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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Kinetics of Hole Burning in Inhomogeneously Broadened Spectra: the Origin of Nonexponentiality and Problem of Burning Efficiency Dispersion

E.I. Al’shits, B. M. Kharlamov, N.I. Ulitsky

Published Jan 1, 1991• 0 citations

Abstract

High inhomogeneous broadening of impurity spectra in amorphous media reflects one type of dispersion, characteristic for disordered systems: dispersion of electronic transition frequency. In principle, there can exist a pronounced dispersion of other parameters: homogeneous line width (Γ), Debay-Waller factor (α), hole burning efficiency (ϕ), etc. The problem of the burning efficiency dispersion (BED) was extensively discussed in the recent years ([1-6] and references therein). The nonexponentiality of the burning kinetics was treated in some publications [1-3,6] as an evidence of such dispersion. But burning kinetics is always nonexponential in strongly inhomogeneously broadened systems, if a burning laser line width Δνl is much less then Γ. That was found experimentally and treated theoretically in one of the first publications on a hole burning [7] (see, also [8]). All other sources of the nonexponentiality are, in fact, additional to this one. So, it’s not easy to attain experimentally the BED parameters on such background. The procedure of a numerical fit ting of the burning kinetic with BED, developed in [4,5], is correct, but it looks unreliable due to many fitting parameters.

DOI: 10.1364/pshb.1991.fe2

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Because of inevitable size distribution, shape variations, different concentration of impurities and defects, and fluctuations of local environment and charge distribution, every ensemble of nanocrystals dispersed in some solid or liquid medium possesses inhomogeneously broadened absorption and emission spectra. Therefore, a number of properties inherent in molecular and atomic inhomogeneously broadened spectra can be a priori foreseen for nanocrystals. These include spectral hole-burning, fluorescence line narrowing under selective excitation, and decay time distribution. At the same time, spectrally selective techniques developed for inhomogeneously broadened molecular and atomic structures have been successfully applied to nanocrystals providing evaluation of individual parameters smeared as a result of inhomogeneous broadening. This chapter gives a brief overview of specific phenomena inherent in all spectrally inhomogeneous media and a survey of the relevant experimental techniques including nonlinear pump-and-probe spectroscopy, fluorescence excitation spectroscopy, and single molecule spectroscopy. Population-induced optical nonlinearity and spectral hole-burning Every real system consisting of particles with discrete energy levels exhibits absorption saturation under intense optical excitation. The only example of a nonsaturable system is an ensemble of ideal harmonic oscillators that possess an infinite number of equally spaced energy levels, optical transitions allowed only for a couple of neighboring levels, and the probability of optical transitions being proportional to the level number (Stepanov and Gribkovskii 1963).

Persistent spectral hole burning (PSHB) was discovered in organic molecular system in 1974[1]. Five years later, PSHB in inorganic materials was discovered in NaF by R. M. Macfarlane et al [2]. In 1985, A. Winnacker et al [3] first observed photon gated spectral hole burning in BaFCl: Sm2+ at 2K. Hole burning(HB) is useful in high resolution spectroscopy. It is also of crucial importance for the application to frequency domain optical storage. The storage density is proportional to the ratio of inhomogeneous linewidth(Γi) to the homogeneous linewidth(Γh), N(= Γi/Γh). The inhomogeneous linewidth of 5D0-TF0 transition of Sm2+ is 16GHz and the hole width is 25MHz in BaFCl at 2K[3]. For this material, the inhomogeneous linewidth changes only moderately with the temperature; On the other hand, the homogeneous linewidth increases rapidly as the temperature rises. Then, a small value of N(~2) can be estimated when HB temperature is raised to 77K. That means, it is difficult to burn a hloe in the inhomogeneous line in BaFCl:Sm2+ at 77K. To maintain a reasonable storage capacity or to study HB at a quite high temperature, a large inhomogeneous linewidth is in great request.

The dynamics of laser hole burning in a three-dimensional system of fixed isotropically oriented oscillators is simulated. The kinetic curves obtained are analyzed using methods of solving the inverse problem. The contribution of orientational effects to the total dispersion is studied and a quantitative characteristic of this contribution in the form of the standard deviation is obtained. The influence of the broadening of impurity centers on the dispersion of the burning kinetics of persistent and dynamical holes is studied. It is shown how some experimental instrumental factors can distort the results of the analysis of kinetic curves. On the basis of spectral and fluorescence experimental kinetic data, a method for determining the rate constants of the hole burning is proposed.

One-step (0 to 1) spectral hole burning (SHB) is widely used as a method of eliminating inhomogeneous broadening of spectra: the minimal width of the hole in the inhomogeneous distribution function (IDF) of the transition frequency Omega 01 is obtained by SHB with monochromatic light and is determined by the homogeneous linewidth sigma 0 = gamma 1 + Gamma (where gamma 1 and Gamma are the constants of the energetic and the phase relaxation of the (first) excited level respectively). Two-step (0 to 1 to 2) SHB is considered where the selective excitation of the first step is fixed by a photochemical transformation through the second excitation step. If the selective pulse is a coherent and single-sided exponential then, in the case of an extremely short fixing pulse ( delta pulse), on the increase of the time delay T between the selective and fixing pulses, a monotonic narrowing of the spectral hole in the IDF of the frequency Omega 01 takes place up to the limit width Gamma + mod gamma 1 - Delta mod (where Delta is the spectral width of the selective pulse).