Recently reported colloidal lead halide perovskite quantum dots (QDs) with tunable photoluminescence (PL) wavelengths covering the whole visible spectrum and exceptionally high PL quantum yields (QYs, 50-90%) constitute a new family of functional materials with potential applications in light-harvesting and -emitting devices. By transient absorption spectroscopy, we show that the high PL QYs (∼79%) can be attributed to negligible electron or hole trapping pathways in CsPbBr3 QDs: ∼94% of lowest excitonic states decayed with a single-exponential time constant of 4.5 ± 0.2 ns. Furthermore, excitons in CsPbBr3 QDs can be efficiently dissociated in the presence of electron or hole acceptors. The half-lives of electron transfer (ET) to benzoquinone and subsequent charge recombination are 65 ± 5 ps and 2.6 ± 0.4 ns, respectively. The half-lives for hole transfer (HT) to phenothiazine and the subsequent charge recombination are 49 ± 6 ps and 1.0 ± 0.2 ns, respectively. The lack of electron and hole traps and fast interfacial ET and HT rates are key properties that may enable the development of efficient lead halide perovskite QDs-based light-harvesting and -emitting devices.

Suppression of Auger recombination in colloidal quantum dots (QDs) is important for their many applications, ranging from biological tagging, QD lasing, to solar energy conversion. Although it has been reported that the biexciton Auger recombination time of core/shell QDs can be significantly prolonged compared to core-only QDs, a systematic investigation of their dependence on the shell thickness is lacking. In this work, using CdSe@CdS core/shell QDs as a model system, we investigated the shell thickness dependence of biexciton lifetimes in both type I and quasi-type II QDs, prepared using large and small core sizes, respectively. We observe a strong increase of biexciton lifetime with the shell thickness and a larger saturation volume in quasi-type II CdSe@CdS QDs, compared to type I CdSe@CdS QDs. These trends can be attributed to the different thickness dependences of electron–hole wave function overlaps in these materials, which reflect their different extents of conduction band electron delocalization. Our findings provide further insight for rational design of core/shell QDs with suppressed Auger recombination rates.