Deciphering Ultrafast Carrier Dynamics of Eco-Friendly ZnSeTe-Based Quantum Dots: Toward High-Quality Blue-Green Emitters.

Abstract

Developing non-toxic and high-performance colloidal semiconductor quantum dots (CQDs) represents the inevitable route toward CQD-enabled technologies. Herein, the spectral and dynamic properties of heavy-metal-free ZnSeTe-based CQDs are investigated by transient absorption spectroscopy and theoretical modeling. We for the first time decode the ultrafast hot carrier trapping (<2 ps) and band-edge carrier trapping processes (∼6 ps) in the CQD system, which plagues the emission performance. The ZnSe/ZnSeS/ZnS shell engineering greatly suppresses the non-radiative trapping process and results in a high photoluminescence quantum yield of 88%. We demonstrate that the core/shell nano-heterostructure forms the quasi-type II configuration, in contrast to the presumed type I counterpart. Moreover, the Auger recombination and hot carrier cooling processes are revealed to be ∼454-405 ps and 160-370 fs, respectively, and their relationship with the composition in the spectral range of 470-525 nm is clarified. The above merits render these ZnSeTe CQDs as outstanding blue-green emitters for optoelectronic applications, exemplified by the white light-emitting diodes.