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Physical Review Letters

Temperature Dependence of Fluorescence Linewidths in Pr F3 : A Comment on "Excited-State Exchange Broadening of Optical Transitions in Pr Cl3 ".

J. W. Allen

Published Aug 25, 1975• 0 citations
Publisher
DOI
10.1103/physrevlett.35.547

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Temperature Dependence of Fluorescence Linewidths in Pr F3 : A Comment on "Excited-State Exchange Broadening of Optical Transitions in Pr Cl3 "

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Spectral energy transfer in Pr F3 , Pr Cl3

D. S. Hamilton, Peter M. Selzer, William M. Yen

Time-resolved fluorescence line narrowing is used to study spectral energy transfer in Pr${\mathrm{F}}_{3}$ and Pr${\mathrm{Cl}}_{3}$. The excitation spectrum of Pr${\mathrm{F}}_{3}$ in the region of the ${(^{3}H_{4})}_{1}\ensuremath{\rightarrow}^{3}P_{0}$ absorption indicates that several strong satellite lines accompany the main transition, their origin being ascribed to different ${\mathrm{Pr}}^{3+}$ ions lying in strongly perturbed lattice sites. The spectral transfer within the inhomogeneously broadened main transiton is measured, where the energy mismatch is about 2 ${\mathrm{cm}}^{\ensuremath{-}1}$. This process is characterized by a strong ($\ensuremath{\sim}{T}^{4.3}$) dependence of the transfer probability on sample temperature. The growth of the full inhomogeneous emission profile accompanies a uniform decay of the donor line shape. A transfer process between the lowest-energy satellite ions is also measured. Here the energy mismatch is 32 ${\mathrm{cm}}^{\ensuremath{-}1}$ resulting in a weak temperature dependence for the transfer rate. Both the intraline and intersatellite transfer are characterized by simple exponential rate equations. Recent calculations of phonon-assisted transfer probabilities are compared to our measurements, with the intersatellite transfer ascribed to a "one-phonon direct" process whereas the transfer within the main transition occurs by a "one-phonon second-order" mechanism. In Pr${\mathrm{Cl}}_{3}$ the transfer times are faster than the 15-nsec response time of our detection system indicating a much stronger ion-ion coupling.

Physical review. B, Solid state•Sep 1, 1977•62 citations
Data are reported which show that the temperature dependence of fluorescence linewidths in PrF3{\mathrm{F}}_{3}F3​ are qualitatively like those in LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+. This result is interpreted as supporting the explanation of German and Kiel for the anomalous temperature dependence of fluorescence linewidths in PrCl3{\mathrm{Cl}}_{3}Cl3​.
We have observed an anomalous broadening of two fluorescence lines in PrCl3{\mathrm{Cl}}_{3}Cl3​. The new effect is observed only when the terminal state is a magnetic doublet and only at low temperatures (T<100T<100T<100 K). However, the effect is seen far above any transition or ordering temperature. The broadening can be, at least partially, suppressed by application of a large magnetic field. The effect is almost certainly a cooperative phenomenon arising from an interaction between ground- and excited-state ions.
Time-resolved fluorescence line narrowing is used to study spectral energy transfer in PrF3{\mathrm{F}}_{3}F3​ and PrCl3{\mathrm{Cl}}_{3}Cl3​. The excitation spectrum of PrF3{\mathrm{F}}_{3}F3​ in the region of the ${(^{3}H_{4})}_{1}\ensuremath{\rightarrow}^{3}P_{0}$ absorption indicates that several strong satellite lines accompany the main transition, their origin being ascribed to different Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions lying in strongly perturbed lattice sites. The spectral transfer within the inhomogeneously broadened main transiton is measured, where the energy mismatch is about 2 ${\mathrm{cm}}^{\ensuremath{-}1}$. This process is characterized by a strong ($\ensuremath{\sim}{T}^{4.3}$) dependence of the transfer probability on sample temperature. The growth of the full inhomogeneous emission profile accompanies a uniform decay of the donor line shape. A transfer process between the lowest-energy satellite ions is also measured. Here the energy mismatch is 32 ${\mathrm{cm}}^{\ensuremath{-}1}$ resulting in a weak temperature dependence for the transfer rate. Both the intraline and intersatellite transfer are characterized by simple exponential rate equations. Recent calculations of phonon-assisted transfer probabilities are compared to our measurements, with the intersatellite transfer ascribed to a "one-phonon direct" process whereas the transfer within the main transition occurs by a "one-phonon second-order" mechanism. In PrCl3{\mathrm{Cl}}_{3}Cl3​ the transfer times are faster than the 15-nsec response time of our detection system indicating a much stronger ion-ion coupling.