Chromium ions tend to diffuse outward during the laser-heated pedestal growth (LHPG) of Y 3 Al 5 O 12 (YAG) crystal fiber, in which the average Cr 4þ ion concentration decreases significantly after each diameter-reduction step. The Cr 4þ ions are replenished using an electron gun to deposit Cr 2 O 3 and divalent-ion oxide (CaO or MgO) on the source rod circumference before LHPG. It was observed that Ca 2þ has better efficiency to diffuse into the source rod more efficiently than Mg 2þ generating fewer defects and stacking faults. By CaO deposition and post growth annealing at 1350 C under an oxygen environment, a 110% increase in Cr 4þ concentration was obtained. The achieved Cr 4þ concentration and the ratio of Cr 4þ to total Cr were 1:76 Â 10 18 cm À3 and 5.5, respectively. The Ca,Cr:YAG crystal fiber can thus be used as an ultra broadband laser material and amplified spontaneous emitter.