The ArF laser sputtering of calcium hydroxide, strontium hydroxide, and sucrose crystals is studied by laser induced fluorescnce (LIF) and LIF time of flight (TOF) techniques under vacuum conditions. Studied using LIF for these three materials, at several fluences (0.83, 1.7, and 2.2 J /cm2) and probe distance (0.4, 0.8, 1.2, 1.5, and 2.1 cm) yield an average rotational temperature of 560±16 K from the first six rotational states for the Q1, R1, R2, and Q2 lines. No rotational cooling was observed as a function of distance. The translational temperature analysis by LIF-TOF indicates that the process can be represented by a fast and slow component.