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International Conference on Luminescence - 1984

Hyperfine Spectroscopy and Spin Dynamics by Optical and Sublevel Coherence

Robert M. Shelby, R. M. Macfarlane

Published Jan 1, 1984• 0 citations
Publisher

Abstract

It has been well established that for many metastable electronic levels of impurity ions in insulators, optical coherence times at liquid helium temperatures are limited by magnetic interactions with host nuclear spins. 1 To understand coherence loss in detail, one needs measurements of optical and spin dephasing, magnetic properties and hyperfine structure of impurity ions, and spin dynamics of host nuclei. To this end techniques such as spectral hole burning, 2 coherent transients (e.g. photon echo), 1,3 and optical-rf double resonance 4 have been used. All of these are limited directly or indirectly by optical T2, and have not directly probed the dynamics of host nuclei.

DOI
10.1364/icol.1984.tuk1

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It has been well established that for many metastable electronic levels of impurity ions in insulators, optical coherence times at liquid helium temperatures are limited by magnetic interactions with host nuclear spins. 1 To understand coherence loss in detail, one needs measurements of optical and spin dephasing, magnetic properties and hyperfine structure of impurity ions, and spin dynamics of host nuclei. To this end techniques such as spectral hole burning, 2 coherent transients (e.g. photon echo), 1,3 and optical-rf double resonance 4 have been used. All of these are limited directly or indirectly by optical T2, and have not directly probed the dynamics of host nuclei.
The dynamics of nuclear spins in atomic and molecular environments have been examined in exquisite detail over the past 27 years by the methods of pulsed nuclear magnetic resonance. The early discovery of the spin echo by Erwin Hahn and the transient nutation effect by Henry Torrey initiated the field by introducing coherent transient phenomena to radio-frequency spectroscopy. An entire class of coherent spin transients could be observed by a simple variation of the rf pulse sequence, and from the decay characteristics the various spin-dephasing mechanisms could be examined separately. In short, these methods allowed decomposition of the spin-transition linewidth into its broadening components, and also offered new and versatile ways for performing high-resolution rf spectroscopy.
Optical spectroscopy provides a useful tool for probing the structure and dynamics of solids. Over the years, optical methods have evolved from absorption spectroscopy to more complex methods such as spectral hole burning, photon echoes, and luminescence line narrowing. The absorption spectrum provides information about inhomogeneous broadening, while the latter approaches provide information about the systematics of the homogeneous line shape information that is often obscured by inhomogeneous broadening. When external perturbations such as strain or electric fields are applied, details of the local site can be obtained. Recently, the ultimate limit of optical spectroscopy has been attained, in which the spectral properties of individual single impurity molecules in a solid can be measured, with all ensemble averaging removed. This novel regime has provided additional, previously unobtainable, information on a highly local scale, such as the direct observation of the spectral shifting of a single molecule produced by configurational transitions of the host. It is to be expected that further surprises await us in this new frontier of single-molecule spectroscopy in solids.
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:
Recent experiments on time-resolved hole-burning (TRHB) [1-3] and nonexponential photon-echo decays [4,5] in low-temperature ion-doped crystals have demonstrated the multi-timescale dynamics of host nuclei whose spin flips provide the main source of stochastic fluctuations Ut of an impurity ion transition frequency ωab(ωabt=ωab+Ut) leading to optical dephasing and spectral diffusion. Such complicated spin dynamics results from the existence around the impurity ion of the "frozen core" of nuclear spins with their flip rates to be greatly slowed compared to the unperturbed bulk spins.
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