Here we study the new capabilities provided by entangled photons in coherent Raman spectroscopy. An ultrafast frequency-resolved Raman spectroscopy with entangled photons is developed for condensed-phase molecules, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions 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 even at timescale of 50fs. This suggests new paradigms of optical signals and spectroscopy, with potential to push detection below standard quantum limit.
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This content will become publicly available on January 15, 2026
Pathway Selectivity in 2D Electronic‐Vibrational Spectroscopy with Quantum Light
Abstract Pathway selectivity in quantum spectroscopy with entangled photons is a powerful spectroscopic tool. Phase‐matched signals involving classical light contain contributions from multiple material pathways, whereas quantum spectroscopy may allow the selection of individual pathways. 2D electronic‐vibrational spectroscopy (2DEVS) is a four‐wave mixing technique which employs visible and infrared entangled photons. It is showed how the three contributing pathways—ground state bleach, excited state absorption, and excited state emission—can be separated by photon‐number‐resolved coincidence measurements. Entangled photons thus reveal spectral features not visible in the classical signal, with an enhanced spectral resolution.
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- Award ID(s):
- 2246379
- PAR ID:
- 10566543
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Laser & Photonics Reviews
- Volume:
- 19
- Issue:
- 8
- ISSN:
- 1863-8880
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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