We introduce stoichiometry control within both core and shell regions of InP/ZnSe/ZnS core/shell/shell quantum dots (QDs) to advance their properties drastically, approaching those of state-of-the-art CdSe-based QDs. The resulting QDs possess near-unity photoluminescence quantum yield, monoexponential decay dynamics, narrow line width, and nonblinking at a single-dot level. Quantum-dot light-emitting diodes (QLEDs) with the InP/ZnSe/ZnS core/shell/shell QDs as emitters exhibit a peak external quantum efficiency of 12.2% and a maximum brightness of >10 000 cd m–2, greatly exceeding those of the Cd/Pb-free QLEDs reported in literature. These results pave the way toward Cd/Pb-free QDs as outstanding optical and optoelectronic materials.

CdSe magic-size clusters with close-shell surface and fixed molecular formula are well-known in the size range between ∼1 and 3 nm. By applying high concentration of cadmium alkanoates as ligands, a conventional synthetic system for CdSe nanocrystals was tuned to discriminate completion from initiation of atomic flat facets. This resulted in ∼4-13 nm CdSe nanocrystals with hexahedral shape terminated with low-index facets, namely three (100), one (110), and two (111) facets. These low-symmetry (Cs group with single mirror plane) yet monodisperse hexahedra were found to be persistent not only in a broad size range but also under typical synthetic temperatures for growth of both CdSe and CdS. Atomic motion on the surface of the nanocrystals under enhanced ligand dynamics initiated intraparticle ripening without activating interparticle ripening, which converted the hexahedral nanocrystals to monodisperse spherical ones. This new synthetic strategy rendered optimal color purity of photoluminescence (PL) of the CdSe and CdSe/CdS core/shell nanocrystals, with the ensemble PL peak width comparable with that of a corresponding single dot.

Auger recombination is the main non-radiative decay pathway for multi-carrier states of colloidal quantum dots, which affects performance of most of their optical and optoelectronic applications. Outstanding single-exciton properties of CdSe/CdS core/shell quantum dots enable us to simultaneously study the two basic types of Auger recombination channels—negative trion and positive trion channels. Though Auger rates of positive trion are regarded to be much faster than that of negative trion for II-VI quantum dots in literature, our experiments find the two rates can be inverted for certain core/shell geometries. This is confirmed by theoretical calculations as a result of geometry-dependent dielectric screening. By varying the core/shell geometry, both types of Auger rates can be independently tuned for ~ 1 order of magnitude. Experimental and theoretical findings shed new light on designing quantum dots with necessary Auger recombination characteristics for high-power light-emitting-diodes, lasers, single-molecular tracking, super-resolution microscope, and advanced quantum light sources.

Auger recombination is the main nonradiative process in multicarrier states of high-quality quantum dots (QDs). For the most-studied CdSe/CdS core/shell QDs, we effectively reduce the biexciton Auger rate by enhancing dielectric screening of band-edge carriers via epitaxial growth of additional ZnS shells. Super volume scaling of negative-trion Auger lifetime for CdSe/CdS core/shell QDs is achieved with the outermost ZnS shells. The volume of CdSe/CdS/ZnS QDs can be less than half that of CdSe/CdS QDs with the same negative-trion Auger lifetime. Auger suppression by the ZnS shells is more pronounced for QDs with wave functions of band-edge carriers spreading close to the inorganic–organic interface, such as CdSe/CdS QDs with small cores. A maximum drop of biexciton Auger rate of ∼50% and a maximum enhancement of biexciton emission quantum yield of 75% are achieved. Auger engineering by dielectric screening opens up new opportunities to improve the emission properties of multicarrier states in QDs.