Photoluminescence color stability of green-emitting InP/ZnS core/shell quantum dots embedded in silica prepared via hydrophobic routes

Abstract

In this work, green-emitting InP/ZnS quantum dots (QDs) modified with 1-dodecanethiol were embedded into silica by two methods to improve their photostability while maintaining a high photoluminescence quantum yield (PLQY) and a color coordinate. A monolithic QD-silica composite prepared by a non-aqueous route with tetraethyl orthosilicate and lactic acid featured low transparency, a loss of the color purity of green, and a PLQY of 1.6%, which was considerably lower than that of the original QDs (67%). The decrease of the PLQY was attributed to QD aggregation in the sol–gel process and degradation of the QDs by the acid. The alternative method involved stirring a toluene dispersion of the QDs with tetramethyl orthosilicate (TMOS) for 20 h or 7 days. The PLQY of the TMOS-modified InP/ZnS QDs (20 h) was 62%, which was only slightly lower than that of the original QDs. The PLQY decreased to 52% when the duration of aging was prolonged to 7 days. This decrease was attributed to desorption of surface modifiers from the QD surface and oxidative degradation by oxygen dissolved in toluene. Herein, the color coordinate was maintained stably. Photostability was evaluated by continuous irradiation of the samples by a blue light emitting diode. The decrease of photoluminescence (PL) intensity was suppressed by the silica encapsulation. In particular, the PL intensity of the TMOS-modified InP/ZnS QD sample (7 d) maintained 99% of its initial intensity. Silica encapsulation of InP/ZnS QDs prevented contact of the QDs with oxygen in the air, resulting in improved photostability.