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Journal of the Magnetics Society of Japan

A STUDY OF MAGNETIC INTERACTIONS IN RARE EARTH DOPED INSULATORS USING SPECTRAL HOLEBURNING AND OPTICAL COHERENT TRANSIENTS

R. M. Macfarlane

Published Jan 1, 1987• 0 citations
Publisher

Abstract

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.

DOI
10.3379/jmsjmag.11.s1_1

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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.
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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.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,
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:
Following a brief review of laser frequency and time domain techniques for overcoming inhomogeneous broadening of optical transitions in solids, recent studies on the failure of the optical Bloch equations (OBE) in describing saturation and coherent transient phenomena in ruby will be discussed. Experiments using free induction decay (FID), as in the original work on the system Pr3+:LaF3 by DeVoe and Brewer1, as well as extensions to rotary echos2 and hole-burning3 will be described. At low fields (~ 0.4 T), the time and frequency domain linewidth variation with Rabi frequency agree provided care is taken to avoid line broadening caused by spectral diffusion4. Recent work at high fields (~ 5 T), where Cr-Cr electron spin flipping is suppressed5, shows that spectral diffusion decreases and the dephasing time increases. Observed frequency domain hole widths as narrow as 18 kHz (FWHM) have been obtained for the 4 A2(−1/2)→E¯(−1/2) optical transition in dilute ruby using a pump-probe technique4. Work with such narrow holes emphasizes the fundamental limits imposed by the uncertainty principle and as an aside, a thought experiment where single photons are transmitted through "frequency slits" will be discussed.