KrF excimer laser irradiation of CdTe at fluences below the melt threshold (≤75 mJ/cm2) removes surface layers and produces reversible changes in the surface composition that depend upon the laser fluence and number of laser pulses delivered to the surface. At fluences above ∼40 mJ/cm2 a Te-rich layer is obtained. A stoichiometric composition can be restored by irradiation at reduced laser fluence. The primary desorption products are Cd and Te2, and the velocities of these species are well described by a Maxwellian distribution. The fluence-dependent changes in CdTe surface composition are consistent with a photothermal mechanism based on the competition between formation and desorption of Te2 and desorption of Cd atoms from the laser-irradiated surface.