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Soviet Journal of Quantum Electronics

OPTICAL ABSORPTION SPECTRUM OF EXCITED Cr3+IONS IN YTTRIUM ALUMINUM GARNET

B. K. Sevast’yanov, D. T. Sviridov, V. P. Orekhova, L B Pasternak, R. K. Sviridova, T. F. Veremeĭchik

Published Apr 30, 1973• 13 citations
Publisher

Abstract

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.

DOI
10.1070/qe1973v002n04abeh004456

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Quantum Electronics•Nov 30, 1996•4 citations
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 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.
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 spectra of luminescence and magnetic circular polarization of luminescence in the 1 D 2 → 3 F 4 emission band in thulium:yttrium-aluminum garnet Tm3+:YAG (Tm3+:Y3Al5O12) have been investigated at temperatures T = 78 and 293 K, respectively. Based on the analysis of the magnetooptical and optical spectra, the optical transitions between the Stark sublevels of the 3 F 4 and 1 D 2 multiplets in Tm3+:YAG were identified. It is shown that the symmetry and energies of the Stark sublevels of the 3 F 4, 1 D 2, and 3 H 6 multiplets, found experimentally from magnetic and magnetooptical studies, confirm the results of theoretical calculations of the energy spectrum of the rare earth Tm3+ ion in YAG.
An experimental study of saturable absorption and excited-state absorption (ESA) in several inorganic saturable absorbers, Cr/sup 4+/:YAG, Cr/sup 4+/:GGG, and Cr/sup 4+/:YSGG, is presented. We provide the theoretical background of absorption characteristics in saturable absorbers that exhibit ESA, with some new results: approximate analytical solutions are proposed for the optical transmission in the case of a slow absorber, and for various light intensity conditions of spatially or temporally Gaussian beams in fast and slow absorbers. Experimentally, partial bleaching of the first excited state itself could be observed in Cr/sup 4+/:YAG at /spl lambda/=1064 nm, yielding the higher excited-state lifetime as /spl tau/*=(0.55/spl plusmn/0.1) ns. The regular transmission bleaching curve was measured in Cr/sup 4+/:GGG, for the first time in this material, yielding /spl sigma//sub ga/=(58/spl plusmn/5)/spl times/10/sup -1/ cm/sup 2/, and /spl sigma/e/sub s/=(13/spl plusmn/2)/spl times/10/sup -19/ cm/sup 2/ at /spl lambda/=1064 nm, ESA spectra were measured for the three materials between /spl sim/700 and 900 nm. All three exhibit crossing between saturable absorption at longer wavelengths and inverse saturable absorption at shorter wavelengths.
The differential absorption spectra of an V 3+ :Y 3 Al 5 O 12 crystal were investigated by a picosecond pump-and-probe method. An analysis of the results led to the conclusion that the induced absorption bands observed in the 850–890 and 650–770 nm ranges were due to, respectively, the 1 E ( 1 D )→ 1 T 1 ( 1 G ) and 1 E ( 1 D )→ 1 E ( 1 G ), 1 T 2 ( 1 G ) transitions in a tetrahedrally coordinated V 3+ ion. The lifetime of the 1 E ( 1 D ) level was estimated to be ~ 130 ps. Bleaching of the 3 A 2 → 3 T 1 ( 3 P ) absorption band of the tetrahedral V 3+ ion was also observed.