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High resolution laser spectroscopy of colour centres

R. M. Macfarlane, Richard T. Harley, Robert M. Shelby

Published Dec 1, 1982• 0 citations
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Abstract

The application of narrow band dye lasers to high resolution spectroscopy within the inhomogeneously broadened zero-phonon lines of colour centres is reviewed. Most work so far has centred on the use of holeburning which is exhibited by the majority of centres examined. This technique has been used to make detailed Stark and Zeeman effect measurements. In addition, optical coherent transients have been used to determined dephasing times and the results of optical phase switching and free decay experiments are discussed. (Author)

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The application of narrow band dye lasers to high resolution spectroscopy within the inhomo-geneously broadened zero-phonon lines of colour centres is reviewed. Most work so far has centered on the use of holeburning which is exhibited by the majority of centres examined. This technique has been used to make detailed Stark and Zeeman effect measurements. In addition, optical coherent transients have been used to determine dephasing times and the results of optical phase switching and free decay experiments are discussed.

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Le Journal de Physique Colloques•Feb 1, 1979•0 citations
The application of narrow band dye lasers to high resolution spectroscopy within the inhomogeneously broadened zero-phonon lines of colour centres is reviewed. Most work so far has centred on the use of holeburning which is exhibited by the majority of centres examined. This technique has been used to make detailed Stark and Zeeman effect measurements. In addition, optical coherent transients have been used to determined dephasing times and the results of optical phase switching and free decay experiments are discussed. (Author)
The application of narrow band dye lasers to high resolution spectroscopy within the inhomo-geneously broadened zero-phonon lines of colour centres is reviewed. Most work so far has centered on the use of holeburning which is exhibited by the majority of centres examined. This technique has been used to make detailed Stark and Zeeman effect measurements. In addition, optical coherent transients have been used to determine dephasing times and the results of optical phase switching and free decay experiments are discussed.
The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site­ selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry­ Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:
High resolution laser spectroscopy is providing new insights into magnetic interactions in insulating solids by providing a way of measuring small interactions in the presence of much larger inhomogeneous broadening. Here we briefly review some of the techniques and examples of the information obtained with them. Included in this discussion are the use of spectral holeburning to measure linear and nonlinear Zeeman interactions, the magnetic field dependence of optical dephasing times determined from coherent transients and quantum beat free induction decay measurements of small sublevel splittings.
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.
At very low temperatures, the spread in the different environments of matrix embedded dye molecules results in an inhomogeneously broadened S1 ← S0 band. Spectroscopic techniques based on the appearence of optical zero phonon lines, such as fluorescence line narrowing, spectral hole-burning, and single molecule spectroscopy provide an experimental resolution limited by the homogeneous linewidth. From the investigation of the homogeneous line width as a function of different parameters (time, temperature) information on the guest host interactions responsible for the observed linewidth is obtained. Spectrally narrow features are extremely sensitive probes for external perturbations, such as electric fields, magnetic fields, or hydrostatic pressure.
A review of coherent transients is presented in this article. After a brief discussion of single-wave transients (free induction decay, optical nutation, etc...), two-wave transients, i.e. time-resolved saturation spectroscopy, are treated in more detail. It is shown that this technique of combining both frequency-and-time-resolution in laser spectroscopy allows one to study the various quantum-mechanical processes contributing to the lineshape, in particular (i) the interaction between the laser field and the atomic (or molecular) system, and (ii) the dynamics of the relaxation of the system. Applications to the analysis of Raman-type processes in three-level systems, power-broadening and velocity diffuston are given.