2021/06/21 by Zhedong Zhang, Tao Peng, Zhang, Zhedong +7
Biochemistry, Genetics and Molecular Biology · Neuroscience · Physics and Astronomy · #FOS: Physical sciences #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Photoreceptor and optogenetics research #Quantum Physics (quant-ph) #Spectroscopy Techniques in Biomedical and Chemical Research #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2106.10988
openalex publication_date 2021/06/21 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are 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 which often shows a rapid decay within ∼50fs. The heterodyne-detected Raman signal is further developed to capture the phases of electronic coherence and emission in real-time domain.