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Acta Physica Sinica

STUDY OF THE PHOTON ECHO IN UMSCTS

P An, An M

Published Jan 1, 1998• 0 citations
OpenAlex

Abstract

AbstractWe have studied the photon echo in ultrafast modulation spectroscopy in a cascade three level system (UMSCTS).When the pump beams have broadband linewidth,the one photon and two photon four wave mixings are related to the three pulse stimulated photon echo and sum frenquency three level echo when τ0,respectively;while the result should coincide with the case that the beams have narrow linewidth when τ0.

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AbstractWe have studied the photon echo in ultrafast modulation spectroscopy in a cascade three level system (UMSCTS).When the pump beams have broadband linewidth,the one photon and two photon four wave mixings are related to the three pulse stimulated photon echo and sum frenquency three level echo when τ0,respectively;while the result should coincide with the case that the beams have narrow linewidth when τ0.
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.
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.
The three-pulse stimulated photon echo has been considered as one of the most fundamental transient four wave mixing processes1, where each of the three excitation pulses induces a single elementary interaction process between a laser field and an inhomogeneously broadened two-level system., resulting in a burst of the fourth wave, i.e., echo. Now if four or more optical pulses are applied to a medium, a number of photon echoes should be expected, in general. At low excitation intensities where the perturbation theory is applicable, however, the dominant nonlinear process is still the three-pulse stimulated echo and consequently each echo signal is generated only by three of the preceding pulses. It is rather a remarkable result that the echo intensity is unaffected by the presence of all the rest of the pulses other than its three generators. With this in mind, it is theoretically and experimentally shown that by applying a single optical pulse (#1) propagating along k1 followed by N pairs of counter-propagating pulses (#2j (k2j) and #3j− (k3j = −k2j); j=1,…N) in various directions, it is possible to obtain N photon echoes along the direction -k1 opposite to the first pulse #1. We will call this degenerate photon echoes, degenerate in. the sense that the echoes are spatially overlapping and temporally simultaneous. When N=l, this scheme is reduced to the ordinary backward photon echo2,3. The doubly degenerate case (N=2) is illustrated in Fig. 1. The j-th echo will be generated by the set of pulses (#1, #2j, #3j) and appear at t = t3j + t2j − t1 where t1, i2j and t3j are the arrival times of the pulses #1, #2j and #3j, respectively.
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.