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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Stochastic theory of the transient hole burning in the systems with homo- and heterogeneous broadening

S. Ya. Kilin, Alexander P. Nizovtsev

Published Jan 1, 1992• 0 citations
Publisher

Abstract

Transient hole burning in the impurity crystals is studied by stochastic laser-dependent dephasing theory using the two random telegraph processes model for the frequency fluctuations.
DOI
10.1364/shbl.1992.pd4

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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.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations
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.
In recent years the microscopic description of inhomogeneous broadening of electronic transitions of chromophores in crystals and glasses has attracted much interest [1–3]. In the phenomenological model proposed by Selzer [1], it is assumed that the energies of the initial and final states involved in the optical transition exhibit a one-to-one correlation. In an alternative approach by Lee et al [2], the two states are considered as completely uncorrelated. Very recently, a more general microscopic theory has been presented by Laird and Skinner [3]. In the latter theory the aforementioned models are obtained as limiting cases. So far relatively few experiments have been reported which focus on the origin of inhomogeneous broadening.
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.