INTRODUCTIONTransition-metal-on-doped chalcogenides, because of their absorption and luminescence properties, have particularly attracted investigators as a new class of gain media in broadly tunable mid-infrared (IR) solid-state lasers. Several different tetrahedrally coordinated II-VI compounds have served as hosts for Cr 2ϩ . Room-temperature lasing action has been demonstrated for Cr 2ϩ :ZnSe, 1,2 Cr 2ϩ :ZnS, 1 Cr 2ϩ :Cd 0.85 Mn 0.15 Te, 3 and Cr 2ϩ :CdSe. 4 Chromium can be incorporated in the host material during the growth process or by postgrowth diffusion. It substitutes for the cation and can exist in several charge states. 5,6 The Cr 2ϩ has a [Ar]3d 4 electronic configuration; in a tetrahedral substitutional configuration, the four 3d electrons participate in a tetrahedral coordination of Cr 2ϩ to its nearest-anion neighbors, yielding a neutral chargestate for Cr 2ϩ in II-VI materials. A tetrahedral-crystal field of T d symmetry splits the ground state, 5 D, of the free Cr 2ϩ ion into an excited state, 5 E, and a ground state, 5 T 2 . A Jahn-Teller distortion induces a splitting of each of these states. 7-10 Laser operations occur by mainly Cr 2ϩ intracenter absorption and emission transitions between the 5 T 2 and 5 E multiplets, without any change for the charge state of Cr 2ϩ . The lack of inversion symmetry of the tetrahedral sites is responsible for high absorption and emission cross sections reported, as well as the higher rates of radiative emission of Cr 2ϩ compared to nonradiative decay. 1,4,7,11 The Cr 2ϩ :CdSe has a broad optical-absorption band peaking at 1.9 m and an emission around 2.5 m, which pushes the laser operation further into the mid-IR, compared with the zinc chalcogenides hosts. Cadmium selenide is a hexagonal crystal, exhibiting birefringence, that was used in the past in the construction of IR optical-parametric oscillators (OPO). This opens an exciting new possibility of an integrated mid-IR laser/OPO.A peak-absorption cross section a of 3 ϫ 10 Ϫ18 cm Ϫ2 was estimated by Schepler et al., 12 based on an indirect measurement of the concentration of chromium in one crystal and the consideration of the density of CdSe. They observed an emission broad band in the 1.8-2.8-m spectral region, when pumping at 1.9 m or at 755 nm. Using a 755-nm excitation source (acousto-optically modulated Ti:sapphire), they measured a constant emission lifetime of 6 s from 60-300 K, giving an emissionquantum yield of 100% and bringing the possibility of pumping at 755 nm in a region where solid-stateThe maximum optical-absorption cross section of Cr 2ϩ ions was evaluated from near-infrared (NIR) absorption spectroscopy and direct measurements of the chromium concentration in Cr 2ϩ :CdSe crystals. The emission lifetime of the excited state, 5 E, of Cr 2ϩ was measured as a function of Cr 2ϩ concentration in the 2 ϫ 10 17 -2 ϫ 10 18 ions/cm 3 range and as a function of temperature from 77-300 K. Lifetime values were as high as ϳ6 s in the 77-250 K range and decreased to ϳ4 s at 300 K because of nonradia...