The Effect of Light Intensity, Temperature, and Oxygen Pressure on the Photo-Oxidation Rate of Bare PbS Quantum Dots.

The oxidation speed of PbS quantum dots has been a subject of controversy for some time. In this study, we reveal the precise functional form of the oxidation rate constant for bare quantum dots through analysis of their photoluminescence as a function of temperature, oxygen pressure, and excitation-laser intensity. The combined effect of these factors results in a reduced energy barrier that allows the oxidation to proceed at a high rate. Each absorbed photon is found to have a 10(-8) probability of oxidizing a PbS atomic pair. This highlights the importance of photo-excitation on the speed of the oxidation process, even at low illumination conditions. The procedure used here may set up a quantitative standard useful for characterizing the stability of quantum dots coated with ligands/linkers, and to compare different protection schemes in a fair quantitative way.