Spontaneous and stimulated emission dynamics of PbS quantum dots in a glass matrix

Abstract

Optical properties and relaxation mechanisms of PbS quantum dots in glass matrix (PbS:Glass) have been systematically investigated by transmission and (steady-state and transient) photoluminescence spectroscopy. Key parameters are determined by combining the data with semiempirical expressions, based on which the recombination mechanisms including spontaneous and stimulated emissions have been discussed as a function of temperature by referring to a multilevel model including intrinsic (or band-to-band transition), bright, dark, and ground states. The results disclose that (i) the existence of a dark exciton state is the main reason for thermal quenching of the emission even at low temperatures due to the strong multiacoustic phonon coupling, (ii) the ``intrinsic'' spontaneous emission related to the intrinsic state is observed with an approximately nanosecond lifetime, in contrast to the ``regular'' spontaneous emission from the bright exciton state with an approximately microsecond lifetime, and (iii) stimulated emission, which has a lifetime of 20--40 ps and shows power-dependence of excitation density (or temperature), only appears from the intrinsic state but not the (bright) exciton state when enough accumulation of photogenerated carriers is reached. Furthermore, we find that the thermal conductivity will become crucial for future PbS:Glass related optoelectronic device applications.