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.

Optics and SpectroscopyAug 1, 20061 citation

Effect of finite correlation time of frequency modulation on resonance Raman scattering and luminescence

T. Takagahara

The effects of the finite correlation time of the external modulation on the secondary-emission spectra are clarified emphasizing the deviation from the motional narrowing limit or the impact approximation in the case of large off-resonance excitation. The dependences of the excitation spectrum of the secondary emission on the modulation parameters and on the inhomogeneous broadening are studied systematically. It is found that the excitation spectrum of the luminescence shows a faster decrease than that of the Raman scattering as the off-resonance frequency increases. The present theory is relevant for explaining the recent experiment by Watanabe, Kinoshita, and Kushida [Chem. Phys. Lett. 126, 197 (1986)] on the \ensuremath{\beta}-carotene in solutions. A general theory of the time-resolved spectra of the secondary emission is formulated to incorporate the effect of the finite correlation time. The luminescence component shows a slow temporal decay with the longitudinal relaxation rate. It is found for the first time that the difference is unexpectedly large between the transient behavior of the luminescence intensity and that of the intermediate-state population for the slow-modulation regime and that the difference indicates the effect of finite correlation time of the frequency modulation. On the other hand, the transient behavior of the Raman scattering contains a fast component that follows the envelope of the excitation-pulse intensity and the same slow component as the luminescence. The ratio of the slow component to the total intensity depends sensitively on the modulation parameters and the off-resonance frequency. The modulation parameters of the system in question can be estimated from these dependences in combination with the spectral characteristics of the emission under stationary excitation.

Physical Review AMar 1, 198710 citations