Linear and nonlinear optical properties of CdSexS1−x microcrystallites

Microcrystals of CdSe_xS_1−x (x≈0.6) with nanometer dimensions have been investigated experimentally by a range of optical techniques. This system of ‘quantum dot’ consists of nanometer sized semiconductor particles embedded within an insulating glass matrix. The existence of microscopic CdSeS crystals within the glass matrix is demonstrated by the observation of Raman scattering from the ‘CdSe-like’ and ‘CdS-like’ LO phonons. The nature of the electronic states within these three dimensionally confined systems is investigated by linear absorption and photoluminescence spectroscopy. The photoluminescence spectra show features which are attributed to direct electron-hole recombination and recombination via states within the ‘blue shifted’ energy gap (which are possibly surface related). Carrier relaxation is also investigated by a pump-probe experiment whereby the absorption is partially bleached by a short pump pulse then probed some variable time later by a delayed probe pulse of much lower intensity. Fast and slow components in the carrier relaxation process are identified, and a relationship is suggested between the carrier relaxation and the features observed in the photoluminescence spectra. The well known ‘photodarkening’ properties of such materials are also investigated by the above techniques.