Evolution of Local Structural Motifs in Colloidal Quantum Dot Semiconductor Nanocrystals Leading to Nanofaceting.
Evolution of Local Structural Motifs in Colloidal Quantum Dot Semiconductor Nanocrystals Leading to Nanofaceting.
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DOI：
10.1021/acs.nanolett.2c04851
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发表时间：
2023-03-22
期刊：
影响因子：
10.8
通讯作者：
Kim, Jong Min
中科院分区：
文献类型：
--
作者：
Hou, Bo;Mocanu, Felix Cosmin;Cho, Yuljae;Lim, Jongchul;Feng, Jiangtao;Zhang, Jingchao;Hong, John;Pak, Sangyeon;Park, Jong Bae;Lee, Young-Woo;Lee, Juwon;Kim, Byung-Sung;Morris, Stephen M.;Sohn, Jung Inn;Cha, SeungNam;Kim, Jong Min
胶体纳米晶体（NCs）在光电子学、能量收集、光子学和生物医学成像方面展现出了显著的应用前景。除了优化量子限域之外，当前的挑战是更好地理解关键的加工步骤以及它们对结构基序演变的影响。本研究中呈现的计算模拟和电子显微镜结果表明，在极性溶剂中的贫铅环境下合成纳米晶体时可能会发生纳米刻面现象。这可以解释在采用这些条件时实验中观察到的弯曲界面和橄榄状纳米晶体。此外，硫化铅纳米晶体固体薄膜的润湿性可通过化学计量控制进一步改变，这会影响界面能带弯曲，进而影响诸如多结沉积和粒子间外延生长等过程。我们的研究结果表明，当用于调节能带结构时，纳米晶体中的纳米刻面现象可成为一种固有优势，这是传统块状晶体所无法实现的。
Colloidal nanocrystals (NCs) have shown remarkable promise for optoelectronics, energy harvesting, photonics, and biomedical imaging. In addition to optimizing quantum confinement, the current challenge is to obtain a better understanding of the critical processing steps and their influence on the evolution of structural motifs. Computational simulations and electron microscopy presented in this work show that nanofaceting can occur during nanocrystal synthesis from a Pb-poor environment in a polar solvent. This could explain the curved interfaces and the olivelike-shaped NCs observed experimentally when these conditions are employed. Furthermore, the wettability of the PbS NCs solid film can be further modified via stoichiometry control, which impacts the interface band bending and, therefore, processes such as multiple junction deposition and interparticle epitaxial growth. Our results suggest that nanofaceting in NCs can become an inherent advantage when used to modulate band structures beyond what is traditionally possible in bulk crystals.
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