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Optics Letters

Quantum beats in forward scattering: subnanosecond studies with a mode-locked dye laser

H. Harde, J. Mlynek, Wulfhard K. Lange, H. Burggraf

Published Jun 1, 1981• 31 citations
Publisher

Abstract

Time-resolved polarization spectroscopy of transient coherent superpositions of atomic substates is extended to the picosecond time scale by using a synchronously pumped mode-locked dye laser. As a first demonstration, hyperfine beats in the sodium D(1) and D(2), lines were resolved. The ground-state splitting could be determined with an accuracy of better than 10(-3).

DOI
10.1364/ol.6.000290

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I. A new technique utilizing the electro-optic frequency switching of a single mode ( 6 Mhz) dye laser was used to observe free induction decay and optical nutation in iodine gas and optical nutation in an organic mixed crystal (pentacene in p-terphenyl) at low temperature. A new technique, incoherent resonance decay (IRO) was also developed. These experiments allow one to determine T_1 and T_2, the longitudinal and transverse relaxation times of the excited ensemble, in analogy with magnetic resonance. For I_2(g) at O∙C; T_l = 2.3 x 10^(-7) sec, T_2 ≃ 1 x 10^(-7) sec. These techniques are limited to a time scale > 10 nsec. II. The construction and characterization of cw, mode-locked dye laser capable of putting out a continuous train of reproducible sub-picosecond pulses is described. Experiments utilizing this laser for the measurement of picosecond coherent transients and time resolved absorption spectroscopy are proposed.

•Jan 1, 1978•0 citations
Time-resolved polarization spectroscopy of transient coherent superpositions of atomic substates is extended to the picosecond time scale by using a synchronously pumped mode-locked dye laser. As a first demonstration, hyperfine beats in the sodium D(1) and D(2), lines were resolved. The ground-state splitting could be determined with an accuracy of better than 10(-3).
The method of Synchronized Quantum Beat Spectroscopy has been improved by introducing the amplitude modulation on the excitation pulse train. By using an amplitude-modulated train of picosecond pulses from a cw mode-locked dye laser, we obtain resonance enhancement of the substate coherence (quantum beat) at f 0 = n f p + n ' f m ( n , n ' : integer, f 0 : sublevel splitting, f p : pulse repetition frequency, f m : modulation frequency), which can be detected by monitoring the optical anisotropy due to the substate coherence. Resonances can be obtained in the frequency domain by sweeping f m . Pressure shift coefficients of the hyperfine splitting in Na 3 2 S 1/2 are measured to be 82, 61, -1 and -47 Hz/Torr for He, N 2 , Ar and Kr, respectively, within an accuracy of ±3 Hz/Torr.
A novel technique is described for high-resolution spectroscopy. The time evolution of a coherent superposition of atomic substates created by a short resonant laser pulse is monitored via changes in polarization of a delayed probe pulse due to stimulated emission. As a demonstration the method was applied to the Zeeman splitting of the 63P16^{3}P_{1}63P1​ state of ytterbium.
Recent advances in the development of synchronously mode-locked dye-laser systems have permitted the first low-power measurement of the time-resolved dephasing dynamics of a Raman active molecular vibration. Excitation and delayed probing of the coherent ensemble of vibrators is accomplished with the help of synchronized picosecond pulse trains from two independently tunable mode-locked dye lasers. A new probe technique, based on a gain measurement, is employed that provides a signal that scales linearly with the coherent vibrational amplitude. We demonstrate this technique with the first measurement of the dephasing dynamics of the normal mode (656.5 cm−1) of CS2 in the liquid state. An exponential decay with time constant 20±1 psec is obtained for the isotropic component of the coherent scattering.
Pressure shifts of the hyperfine splitting in Na 3(2)S((1/2)) that are due to buffer gases have been measured for the first time to our knowledge by all-optical means using the method of synchronized-quantum-beat spectroscopy reported previously [Y. Fukuda et al., Opt. Commun. 38, 357 (1981)]. The substate coherence is excited and detected with amplitude-modulated mode-locked laser pulses tuned to the D(1) line (pulse-repetition frequency, f(p); modulation frequency, f(m)), and the resonances observed at f(0) = nf(p) + ńf(m), (n and n' are integers) are used for the measurement. The pressure-shift coefficients obtained at 210 degrees C are 82, 61, -1, and -47 Hz/Torr for He, N(2), Ar, and Kr, respectively, within an accuracy of +/-3 Hz/Torr.
We have demonstrated the feasibility of Doppler-free two-photon spectroscopy with a train of picosecond standing-wave light pulses from a synchronously pumped mode-locked cw dye laser. The actively controlled mode spectrum provides a means for accurate measurements of large frequency intervals. From a multipulse spectrum of the sodium $3s\ensuremath{-}4d$ transition we have determined a new value of the 4d4d4d fine-structure splitting, 1028\ifmmode\pm\else\textpm\fi{}0.4 MHz.
I. A new technique utilizing the electro-optic frequency switching of a single mode ( 6 Mhz) dye laser was used to observe free induction decay and optical nutation in iodine gas and optical nutation in an organic mixed crystal (pentacene in p-terphenyl) at low temperature. A new technique, incoherent resonance decay (IRO) was also developed. These experiments allow one to determine T_1 and T_2, the longitudinal and transverse relaxation times of the excited ensemble, in analogy with magnetic resonance. For I_2(g) at O∙C; T_l = 2.3 x 10^(-7) sec, T_2 ≃ 1 x 10^(-7) sec. These techniques are limited to a time scale > 10 nsec. II. The construction and characterization of cw, mode-locked dye laser capable of putting out a continuous train of reproducible sub-picosecond pulses is described. Experiments utilizing this laser for the measurement of picosecond coherent transients and time resolved absorption spectroscopy are proposed.