The optical absorption, luminescence, luminescence excitation, and luminescence decay kinetics of a dopant with a 3d3 shell (most probably Cr3+) and V3+ ions in natural Ca2Al3Si3O12(OH) zoisite crystal have been measured. The splitting of the R lines for a dopant with a 3d3 shell, equal to 340 cm-1, is one of the largest known. The very broad infrared luminescence spectrum is associated with various dopants present in the crystal. We show that possible application of zoisite as a laser material is hindered by efficient nonradiative transitions at room temperature related to the presence of trace impurities. © 1994 The American Physical Society.