Nonradiative relaxation in tunable solid state laser crystals

The characteristics of nonradiative transitions between the 4T2 and 2E excited states of trivalent-chromium-ion-activated ruby (containing 0.04 percent Cr2O3 by weight) and alexandrite (containing 0.4 at. percent chromium ion) laser crystals were studied using the technique described by Gayen et al. (1985). In this technique, a 527-nm pulse excites the 4T2 band of the Cr(3+), and the subsequent population kinetics among excited states is monitored by an IR picosecond probe pulse as a function of pump-probe delay. In ruby, a resolution-limited sharp rise in the excited state population was followed by a long-lifetime decay, leading to an upper limit of 7 ps for the 4T2-state nonradiative lifetime. In alexandrite, a longer rise time was followed by a multicomponent decay. A theoretical model is proposed for explaining the induced absorption and the transition dynamics observed in these crystals.