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Optics and Spectroscopy

The influence of orientational effects on the dispersion of the kinetics of hole burning in impurity centers

Ivan V. Stanishevsky, K. N. Solovyov

Published Aug 1, 2004• 1 citation
Publisher

Abstract

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.

DOI
10.1134/1.1790644

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Radiation effects and defects in solids•Nov 1, 1991•4 citations
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.
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.
The rate equation for the population inversion of homogeneously broadened 4-level lasers is solved for the cases of small and large mobility of excited states. Considered are drift and diffusion, i.e., collective and random motions along the laser axis. Both drift and diffusion smooth spatial holes which are burned into the population inversion by standing-wave fields. A drift results also in a drag effect, i.e., a phase lag between the population inversion and the standing-wave field. For homogeneously broadened lasers, sufficient smoothing of spatial holes will result in spontaneous full-power single-frequency operation. This is examined by calculating the unsaturated gains of secondary modes as a function of the excitation, drift, and diffusion parameters. Spatial hole burning is insignificant for gas lasers because of their large carrier diffusion. Furthermore, ionic drift in gas-ion lasers alone could effectively quench spatial hole burning. This is in contrast to dye lasers where drifts, i.e., longitudinal flow rates of the order of the sound velocity, would be required to obtain a single-frequency output. In solid-state lasers like ruby and Nd: YAG, energy diffusion between lattice sites is shown to significantly reduce spatial hole depths although the matrix elements for the exchange are quite small. An experiment is described which confirms the theory and allows the measurement of small diffusion constants of excited laser states. For the 4F3/2 level in Nd: YAG a value of 5×10−7 cm2/sec is obtained. This energy exchange among Nd3+ sites contributes 0.3 GHz to the homogeneous linewidth. Implications for axial mode selection and single-frequency oscillation of various lasers are discussed.
The authors consider photochem. hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. The authors derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these satn. curves to exptl. data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In expts. with pulsed lasers strong deviations from this ideal behavior are obsd. An extended theory including satn. gives a satisfactory description of this phenomenon and provides a new method for the detn. of photochem. quantum yields.
The dispersive kinetics of nonphotochemical burning and spontaneous filling of the zero-phonon hole of Cresyl Violet in polyvinyl alcohol at 1.6 K are analyzed in terms of the standard external two-level system (TLSezt) model for probe–glass systems and a distribution function for the tunnel frequency derived from a normal distribution function for the tunnel parameter λ. Average values for the relaxation rates for burning and filling are determined. It is shown that the dominant mechanism for filling is not global spectral diffusion but rather antihole reversion. A high degree of positive correlation between the rates of burning and filling associated with the TLSext is found. A new methodology that permits a more physically reasonable interpretation of spontaneous hole-filling kinetics is described. It is based on the hypothesis that only a fraction of burned sites, on reversion to the ground state, yield sites with resonance frequencies that lie within the hole profile.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.