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Physical Review Letters

Ultrafast Modulation Spectroscopy

D. DeBeer, L. G. Van Wagenen, Raymond John Beach, Sven R. Hartmann

Published Mar 17, 1986• 60 citations
Publisher

Abstract

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 $D$ doublet by use of 7-nsec pulses of light spectrally peaked at each of the $D$-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.

DOI
10.1103/physrevlett.56.1128

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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.
Two transient time-delayed four-wave mixing experiments have been performed on the Na D doublet and modulations of 1.9 ps and 980 as have been observed. These periods correspond to the difference and sum frequencies of the two Na D lines. Both experiments were performed using 7-ns pulses of light with frequency components at each of the D-line transitions. The effects of superimposition-state modulations are observed in the integrated TDFWM signal as a function of the time delay. As the time delay is varied, the lowest diffraction order mixing signal is modulated. Higher diffraction order mixing signals contain modulation components at integral multiples of the beat frequency.
Time-delayed four-wave mixing (TDFWM) on the 3S-3P transition in Na vapor has been studied using intense 7-nsec pulses from a broadband laser. Large-scale 1.9-psec modulation associated with the fine structure of the 3P state is observed throughout. At low buffer-gas pressures and low Na-vapor temperatures, pulse-induced relaxation effects are observed while at higher Na-vapor temperatures an anomalous response develops. In the normal region the TDFWM signal is interpreted in terms of either accumulated free decays or photon echoes. We estimate the relaxation induced by the excitation pulses.
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.
Transient, time-delayed, four-wave mixing (TDFWM) experiments have been performed on the Na D doublet with use of a novel angled-beam geometry. The effects of petahertz superposition-state modulations have been observed in the integrated TDFWM signal as a function of the time delay. As the time delay is varied, the lowest-order mixing signal modulates with a period of 980 as---corresponding to the sum frequency of the two Na D lines. Higher-diffraction-order mixing signals contain modulation components at integral multiples of the doublet sum frequency.