Efficient Band-Edge Emission from Indirect Bandgap Semiconductor Quantum Dots upon Shell Engineering.

Zhai, Jingwen; Dong, Tieshuan; Zhou, Yamei; Min, Jingjing; Yan, Yuli; Garoufalis, Christos S; Baskoutas, Sotirios; Xu, Dangdang et al. · Nano Lett · 2023

basic_science · Level V

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Abstract

Environmentally friendly colloidal quantum dots (QDs) of groups III-V are in high demand for next-generation high-performance light-emitting devices for display and lighting, yet many of them (e.g., GaP) suffer from inefficient band-edge emission due to the indirect bandgap nature of their parent materials. Herein, we theoretically demonstrate that efficient band-edge emission can be activated at a critical tensile strain γ<sub>c</sub> enabled by the capping shell when forming a core/shell architecture. Before γ<sub>c</sub> is reached, the emission edge is dominated by dense low-intensity exciton states with a vanishing oscillator strength and a long radiative lifetime. After γ<sub>c</sub> is crossed, the emission edge is dominated by high-intensity bright exciton states with a large oscillator strength and a radiative lifetime that is shorter by a few orders of magnitude. This work provides a novel strategy for realizing efficient band-edge emission of indirect semiconductor QDs via shell engineering, which is potentially implemented employing the well-established colloidal QD synthesis technique.