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Journal of the Optical Society of America B

Ultrafast modulation spectroscopy in cascading three-level and four-level systems

Panming Fu, Yanbang Wang, Qian Jiang, Xin Mi, Zuhe Yu

Published Mar 1, 2001• 14 citations
Publisher

Abstract

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.

DOI
10.1364/josab.18.000370

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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.
We have studied theoretically a phase-conjugate ultrafast modulation spectroscopy (PCUMS) in a Doppler-broadened system. The pump beams consist of two frequency components which drive two different transitions. It is found that the four-wave-mixing (FWM) signal exhibits damping oscillation as the relative time delay between two pump beams is varied, from which the energy-level splitting can be deduced. We have considered the cases that pump beams have either narrow band or broadband linewidth and found that for both cases a Doppler-free precision in the measurement of the energy-level splitting can be achieved. The advantage of PCUMS is that the energy-level splitting between states can be widely separated. Finally, the relationship between PCUMS and other Doppler-free techniques in frequency and time domains has also been discussed.
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.
The effect of fourth-order coherence on ultrafast modulation spectroscopy with phase-conjugation geometry (PCUMS) in a cascade three-level system is investigated using chaotic and phase-diffusion models. It has been found that the temporal behavior of the beat signal depends on the stochastic properties of the lasers and the transverse relaxation rate of the transitions, and the modulation terms of the beat signal depend on the second-order coherence function, which is determined by the laser line shape. Since different stochastic models of the laser field affect only the fourth-order coherence function, they have little influence on the general temporal modulation behavior of the beat signal. The different roles of the phase fluctuation and amplitude fluctuation can be investigated in the time domain. The cases where the pump beams have either a narrow or broad band linewidth are considered and it has been found that for both cases a Doppler-free precision in the measurement of the energy-level difference between two states can be achieved. The difference between the PCUMS and the DeBeer, UMS [D. DeBeer et al., Phys. Rev. Lett. 56, 1128 (1986)] is discussed as well from a physical viewpoint.
We study six-wave mixing (SWM) spectroscopy based on electromagnetically induced transparency in a Doppler-broadened cascade four-level system. It is found that the SWM spectra are extremely sensitive to the configuration of the incident beams, where the linewidth can be either Doppler-free or very broad, due to the polarization interference of atoms of different velocities. This polarization interference can be controlled in the presence of a strong coupling field. Moreover, SWM can be employed as a new type of Doppler-free Autler–Townes (AT) spectroscopy, which has better spectral resolution than conventional AT spectroscopy. Finally, we also reveal the intrinsic connection between frequency-domain SWM spectroscopy and time-domain photon echoes through studying the time-domain correspondence of SWM.