The pressure-induced phase transition in CdS was investigated using picosecond time-resolved electronic spectroscopy in plate impact shock wave experiments. Real-time changes in the electronic spectra were observed, with 100 ps time resolution, in single crystals of CdS shocked along thecandaaxes to peak stresses between 35 and 90 kbar (above the phase transition stress of approximately 30 kbar measured in continuum studies). When shocked to stresses above approximately 50 kbar along the crystalcaxis and 60 to 70 kbar along the crystalaaxis, the crystals undergo a very rapid change in electronic structure, indicating that significant structural changes occur within the first 100 ps. These results, along with previous ns continuum measurements, make a strong case for a metastable state during the phase transition in shocked CdS.Ab-initioperiodic Hartree-Fock calculations (with DFT correlation corrections) were employed to examine the compression of CdS and to determine a possible lattice structure for the proposed metastable structure. These results, along with details of the transformation kinetics and orientational dependence, will be discussed. Work supported by ONR. ©2000 American Institute of Physics.