Ligand Dynamics Time Scales Identify the Surface–Ligand Interactions in Thiocyanate-Capped Cadmium Sulfide Nanocrystals,The Journal of Physical Chemistry Letters

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Ligand Dynamics Time Scales Identify the Surface–Ligand Interactions in Thiocyanate-Capped Cadmium Sulfide Nanocrystals
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2022-03-30 , DOI: 10.1021/acs.jpclett.2c00493
Samadhan H Deshmukh _{1,

2} , Srijan Chatterjee _{1,

2} , Deborin Ghosh ₁ , Sayan Bagchi _{1,

2}

Affiliation

The nanocrystal surface, which acts as an interface between the semiconductor lattice and the capping ligands, plays a significant role in the attractive photophysical properties of semiconductor nanocrystals for use in a wide range of applications. Replacing the long-chain organic ligands with short inorganic variants improves the conductivity and carrier mobility of nanocrystal-based devices. However, our current understanding of the interactions between the inorganic ligands and the nanocrystals is obscure due to the lack of experiments to directly probe the inorganic ligands. Herein, using two-dimensional infrared spectroscopy, we show that the variations in the inorganic ligand dynamics within the heterogeneous nanocrystal ensemble can identify the diversities in the inorganic ligand–nanocrystal interactions. The ligand dynamics time scale in SCN^– capped CdS nanocrystals identifies three distinct ligand populations and provides molecular insight into the nanocrystal surface. Our results demonstrate that the SCN^– ligands engage in a dynamic equilibrium and stabilize the nanocrystals by neutralizing the surface charges through both direct binding and electrostatic interaction.

中文翻译：

配体动力学时间尺度识别硫氰酸盐封端的硫化镉纳米晶体中的表面配体相互作用

纳米晶体表面充当半导体晶格和封端配体之间的界面，在用于广泛应用的半导体纳米晶体的有吸引力的光物理性质中起着重要作用。用短的无机变体代替长链有机配体提高了基于纳米晶体的器件的导电性和载流子迁移率。然而，由于缺乏直接探测无机配体的实验，我们目前对无机配体和纳米晶体之间相互作用的理解是模糊的。在这里，使用二维红外光谱，我们表明异质纳米晶体集合中无机配体动力学的变化可以识别无机配体-纳米晶体相互作用的多样性。^–加帽的 CdS 纳米晶体可识别三种不同的配体群，并提供对纳米晶体表面的分子洞察。我们的结果表明，SCN ^-配体通过直接结合和静电相互作用中和表面电荷，参与动态平衡并稳定纳米晶体。

更新日期：2022-03-30

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