Accumulated photon echoes were observed in
Nd3+-doped silicate glass by using coherent and incoherent light, and it was theoretically and experimentally verified that the time resolution is determined not by the pulse width but by the correlation time of the excitation field. Even by using a cw laser, instead of a mode-locked laser, a subpicosecond time resolution was obtained when it was operated with a broad and smooth spectrum. The broadest output spectrum, and hence the highest time resolution, was attained when the dye laser was pumped by a mode-locked
Ar+ laser, and their cavity lengths were mismatched by a few \ensuremath{\mu}m. In an experiment with a resolution time of 220 fsec, a new very fast decay was observed in the echo decay curve besides a slower decay already reported.
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 (the longitudinal relaxation time) and
T2 (the transverse relaxation time), the correlation trace, i.e., output intensity versus $\ensuremath{\tau}$, represents a decay profile determined mainly by
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 effect. However, it does not cause a significant error in the determination of
T2. Moreover, as $\frac{{T}_{2}}{{T}_{1}}\ensuremath{\rightarrow}0$, the trace becomes a single-exponential decay curve determined only by
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.
In transient spectroscopy, the time-resolution is usually limited by the pulse width or the risetime of light sources or equivalent perturbers. In the extremely short time region, however, its improvement by shortening the pulse width is not an easy way even with the recent development of femtosecond pulse technique. We propose here a new method of transient spectroscopy were the time resolution is not limited by the light duration tp but limited only by the correlation time τc of light sources, being generally much shorter than tp. A temporally incoherent light has a short τc corresponding to the reciprocal bandwidth, and appears like a single pulse of duration τc in the auto-correlation measurement. This kind of light is therefore expected to play essentially the same role as a short pulse in nonlinear spectroscopy utilizing the auto-correlation technique. We present here a basic theory and an experiment which confirm this idea.
Since the first observation of accumulated photon echoes by Hesslink and Wiersna [1], nearly transform-limited mode-locked pulse trains have been used as the excitation source, and the resolution times have been limited by the widths of the pulses. In this paper we show theoretically and experimentally that the time resolution of the accumulated photon echoes is determine not by the pulse width but by the correlation time of the excitation field [2]. This indicates that it is possible to obtain a sub-picosecond resolution in accumulated photon echoes Sven by using a cw laser (non-mode-locked), if the laser output has a sufficiently broad and smooth spectrum.
Stimulated photon echoes (three-pulse echoes) produced by broadband (incoherent) light pulses are discussed. A switching time corresponding to the reciprocal inhomogeneous width is predicted for the echo signal when the time interval between the first two time-overlapping, mutually coherent pulses is scanned across 0. The effect is demonstrated in an experiment performed with cesium vapor. A new method for fast sampling of atomic or molecular velocity distribution is proposed with potential applications to photodissociation and photofragmentation studies.
Accumulated photon echoes have been observed by use of a light-emitting diode. This is to our knowledge the first observation of photon echoes that are excited by a nonlaser light source. In the incoherent-light photon echo, the time resolution is equal to the inverse of the overall spectral width of the excitation light. Therefore we can easily get a high time resolution by using nonlaser light with a broad spectrum. Moreover the use of nonlaser light in the photon-echo experiment will extend the technique into wavelength regions where lasers are not currently available.