Time resolved surface second harmonic generation has been used to probe the photoreduction kinetics of malachite green adsorbed onto single crystal cadmium sulfide. A detailed analysis is presented of how the adsorbates and the noncentrosymmetric substrate contribute separately to the total second harmonic signal. Conditions under which the adsorbates can be cleanly detected are described. To complement kinetic measurements of adsorbate reduction, the time evolution of conduction band carriers was determined using sum frequency up conversion of the recombination luminescence. In addition, the formation and decay of surface trapped carriers was monitored using near infrared transient absorption. Comparing the time scale for photoreduction with the relaxation kinetics of mobile and trapped charge carriers indicates that short lived mobile carriers rather than longer lived surface trapped carriers dominate interfacial charge transfer in this system.