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Physical Review A

Ultrafast modulation spectroscopy in a cascade three-level system

Panming Fu, Xin Mi, Zuhe Yu, Qian Jiang, Yanpeng Zhang, Xiaofeng Li

Published Dec 1, 1995• 46 citations
Publisher

Abstract

Based on the polarization interference between one-photon and two-photon processes, we demonstrated an ultrafast modulation spectroscopy in a cascade three-level system (UMSCTS) in Na vapor, which showed a modulation of the four-wave mixing signal intensity with a 55-fs period, corresponding to the beating between the resonant frequencies of the transitions from 3${\mathit{S}}_{1/2}$ to 3${\mathit{P}}_{3/2}$ and from 3${\mathit{P}}_{3/2}$ to 4${\mathit{D}}_{3/2,5/2}$. We have also discussed the possibility of using UMSCTS to measure the energy levels of the excited states with Doppler-free precision.

DOI
10.1103/physreva.52.4867

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Based on the polarization interference between one-photon and two-photon processes, we demonstrated an ultrafast modulation spectroscopy in a cascade three-level system (UMSCTS) in Na vapor, which showed a modulation of the four-wave mixing signal intensity with a 55-fs period, corresponding to the beating between the resonant frequencies of the transitions from 3S1/2{\mathit{S}}_{1/2}S1/2​ to 3P3/2{\mathit{P}}_{3/2}P3/2​ and from 3P3/2{\mathit{P}}_{3/2}P3/2​ to 4D3/2,5/2{\mathit{D}}_{3/2,5/2}D3/2,5/2​. We have also discussed the possibility of using UMSCTS to measure the energy levels of the excited states with Doppler-free precision.
Based on the interference between two two-photon processes, we reported a four-level ultrafast modulation spectroscopy in Na vapor, where 3S, 3P, 5S, and 4D formed a four-level system. We studied the temporal behavior of the four-wave mixing signal intensity and obtained signal modulation with period 25 fs, corresponding to the splitting between 5S and 4D. This technique can achieve Doppler-free precision in the measurement of the energy level splitting between two excited states which are dipolar forbidden from the ground state.
We study theoretically ultrafast modulation spectroscopy in Doppler-broadened cascading three-level and four-level systems. The pump beams consist of two frequency components that drive two-pathway excitation. The four-wave mixing (FWM) signal exhibits damping oscillation as the relative time delay τ between the two pump beams is varied, from which the resonant frequencies between energy levels can be deduced. Furthermore, Doppler-free precision in the measurement of the resonant frequencies can be achieved when the pump beams have either narrow-band or broadband linewidths. We study two-photon resonant FWM induced by time-delayed correlated fluctuating fields in a Doppler-broadened cascading three-level system. It is related intrinsically to the sum-frequency trilevel echo when the pump beams have broadband linewidths. However, unlike the corresponding incoherent-light stimulated photon echo, the maximum of the FWM signal is shifted from τ≃0. If we consider the fluctuations of the pump beams, the FWM signal exhibits damping oscillation when the laser frequency is off resonant from the two-photon transition.
Photon-echo modulation spectroscopy is extended into a new regime to study coherences between states that are widely separated in frequency compared with the bandwidth of the exciting laser pulses. Time-delayed four-wave mixing (TDFWM) is observed on the Na DDD doublet by use of 7-nsec pulses of light spectrally peaked at each of the DDD-line transitions. As the two double-frequency, 7-nsec light pulses are delayed with respect to each other a 1.9-psec beating of the integrated TDFWM signal is observed, even for delays greater than the excitation pulse width.