
1.Department of Physics, City University of Hong Kong, Kowloon, Hong Kong SAR, China
2.City University of Hong Kong, Shenzhen Research Institute, Shenzhen, Guangdong, 518057, China
3.Institute for Quantum Science and Engineering, Texas A & M University, College Station, TX, 77843, USA
4.School of Physics, Xi'an Jiaotong University, Xi'an, Shaanxi, 710049, China
5.Department of Biological and Agricultural Engineering, Texas A & M University, College Station, TX, 77843, USA
6.Baylor University, Waco, TX, 76704, USA
Zhedong Zhang (zzhan26@cityu.edu.hk)
Published:31 October 2022,
Published Online:14 September 2022,
Received:26 March 2022,
Revised:02 July 2022,
Accepted:07 August 2022
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Zhang, Z. D. et al. Entangled photons enabled time-frequency-resolved coherent Raman spectroscopy and applications to electronic coherences at femtosecond scale. Light: Science & Applications, 11, 2415-2423 (2022).
Zhang, Z. D. et al. Entangled photons enabled time-frequency-resolved coherent Raman spectroscopy and applications to electronic coherences at femtosecond scale. Light: Science & Applications, 11, 2415-2423 (2022). DOI: 10.1038/s41377-022-00953-y.
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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