Suppressing Tail Emission from AgIn<sub>1-<i>x</i></sub>Ga<sub><i>x</i></sub>S<sub>2</sub>/AgGaS<sub>2</sub> Quantum Dots by GaI<sub>3</sub>-Assisted Interface Reinforcement.

Park, Seongkyung; Kim, Byong Jae; Jung, Woon Ho; Lee, Kang Hyun; Lee, Hyeonjun; Lim, Jaehoon · ACS Nano · 2025

basic_science · Level V

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Abstract

Heteroepitaxy of AgGaS<sub>2</sub> (AGS) or GaS<sub><i>x</i></sub> shells on AgIn<sub>1-<i>x</i></sub>Ga<sub><i>x</i></sub>S<sub>2</sub> (AIGS) quantum dots (QDs) enables narrow band-edge emission with a near-unity photoluminescence quantum yield (QY). While this outcome is attributed to the passivation of donor-acceptor pair states on the surface, persistent tail emission, regardless of the QY, implies underlying interfacial defects in the AIGS/AGS QDs. Herein, we identify the latent compositional and crystallographic disorder at the core-shell interface originating from the surface instability of AIGS QDs. The strong coordination of oleylamine to group III cations promotes partial dissolution of the AIGS cores, resulting in a Ga-deficient, structurally disordered phase that contains interfacial donor states that are thermally mixed with the band-edge electron state. The incorporation of GaI<sub>3</sub> weakens the coordination of oleylamine to cations at the surface and in the dissolution products, thereby suppressing the disorder by fostering a Ga-rich environment. The suppressed tail emission, even at 80 K, highlights the importance of surface stabilization in eliminating the interfacial defects.