Rational synthesis of core/shell heterostructured quantum dots for improved self-powered photodetection performance enabled by energy band engineering

Abstract

Colloidal quantum dots (CQDs), especially core-shell QDs, have attracted dramatic interests as emerging materials in optoelectronic devices due to their size tuneable band-gap, high absorption coefficient, facile and low-cost synthesis routing, etc. However, the precise design of core/shell band engineering along with charge carrier transfer efficiency are still challenging, inevitably impacting the performance of optoelectronic devices. Herein, three different types of CdSe/CdS core-shell heterostructured QDs have been obtained via a proposed synthesis strategy of adjusting the core size but fixing the shell thickness. The performance of the core-shell QDs based self-powered photodetectors can be efficiently regulated by the optimization of synthesis strategy with the design of energy band alignment. Compared to the quasi type-II and the type-I QDs devices, the Ilight/Idark ratio of type-II heterostructure based photodetector is increased by ∼2 and ∼5 orders of magnitude, respectively. The champion device exhibits extraordinary optoelectronic performance in terms of ultrahigh light-to-dark current ratio of 105, photoresponsivity of 10.64 mA/W, at bias of 0 V, respectively. The charge carrier dynamics and transfer mechanisms of the QDs were further investigated, revealing the improved carrier separation and transportation efficiency induced by a strong build-in electric field in type-II CdSe/CdS core-shell heterostructure. This work provides a new strategy for the next-generation self-powered QDs optoelectronics enabled by the proposed synthesis approach along with the design of energy band alignment.