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Development of Synthetic Methods to Grow Long-Wavelength Infrared-Emitting HgTe Quantum Dots in Dimethylformamide

DOI:10.1021/acs.chemmater.0c00249 期刊:Chemistry of Materials 出版年份:2020 更新时间:2025-09-23 15:19:57
摘要: Most successful syntheses of long wavelength infrared (IR) absorbing/emitting Hg-chalcogenide quantum dots (QDs) use either aqueous or organic solvent-based methods. Accounts of IR QD growth in aprotic solvents such as dimethyl sulfoxide (DMSO) or dimethyl formamide (DMF) are much less common, and yet producing QDs in such solvents can be useful from the perspective of further reactions to conjugate or incorporate the QDs with other materials since such solvents can be a useful meeting ground for both organic and ionic solutes. Here we start by demonstrating long wavelength infrared emission (across the wide spectral range up to 4500 nm) in HgTe QDs grown in DMF under basic conditions. Whilst many existing synthetic approaches use soluble chalcogen precursors in adduct, salt or organo-chalcogenide forms, we have opted to take the approach of using slow addition of gaseous H2Te generated under programmed control, which allowed us to investigate the growth kinetics in order to manipulate the different competing processes, and to obtain larger HgTe QDs with the best size distributions on a repeatable and controlled basis. We demonstrate how the nucleation process of HgTe QDs can be carried out analogously to how it occurs in classic hot injection syntheses, but in our case at a far lower (sub-ambient) temperature owing to the use of a much more labile Te precursor. We also demonstrate the use of a two stage, seeded QD growth process which allows the synthesis conditions for the initial nucleation step and the subsequent enlargement stage to be decoupled, in other words the QD concentration during the enlargement phase need not be forced to be excessively large by the choice of nucleation conditions. This approach should eventually be extendable to making >5000 nm emitting HgTe QD based materials, and the use of aprotic solvents will offer compatibility with other nanomaterial chemistries, e.g. oxide glass formers etc., for the synthesis of composites. By comparing the emission spectra of HgTe QDs grown in DMF with those grown in DMSO, we show that polaron mediated coupling to ligand and solvents, previously seen when using DMSO, can be substantially suppressed using our new synthetic method.
作者: Stephen V. Kershaw,Wai Kin Yiu,Aleksandr Sergeev,Andrey L. Rogach
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Investigating the development of synthetic methods for growing long wavelength infrared emitting HgTe quantum dots in dimethylformamide (DMF) under basic conditions, focusing on controlling growth kinetics and improving size distributions.

The study successfully developed a synthetic method for growing long wavelength infrared emitting HgTe quantum dots in DMF under basic conditions, demonstrating improved control over growth kinetics and size distributions. The use of an organic base was critical in reducing polaron mediated coupling to ligand and solvents, leading to better optical properties. The method offers potential for extending to larger QD sizes and compatibility with other nanomaterial chemistries.

The study faced limitations in terms of colloidal stability at higher temperatures, which was attributed to the thermal stability of the FMT ligand. Additionally, the synthesis of larger QDs (>5000 nm emitting) was not fully explored due to these stability issues.

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