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Soviet Journal of Quantum Electronics

Optical absorption spectrum of excited Cr3+ions in MgAl2O4spinel crystals

B. K. Sevast’yanov, V. P. Orekhova

Published Jan 31, 1971• 2 citations
Publisher

Abstract

The absorption spectrum of Cr3+ ions in the magnesium spinel MgAl2O4 was determined for crystals excited by strong optical pumping, and for unexcited crystals. The absorption cross section of the 4A2g level was found to be 2.5 10–20 cm2, which was an order of magnitude smaller than that for ruby. The spectrum obtained for the excited crystals consisted of five absorption bands with maxima at 250, 325, 390, 440, and 550 nm. The absorption cross section for the maximum of the first band was ~2 10–18 cm2. The absorption cross sections at the maxima of the other bands were (1 – 2.5) 10–20 cm2. An energy scheme for Cr3+ ions in MgAl2O4 was derived.

DOI
10.1070/qe1971v001n01abeh003025

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The absorption spectrum of Cr3+ ions in the magnesium spinel MgAl2O4 was determined for crystals excited by strong optical pumping, and for unexcited crystals. The absorption cross section of the 4A2g level was found to be 2.5 10–20 cm2, which was an order of magnitude smaller than that for ruby. The spectrum obtained for the excited crystals consisted of five absorption bands with maxima at 250, 325, 390, 440, and 550 nm. The absorption cross section for the maximum of the first band was ~2 10–18 cm2. The absorption cross sections at the maxima of the other bands were (1 – 2.5) 10–20 cm2. An energy scheme for Cr3+ ions in MgAl2O4 was derived.
An investigation was made of the absorption spectrum of Cr 3+ ions in the ground ( 4 A 2 ) and metastable ( 2 E) states, and of the luminescence spectrum of the same ions in Y 3 Al 5 O 12 crystals at 300 and 77°K. The effective absorption cross sections were determined for the 4 A 2 state. The luminescence deexcitation time was found to be 1.5 and 9 msec at 300 and 77°K, respectively. The absorption spectrum of the 2 E state had four wide absorption bands with maxima at 16,700, 23,300, 28,600, and 40,500 cm –1 . The theoretical energy level scheme of Cr 3+ was calculated for Dq = 1725 cm –1 , G = 640 cm –1 , C = 3200 cm –1 , v = 495 cm –1 , and v' = 259 cm –1 , making an allowance for the mixing of the Γ trig S states. The experimentally observed absorption bands were attributed to specific transitions and the theoretical and experimental intensities were compared.
The absorption cross sections of the Cr3+{\mathrm{Cr}}^{3+}Cr3+ ion in the metastable states 2E(E‾and2A‾)^{2}E (\overline{E} \mathrm{and} 2\overline{A})2E(Eand2A) of lightly doped ruby (\ensuremath{\sim}0.01%) have been measured as a function of polarization at temperatures of 30, 105, and 296\ifmmode^\circ\else\textdegree\fi{}K in the region from 2300 to 7000 \AA{}. The lifetime of these states was measured by observing the decay rate of the excited-state absorption, and agreed with the value of the measured fluorescence decay rate at various temperatures. The population of the excited states was measured by the change of the area under the first two vibronic sidebands at low temperatures. At room temperature the population was measured by the change of transmitted intensity of a ruby laser.
This paper investigates the differential absorption spectra of a number of transparent spinel-based cobalt-containing aluminosilicate glass-ceramics in the 550-700-nm range. A stimulated emission band accompanying transitions between the 4T1(4P) and 4A2 levels of the tetracoordinated Co2+ ion is detected in all the materials. Depending on the composition of the glass-ceramic, the effective stimulated-emission cross sections of the Co2+ ions at the maximum of this band are estimated at (4-5)×10−19 cm2.
Absorption cross sections of Cr3+in the metastable2E states of pink ruby (0.05 percent Cr2O3) have been measured forE \perp Cbetween 4000 Å and 7000 Å at 297°K and 115°K. Both 0 degree and 90 degree ruby rods were measured in a flash absorption apparatus having a spectral resolution of 50 Å. The broad excited state absorption bands centered at 5600 Å appear to correlate with the positions of2T1(3T1) level, while the narrow band centered at 4540 Å correlates well with the predicted2A2(1E) level. The effect of excited state absorption on laser operation is discussed in this paper.
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.
We describe a systematic, rigorous procedure for the determination of the optical absorption saturation parameters for Cr4+:YAG and Cr4+:forsterite crystals at 1064 nm. A rate-equation approach was used to analyze the cw and pulsed transmission data of several crystals by accounting for the transverse as well as longitudinal variation of the beam intensity, saturation effects, and excited-state absorption. Use of an iterative procedure whereby the cw and pulsed data were simultaneously analyzed led to a considerable reduction in the error for the determination of cross sections. The average value of the absorption cross section sigmaa and the normalized excited-state absorption cross section fp=sigmaesa/sigmaa were determined to be 6.13×10−19 cm2 and 0.45, respectively, for Cr4+:forsterite and 19.6×10−19 cm2 and 0.06, respectively, for Cr4+:YAG. Detailed comparison was also made with previous saturation measurements in the literature. Our results further show that lumped models based on the thin-length approximation should be used with caution in the determination of cross sections, especially when the pump beam is tightly focused inside the absorber.