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Optics and Spectroscopy

Modulation frequency doubling in the axially periodic dependence of the luminescence of F+3 centers in LiF crystals

Evgueni F. Martynovich, V. P. Dresvyanskiy, С. А. Зилов, N. A. Bronnikova, N. T. Maksimova, Anton A. Starchenko

Published Aug 1, 2006• 1 citation

Abstract

A spatially periodic distribution of the luminescence intensity of F2 and F 3 + color centers is observed in LiF crystals with induced anisotropy. The period of spatially periodic modulation of the luminescence intensity generally coincides with the period of the change in the polarization state of excitation light. For F2 centers, the experimental axial spatially periodic dependence of the luminescence intensity is close to the calculated dependence obtained in the description of the absorption and radiative transitions in the centers by linear oscillators oriented along six C 2 axes of the cubic crystal. However, for F 3 + centers, the same experiment shows a spatially periodic distribution of luminescence intensity with a modulation period shorter by a factor of 2. It is shown that this effect of modulation frequency doubling in the spatially periodic pattern of the luminescence of color centers arises due to the nonlinear dependence of the luminescence intensity on the excitation light intensity. For F 3 + centers, upon luminescence excitation in the absorption band with λmax = 452 nm, the modulation frequency doubling is due to the saturation of the metastable triplet state of such a center.

DOI: 10.1134/s0030400x06080145

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A spatially periodic distribution of the luminescence intensity of F2 and F 3 + color centers is observed in LiF crystals with induced anisotropy. The period of spatially periodic modulation of the luminescence intensity generally coincides with the period of the change in the polarization state of excitation light. For F2 centers, the experimental axial spatially periodic dependence of the luminescence intensity is close to the calculated dependence obtained in the description of the absorption and radiative transitions in the centers by linear oscillators oriented along six C 2 axes of the cubic crystal. However, for F 3 + centers, the same experiment shows a spatially periodic distribution of luminescence intensity with a modulation period shorter by a factor of 2. It is shown that this effect of modulation frequency doubling in the spatially periodic pattern of the luminescence of color centers arises due to the nonlinear dependence of the luminescence intensity on the excitation light intensity. For F 3 + centers, upon luminescence excitation in the absorption band with λmax = 452 nm, the modulation frequency doubling is due to the saturation of the metastable triplet state of such a center.

Non-stationary mechanisms of spatial modulation of luminescence intensity in anisotropic quantum systems within birefringent crystals under their interaction with ultrashort polarized laser pulses were studied. We have found connection between this phenomenon and phase relaxation of excited quantum systems. We have as well grounded a new method for investigation of coherency of quantum systems based on study of characteristic properties of modulation phenomena. It was shown that the influence of the frequency dispersion on the clarity of the modulation picture in insignificant at durations of 100 fs and greater, even for crystals with strong dispersion. Due to the existence of chirp in femtosecond pulses exciting the luminescence, modulation period in instant distribution of absorbed power decreases over distance. In the time-integrated picture of spatial distribution of luminescence intensity, the rate of decrease of modulation depth grows. This leads to new possibilities in experimental investigation of the value of chirp of femtosecond pulses.

Abstract This work is an experimental study of the modulation which has been found in resonance radiation when the fluorescing vapour is subjected to static and radio-frequency magnetic fields, as in the double resonance experiment of Brossel & Bitter. The particular example chosen for study in this work also was the resonance line λ 2537 Å of mercury. The experimental observations are compared with the predictions of a theoretical treatment which has already been published. The phenomenon was studied under a variety of geometrical configurations. When the polarization of the exciting light allowed excitation to only one excited state (a component of a Zeeman multiplet), the depth of modulation was found to depend on the closeness to resonance of the frequency, ω0, of the radio-frequency field to the Larmor precessional frequency, ω = γH , in the static field H. When the polarization of the exciting light allowed excitation to more than one component of the multiplet, resonance effects were found in the depth of modulation and in the mean intensity of the fluorescent light at fields where the applied frequency was equal, not to the Larmor frequency alone, but to combinations of the Larmor frequency with the nutational frequency. From a quantum-mechanical point of view, these new phenomena are related to the interference effects which are found in resonance fluorescence when there is degeneracy between excited states: in the present case the degeneracy is induced by the radio-frequency field. The ease with which the geometrical conditions could be altered allowed the theory to be tested in considerable detail without quantitative assessment of the resonance line contours: nevertheless, a quantitative study was made of one particular feature. The predictions of the theory were confirmed at all points where they were tested.