journal article·2025-11Open access

Tunable photoluminescence in stoichiometric tetragonal AgInS2 quantum dots: Effect of sulfur injection temperature

Sandhuli S. Hettiarachchi Dehigaspitiya, Jonghoon Han, Aarti Aarti, Long Hu, Guozheng Shi, Chao Shen, Robert John Patterson, Jincheol Kim, Koushik Venkatesan, David Neil Roger Payne, Binesh Puthen Veettil, Shujuan Huang

Abstract

Achieving high photoluminescence quantum yield (PLQY) in stoichiometric, heavy metal-free AgInS 2 quantum dots (QDs) remains a significant challenge, primarily due to the persistent formation of phase impurities during synthesis. In this study, we addressed this limitation by incorporating 1-dodecanethiol (DDT) as a coordinating ligand in both cationic and anionic precursors. This approach allowed for precise control over precursor reactivity, ultimately enabling the synthesis of phase-pure, stoichiometric tetragonal AgInS 2 QDs. Systematic variation of sulfur injection temperatures revealed its critical role in tuning QD size (3.2–6.3 nm), optical properties, and defect states. An optimum sulfur injection temperature of 180 °C resulted in a maximum PLQY of 66 %, among the highest reported PLQY for stoichiometric tetragonal AgInS 2 QDs synthesized via the hot injection method. The QDs exhibited size-tunable emission across 581.6–745.6 nm and large Stokes shifts of up to 210 nm. Time-resolved photoluminescence and temperature-dependent studies revealed defect-mediated donor–acceptor pair (DAP) recombination dynamics, with average lifetimes reaching 836 ns at optimal synthesis conditions. A size–bandgap relationship was established using both empirical fitting and effective mass approximation (EMA). This work provides new insights into the synthesis of stoichiometric tetragonal AgInS 2 QDs and establishes a synthetically accessible, reproducible route towards heavy metal-free QDs for advanced optoelectronic applications.
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Research context

OpenAlex topics: Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films · Chemical and Physical Properties of Materials

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