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Physical review. B, Condensed matter

Two-photon transition from H43 to S01 of Pr3+ in La F3

C. D. Cordero-Montalvo, N. Bloembergen

Published Jul 1, 1984• 37 citations
Publisher

Abstract

A direct two-photon absorption between crystal-field components of the $^{3}H_{4}$ ground-state configuration to the highest excited state $^{1}S_{0}$ in the $4{f}^{2}$ manifold of ${\mathrm{Pr}}^{3+}$ in La${\mathrm{F}}_{3}$ has been observed. The magnitude of the intensities and the polarization dependence require a third- and fourth-order theoretical analysis, similar to that developed for two-photon absorption of ${\mathrm{Gd}}^{3+}$ in La${\mathrm{F}}_{3}$.

DOI
10.1103/physrevb.30.438

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A direct two-photon absorption between crystal-field components of the 3H4^{3}H_{4}3H4​ ground-state configuration to the highest excited state 1S0^{1}S_{0}1S0​ in the 4f24{f}^{2}4f2 manifold of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ has been observed. The magnitude of the intensities and the polarization dependence require a third- and fourth-order theoretical analysis, similar to that developed for two-photon absorption of Gd3+{\mathrm{Gd}}^{3+}Gd3+ in LaF3{\mathrm{F}}_{3}F3​.
Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited 1D2^{1}D_{2}1D2​ state of LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. Our measurements are in agreement with the results obtained by Erickson from his saturated-and-enhanced-absorption study of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ transition in LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+.
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A comprehensive report and analysis of our observations of numerous parity-allowed direct two-photon transitions within the 4f74{f}^{7}4f7 configuration of the Gd3+{\mathrm{Gd}}^{3+}Gd3+ ion is presented. The experimental technique is ultraviolet fluorescence detection following optical excitation with a dye-laser beam. Previous results and analyses are extended in three ways. (1) The intensities and polarization dependence of individual Stark components, in addition to integrated multiplet intensities, are reported and analyzed for Gd3+{\mathrm{Gd}}^{3+}Gd3+:LaF3{\mathrm{F}}_{3}F3​. In those cases ($^{8}S_{\frac{7}{2}}\ensuremath{\rightarrow}^{6}P_{\frac{5}{2}},^{6}D_{\frac{9}{2},\frac{3}{2},\frac{5}{2}}$) where a second-order theory of two-photon absorption adequately explains the integrated intensity, it also (with the exception of 6D92^{6}D_{\frac{9}{2}}6D29​​) explains the Stark-component intensities. The remaining transitions are anomalously strong, and in some cases violate the angular momentum selection rules $\ensuremath{\Delta}L,\ensuremath{\Delta}J\ensuremath{\le}2$ and exhibit strong anisotropies, in contradiction to the second-order theory. It is shown that introduction of third- and fourth-order contributions involving spin-orbit and/or crystal-field interactions among levels of the 4f65d4{f}^{6}5d4f65d configuration, which serve as intermediate states, can account for both the integrated and Stark-component intensities of these transitions. (2) The strong anisotropy observed for the transitions $^{8}S_{\frac{7}{2}}\ensuremath{\rightarrow}^{6}P_{\frac{3}{2}},^{6}I_{J},^{6}D_{\frac{1}{2}}$ in Gd3+{\mathrm{Gd}}^{3+}Gd3+:LaF3{\mathrm{F}}_{3}F3​ is explained quantitatively as a polarization-dependent interference between contributions to the intensity which are comparable in magnitude. Interference is destructive for $\stackrel{\ensuremath{\rightarrow}}{E}\ensuremath{\parallel}\stackrel{^}{z}$ and constructive for $\stackrel{\ensuremath{\rightarrow}}{E}\ensuremath{\perp}\stackrel{^}{z}$, creating an order-of-magnitude contrast in the line strength for the two polarizations. (3) A two-photon excitation spectrum of Gd3+{\mathrm{Gd}}^{3+}Gd3+ in aqueous solution is reported. Linewidths comparable to those of room-temperature solids and Stark splittings which suggest a low-symmetry quasistatic environment are observed.
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