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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 Jul 14, 1975• 2 citations
Publisher

Abstract

Data are reported which show that the temperature dependence of fluorescence linewidths in Pr${\mathrm{F}}_{3}$ are qualitatively like those in La${\mathrm{F}}_{3}$: ${\mathrm{Pr}}^{3+}$. This result is interpreted as supporting the explanation of German and Kiel for the anomalous temperature dependence of fluorescence linewidths in Pr${\mathrm{Cl}}_{3}$.

DOI
10.1103/physrevlett.35.128

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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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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.
Optical homogeneous linewidths of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}(1)$ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in BeF2{\mathrm{F}}_{2}F2​ and GeO2{\mathrm{O}}_{2}O2​ glasses reveal an anomalously smooth quadratic dependence on temperature from 8 to 300 K. The low-temperature behavior is consistent with a recent model of Lyo and Orbach involving an interaction with a single two-level system but the smooth quadratic behavior at all temperatures has deep consequences for the relative roles played by the ordinary phonons and the two-level system in line broadening.
We report the direct observation of energy migration and spectral diffusion in the 3P0^{3}P_{0}3P0​ state of LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.
The origin of inhomogeneous broadening in Pr-doped LaF3{\mathrm{F}}_{3}F3​ is examined by making time-resolved fluorescence measurements. Different positions in the inhomogeneous line are selectively excited, and the lifetime of the fluorescence is measured. The lifetime changes in a systematic way as the pump laser is scanned across the line. We have explained this change as a variation in local concentration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions at the different energies within the inhomogeneous line.