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Optics and Spectroscopy

Effect of the migration of optical excitation along a nonuniform broadening profile on the luminescence spectrum

Semyon Vladimirovich Yakovlev

Published Aug 1, 1977• 0 citations
OpenAlex

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

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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 A•Mar 1, 1987•10 citations
Neodymium (Nd 3+ ) ions in mixed yttrofluorite crystals were excited by Y 3 Al 5 O 12 :Nd 3+ laser radiation. Luminescence spectra of these ions were recorded in 5x10 –6 sec after a delay time (relative to a short excitation pulse), which was varied within the range from 3 × 10 –5 to 2 × 10 –3 sec. The spectra recorded during the initial stages of the decay of the 4 F 3/2 metastable state were quite different from the spectra recorded under nonselective excitation conditions. The selectively excited spectra varied with time because of the migration of energy between metastable states but this migration was completed in a time of the order of 10 –3 sec at T = 300°K when the concentration of NdF 3 was 1 wt.%. The results indicated a correlation between the spectra of the energy levels of Nd 3+ in yttrofluorite crystals and structural disorder.
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.