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Journal of the Physical Society of Japan

Cr3+ Ion Pair Spectrum in Ruby

Masayoshi Naitō

Published Jun 1, 1973• 33 citations
Publisher

Abstract

The optical spectrum due to the exchange coupled Cr 3+ ions in ruby has been studied theoretically. The effect of the lowering of the Cr 3+ site symmetry due to the formation of a pair was taken into account. For the 2nd neighbor pair, a good fitting of the excited state energies between theory and experiment was obtained. The effect of the higher order exchange is found to be very important for this pair. It is also found that the deviation of the Cr 3+ site symmetry from C 3 is rather large for this pair. For the 4th neighbor pair, the level diagram of the excited state was obtained and the absorption intensities were calculated. Most of the observed lines in this pair are explained by this theory. The lines so called N 1 and N 2 are found to be the transitions due to the exchange induced electric dipole.

DOI
10.1143/jpsj.34.1491

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Physical review. B, Solid state•Sep 1, 1973•13 citations
The optical spectrum due to the exchange coupled Cr 3+ ions in ruby has been studied theoretically. The effect of the lowering of the Cr 3+ site symmetry due to the formation of a pair was taken into account. For the 2nd neighbor pair, a good fitting of the excited state energies between theory and experiment was obtained. The effect of the higher order exchange is found to be very important for this pair. It is also found that the deviation of the Cr 3+ site symmetry from C 3 is rather large for this pair. For the 4th neighbor pair, the level diagram of the excited state was obtained and the absorption intensities were calculated. Most of the observed lines in this pair are explained by this theory. The lines so called N 1 and N 2 are found to be the transitions due to the exchange induced electric dipole.
A rather simple method of determining the lifetimes of the excited states of exchange-coupled ion pairs in ruby is described. The technique utilizes a chopped pump light and phasesensitive detection. It has permitted a great increase in the resolution of optical transitions, and in particular, it allows for a virtual elimination of the vibronic sidebands of the RRR lines, in order that the true pair spectrum may stand out clearly. Furthermore, transitions originating from different excited levels may be definitely distinguished, thus aiding in the identification of particular transitions with a given pair type. The chronospectroscopic method is of potential value in the studies of energy-transfer mechanisms between single ions and pairs. It has also provided evidence for a fourth-neighbor absorption band at 6050 \AA{}.
Absorption transitions between two excited optical states in ruby have been studied by comparing the absorption coefficients measured under optically pumped and unpumped conditions. The spectrum has been determined in the π-and σ-polarizations in the photon energy range from 5,500 to 45,000 cm -1 . Several absorption bands have been found which arise from the transitions from the excited states t 2g 3 2 E g and t 2g 3 2 T 1g of the Cr 3+ ion. From the locations and intensities of these bands, the terminal states of the observed transitions are assigned to the charge transfer state, the t 2g 3 2 T 2g state, and the doublet states belonging to the electron configuration t 2g 3 e g . Calculated energies between these states and the metastable states, t 2g 3 2 E g and t 2g 3 2 T 1g , are in good agreement with the peak energies of the observed absorption bands. The present experiment gives new information inaccessible by the ordinary ground state absorption measurement, such as the locations of several doublet states with the configuration t 2g 2 e g and the intensities of doublet-doublet transitions in ruby.
The absorption intensities, widths and wave-numbers of R 1 , R 2 and B 1 B 2 lines of Cr 3+ in ruby for the polarized light E ⊥ C 3 and E // C 3 are experimentally studied at 20°K and 4.2°K. Zeeman effect is also studied, using a magnetic field H 0 =24,000 φ, for both R and B lines. The Zeeman effect has not been observed yet for the B lines, while Lehmann has already observed the Zeeman effect for R lines. In our results of R lines, the quantitative aspects of Lehmann's experiment are improved. The comparison is made with the theoretical results given in Part A and it is shown that nice agreements can be obtained when suitable assignments of the spectra are adopted and when fairly large g -shifts of the excited states are introduced.
Transitions to the states of Cr3+{\mathrm{Cr}}^{3+}Cr3+ pairs where both ions are excited to the 2Eg^{2}E_{g}2Eg​ levels have been observed in LaAlO3{\mathrm{O}}_{3}O3​:Cr3+{\mathrm{Cr}}^{3+}Cr3+. Of the predicted eight pair levels, three of the S=0S=0S=0 and one of the S=1S=1S=1 levels have definitely been identified at approximately twice the 2Eg^{2}E_{g}2Eg​ energy absorption. The remaining transitions either are obscured by the strong vibronic spectrum or are very weak. The polarization of the lines agrees with a model based on the mechanism of exchange-induced electric dipole moment.
Absorption and emission involving exchange-coupled nearest-neighbor Cr3+{\mathrm{Cr}}^{3+}Cr3+ and Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions have been observed in Cr3+{\mathrm{Cr}}^{3+}Cr3+-doped EuAlO3{\mathrm{O}}_{3}O3​ at the sum of the chromium 2Eg^{2}E_{g}2Eg​ and europium 7F1^{7}F_{1}7F1​ energies. Weak absorption at the difference energy has also been observed. The latter is the inverse of the previously studied europium terminated chromium emission. The intensities of the Eu3+{\mathrm{Eu}}^{3+}Eu3+ sideband transitions vary with the strength of the exchange-induced electric dipole moment.