Solid-structured phosphine sulfide as a new precursor in the synthesis of mercury sulfide quantum dots

IF 5.45 Q1 Physics and Astronomy Nano-Structures & Nano-Objects Pub Date : 2024-06-19 DOI:10.1016/j.nanoso.2024.101238
Alaa A. Mardini , Ivan A. Shuklov , Anna A. Lizunova , Vladimir F. Razumov
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Abstract

Tricyclohexylphosphine sulfide (Cy)3PS, a solid-structured phosphine sulfide precursor, was used for the first time in the synthesis of sphere-shaped colloidally stable β-HgS CQDs. DFT calculations applying the TPSS-D3/def2-TZVP level of theory in the gas phase showed that the chemical reactivity of the titled precursor is similar to that of TOPS. The nanocrystals produced using HgCl2/(Cy)3PS/THF were colloidally stable, possessing near- and mid-infrared absorptions. As the reaction time increased, the first excitonic peaks were redshifted in the near-infrared window between 0.8 and 1.1 µm. Meanwhile, the red shifting of the mid-wavelength intraband (1Se‐1Pe) absorption peaks was between 3.9 and 4.8 µm. A good agreement between the diameters calculated using the atomistic tight-binding approach and those obtained using TEM was observed. The concentration and molar absorption coefficient (ε400) of the prepared QDs were determined as well. An increase in the ε400 of the quantum dots with increasing reaction time was shown. XPS elemental analysis showed that HgS NCs with a nearly equal atomic ratio of Hg:S were poorly colloidally stable, and their FT-IR spectra had no intraband absorptions in the mid-IR window. Meanwhile, high colloidally stable and mid-wavelength intraband absorption peaks in the FT-IR spectra were shown for mercury-rich HgS CQDs.

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固体结构硫化膦作为合成硫化汞量子点的新前体
三环己基硫化膦(Cy)3PS 是一种固体结构的硫化膦前驱体,被首次用于合成球形胶体稳定的 β-HgS CQDs。在气相中应用 TPSS-D3/def2-TZVP 理论水平进行的 DFT 计算表明,该前驱体的化学反应活性与 TOPS 相似。使用 HgCl2/(Cy)3PS/THF制备的纳米晶体具有胶体稳定性,具有近红外和中红外吸收。随着反应时间的延长,第一个激发峰在 0.8 至 1.1 µm 的近红外窗口发生了红移。同时,中波带内(1Se-1Pe)吸收峰的红移在 3.9 至 4.8 微米之间。使用原子紧密结合方法计算出的直径与使用 TEM 获得的直径之间具有良好的一致性。还测定了制备的 QDs 的浓度和摩尔吸收系数(ε400)。结果表明,量子点的ε400 随反应时间的延长而增大。XPS 元素分析表明,Hg:S 原子比接近相等的 HgS NCs 的胶体稳定性较差,其傅立叶变换红外光谱在中红外窗口没有带内吸收。而富含汞的 HgS CQDs 的傅立叶变换红外光谱则显示出较高的胶体稳定性和中波带内吸收峰。
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来源期刊
Nano-Structures & Nano-Objects
Nano-Structures & Nano-Objects Physics and Astronomy-Condensed Matter Physics
CiteScore
9.20
自引率
0.00%
发文量
60
审稿时长
22 days
期刊介绍: Nano-Structures & Nano-Objects is a new journal devoted to all aspects of the synthesis and the properties of this new flourishing domain. The journal is devoted to novel architectures at the nano-level with an emphasis on new synthesis and characterization methods. The journal is focused on the objects rather than on their applications. However, the research for new applications of original nano-structures & nano-objects in various fields such as nano-electronics, energy conversion, catalysis, drug delivery and nano-medicine is also welcome. The scope of Nano-Structures & Nano-Objects involves: -Metal and alloy nanoparticles with complex nanostructures such as shape control, core-shell and dumbells -Oxide nanoparticles and nanostructures, with complex oxide/metal, oxide/surface and oxide /organic interfaces -Inorganic semi-conducting nanoparticles (quantum dots) with an emphasis on new phases, structures, shapes and complexity -Nanostructures involving molecular inorganic species such as nanoparticles of coordination compounds, molecular magnets, spin transition nanoparticles etc. or organic nano-objects, in particular for molecular electronics -Nanostructured materials such as nano-MOFs and nano-zeolites -Hetero-junctions between molecules and nano-objects, between different nano-objects & nanostructures or between nano-objects & nanostructures and surfaces -Methods of characterization specific of the nano size or adapted for the nano size such as X-ray and neutron scattering, light scattering, NMR, Raman, Plasmonics, near field microscopies, various TEM and SEM techniques, magnetic studies, etc .
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