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Picosecond dephasing studies in atomic vapors and observation of a 139-fs beat

J. E. Golub, THOMAS W. MOSSBERG

Published Jun 9, 1986• 0 citations
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Abstract

Several groups1–4 have recently proposed a simple and powerful optical technique for obtaining ultrahigh time resolution, which is limited only by the coherence time of the excitation light rather than by the overall pulse duration. The present work reports an application of this technique to study the dephasing rates of the Na and Rb resonance lines perturbed by several atmospheres of argon gas. By comparison with traditional measurements, we demonstrate that relaxation processes occurring on time scales much shorter than the excitation pulse duration can indeed be accurately and unambiguously measured using the present technique.

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Several groups1–4 have recently proposed a simple and powerful optical technique for obtaining ultrahigh time resolution, which is limited only by the coherence time of the excitation light rather than by the overall pulse duration. The present work reports an application of this technique to study the dephasing rates of the Na and Rb resonance lines perturbed by several atmospheres of argon gas. By comparison with traditional measurements, we demonstrate that relaxation processes occurring on time scales much shorter than the excitation pulse duration can indeed be accurately and unambiguously measured using the present technique.
We have employed dye-laser pulses of 10-nsec duration and 1.5–10-nm bandwidth in a transient four-wave-mixing experiment to study high-perturber-pressure collisional dephasing in dilute atomic sodium vapor. Working at argon perturber pressures of several atmospheres, we are able clearly to resolve dephasing times over a thousand times shorter than our excitation pulse duration. Measured dephasing rates are in excellent agreement with those measured by more traditional methods. When both of the sodium D lines are excited, our signal displays quantum-beat-like oscillations at the 0.52-THz frequency difference between these two states. We provide a simple picture explaining the origin of these beats.
Over the past few years, dramatic advances in short pulse technology have pushed studies of dynamical processes to ever shorter time scales. Unfortunately, short pulse technology remains beyond the means of many investigators. A simple and clever alternative approach to achieving high temporal resolution was recently proposed by several groups1−4. In this approach, time resolution is limited only by the coherence time of the excitation light, rather than by its duration. Since laser light of short coherence time (i.e. large bandwidth) is much more easily generated than the corresponding short pulse, this result is of great importance.
A technique for producing phase-related picosecond optical pulses is described. A sequence of two phase-related pulses, well separated in time, is applied to the D1 line in Na vapor. When the phase between the two pulses is scanned, oscillations in the incoherent fluorescence are observed. This demonstrates the well-defined phase relationship between the pulses. Measuring the amplitude of the oscillations as a function of pulse separation yields the Na optical coherence decay. A beat arising from the ground-state hyperfine splitting is observed, and the results agree well with calculation.
A new method of picosecond and femtosecond transient spectroscopy yielding information about ultrafast relaxation processes without requiring ultrashort light pulses is presented. It is based on the present theoretical analysis of the resonant degenerate four-wave-mixing process excited by two temporally incoherent light beams with wave vectors ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{1}$ and ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{2}$ which are originated from a single beam at frequency $\ensuremath{\omega}$ but have mutual time delay $\ensuremath{\tau}$. Under the assumption that the incoherent light field has Gaussian random complex amplitude and that the resonant material consists of the usual two-level atoms, the statistically averaged intensity of the output light field with ${\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{3}=2{\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{2}\ensuremath{-}{\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}}_{1}$ at $\ensuremath{\omega}$ is calculated as a function of $\ensuremath{\tau}$. Even with the light having a much longer duration than both T1{T}_{1}T1​ (the longitudinal relaxation time) and T2{T}_{2}T2​ (the transverse relaxation time), the correlation trace, i.e., output intensity versus $\ensuremath{\tau}$, represents a decay profile determined mainly by T2{T}_{2}T2​ for both homogeneously and inhomogeneously broadened transitions, as long as the light correlation time ${\ensuremath{\tau}}_{c}$ is much shorter than the relaxation times. The correlation trace does not always represent a single-exponential decay but is sometimes slightly deformed by the T1{T}_{1}T1​ effect. However, it does not cause a significant error in the determination of T2{T}_{2}T2​. Moreover, as $\frac{{T}_{2}}{{T}_{1}}\ensuremath{\rightarrow}0$, the trace becomes a single-exponential decay curve determined only by T2{T}_{2}T2​. The feature of the results obtained by the present method is similar to that obtained by the conventional coherent transient spectroscopy with short pulses, such as the photon echo. The time resolution in the present method, however, is limited only by ${\ensuremath{\tau}}_{c}$ much shorter than the light duration. By regarding the incoherent light as a series of random ultrashort pulses, the present four-wave-mixing process is also interpreted as the ensemble of numerous transient four-wave-mixing processes caused by various combinations of these pulses.
The conventional method to measure atomic interference is usually based on incoherent processes which can be scaled by nano or microseconds. However, atomic interference may be studied in association with coherent process such as superfluorescence. Producing superfluorescent picosecond pulses in 87Rb vapor pumped by ~100 fs laser pulses, we report an observation of quantum beat due to D-lines. The relative delay of the superfluorescent pulses is measured by the streak camera with picosecond time resolution, as a function of time interval between input pulses, which also enables us to study atomic interference.