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The strength of electrostatic interactions (EI) between electrons and holeswithin semiconductor nanocrystals profoundly impact the performance of theiroptoelectronic systems, and different optoelectronic devices demand distinct EIstrength of the active medium. However, achieving a broad range, fine-tuning ofthe EI strength for specific optoelectronic applications is a dauntingchallenge, especially in quasi 2-dimensional core-shell semiconductornanoplatelets (NPLs), as the epitaxial growth of the inorganic shell along thedirection of the thickness that solely contributes to the quantum confinedeffect significantly undermines the strength of the EI. Herein we propose anddemonstrate a novel doubly-gradient (DG) core-shell architecture ofsemiconductor NPLs for on-demand tailoring of the EI strength by controllingthe localized exciton concentration via in-plane architectural modulation,demonstrated by a wide tuning of radiative recombination rate and excitonbinding energy. Moreover, these exciton-concentration-engineered DG NPLs alsoexhibit a near-unity quantum yield, remarkable thermal and photo stability, aswell as considerably suppressed self-absorption. As proof-of-conceptdemonstrations, highly efficient color converters and high-performancelight-emitting diodes (external quantum efficiency: 16.9%, maximum luminance:43,000 cd/m2) have been achieved based on the DG NPLs. This work thus opens upnew avenues for developing high-performance colloidal optoelectronic deviceapplications.

Near-Unity Emitting, Widely Tailorable and Stable Exciton Concentrators Built from Doubly Gradient 2D Semiconductor Nanoplatelets