Publication date: 28th August 2024
Indium phosphide (InP)-based quantum dots (QDs) are the most industrially relevant Cd- and Pb-free QDs for photonic applications due to their excellent optoelectronic properties, including a tunable band gap, tolerance to dopants, high absorption coefficients, near-unity photoluminescent (PL) quantum yields (QYs), and narrow PL linewidths.[1] In recent years, research efforts have successfully improved the quality of InP-based QDs.[1] However, their long-term stability and the deterioration of their optoelectronic properties are not yet well understood. In this work, we systematically investigate how the optoelectronic properties of colloidal InP/ZnSe/ZnS core/shell QDs in solution are affected by continuous white LED light exposure under a nitrogen atmosphere (< 0.1 ppm O2, < 0.1 ppm H2O).
Characterization of the absorption spectrum over time shows that the QDs are colloidally stable in solution and do not photodegrade. Remarkably, the PLQY of the InP/ZnSe/ZnS QDs decreased rapidly over time and did not recover after light exposure, indicating irreversible photodarkening of the QDs. A control experiment conducted in the dark demonstrated no degradation of the QDs or reduction in their PLQY throughout the duration of the experiment. The photodarkening effect was mitigated by reducing the incoming photon flux. However, when the changes in QY are plotted against the absorbed photon dose, the data collapses in a master curve with a logarithmic dependence on the dose. These ensemble-level results are further complemented by single-particle measurements for a comprehensive interpretation. In summary, our findings provide new insights into the photodarkening of InP-based core/shell QDs relevant for photonic applications.