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IEEE Journal of Quantum Electronics

Fast dephasing processes studied with a femtosecond coherent Raman system

Wolfgang Zinth, R. Leonhardt, W. Holzapfel, W. Kaiser

Published Feb 1, 1988• 73 citations
Publisher

Abstract

Synchronous pumping of a femtosecond and a tunable picosecond dye laser provides synchronized trains of ultrashort pulses at variable frequency difference. The system allows the authors to study coherently excited Raman transitions with femtosecond time resolution. Fast dephasing processing with decay times of a few hundred femtosecond are measured.>

DOI
10.1109/3.145

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Journal of the Optical Society of America B•Dec 1, 1989•4 citations
Synchronous pumping of a femtosecond and a tunable picosecond dye laser provides synchronized trains of ultrashort pulses at variable frequency difference. The system allows the authors to study coherently excited Raman transitions with femtosecond time resolution. Fast dephasing processing with decay times of a few hundred femtosecond are measured.>
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.
Synchronous mode locking of two dye lasers was employed to obtain pairs of independently tunable picosecond pulses that were precisely synchronized in time. Overlapped pulses in strontium vapor were used to generate tunable picosecond pulses in the vacuum uv. The tunability was employed to study resonant enhancement of a four-wave parametric process by the 4d6p autoionizing resonance. Mutually separated pulses were employed to measure the build-up and decay of coherence for a two-quantum excited state. The decay was found to be faster than theoretical predictions that assume only velocity dephasing.
A new method to measure picosecond or subpicosecond vibrational-dephasing dynamics with the use of incoherent or broadband light is presented theoretically and experimentally. It is based on a transient coherent Raman process with three beams. In our experimental scheme, two of them are incoherent light from a single source, and a delay time between the two is variable. A third beam has a higher frequency than the incoherent light by a vibrational energy in a molecule of interest, and is coherent in the delay-time range of the measurement. The delay-time dependence of coherent Stokes Raman scattering (CSRS) intensity offers the information about the coherence dynamics of the vibrational transition with a resolution time determined only by the correlation time of the incoherent light. For the theoretical calculation, a three-level model of the molecular system with homogeneous broadening is used, and delay-time dependences of the CSRS signal are calculated for off-resonance and resonance cases. Dephasing dynamics of the 2915-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ mode in dimethylsulfoxide was observed experimentally by the new method with the use of nanosecond laser pulses, and the result agrees well with that obtained with picosecond pulses.
A simple method for observing coherent optical-transient phenomena is described. Effects such as photon echoes and free induction decay (FID) should allow studies of the dynamic properties of atoms, molecules, and solids on a time scale ranging from milliseconds to \ensuremath{\sim} 50 ps. The frequency of a cw dye laser is switched with an intracavity electro-optic modulator, producing in an external sample coherent transients which are detected in the forward beam. Measurements of long dephasing times are possible, as in FID, because the laser can oscillate indefinitely at the new frequency following a step-function switching pulse. Measurements of short decay times are also practical because the switching time is not restricted by the laser gain or cavity ringing time. In addition, the dye's dephasing time of a few picoseconds or less is too rapid to interfere with these observations. Since the pulse sequence can be preselected, the entire class of coherent optical transients is accessible. The method thus incorporates all of the advantages inherent in Stark switching, including heterodyne detection and high sensitivity, without being restricted to Stark-tunable systems. Laser frequency switching is discussed also in terms of a theoretical model which exposes the time-dependent properties of a phase-modulated cavity mode. Dephasing studies have been carried out thus far in atomic and molecular gases and low-temperature solids containing inorganic impurity ions or large organic molecules. The utility of the FID effect is emphasized where precise dephasing times are obtained from time-frequency Fourier transformation of FID signals using a digital computer. The first quantitative and detailed test of FID theory is provided by these experimental techniques.
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.
A detailed theoretical analysis is presented of the dephasing signal measured in four-beam picosecond time-resolved stimulated-Raman-gain experiments. The analytical expressions derived are successful in simulating observations on the CS2 model system under various experimental conditions. It is established that the tail of the curve for sufficiently long delay times is uniquely determined by the vibrational Raman term that yields the vibrational dephasing time T2. It is also found that the rotational dephasing time cannot be fundamentally determined from the rotational Raman peak centered around zero delay. Furthermore, it is shown that the coherence properties of the stimulating laser fields, as distinguished from their pure pulse-envelope properties, are crucially important in determining the time resolution of the experiments and for explaining several experimental phenomena observed under mismatched excitation-pulse conditions. In this respect, the domain model for mode-locked pulses has proved to be useful. It is found that the time resolution of the dephasing measurements is determined by the combined pulse-coherence time of the driving fields and not by the cross-correlation width of the pulse envelopes.