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Pushing up the Size Limit of Metal Chalcogenide Supertetrahedral Nanocluster
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-01-16 , DOI: 10.1021/jacs.7b12092
Xiaofan Xu 1 , Wei Wang 1 , Dongliang Liu 1 , Dandan Hu 1 , Tao Wu 1 , Xianhui Bu 2 , Pingyun Feng 3
Affiliation  

The cubic ZnS structure type and the size-dependent properties of related nanoparticles are of both fundamental and technological importance. Yet, it remains a challenge to synthesize large atom-precise clusters of this structure type. Currently, only supertetrahedral clusters with 4, 10, 20, and 35 metal sites (denoted as T2, T3, T4, and T5, respectively) are known. Because the synthesis of T5 in 2002, numerous synthetic efforts targeting larger clusters only resulted in T2-T5 clusters in various compositions and intercluster connectivity, with T6 (56 metal and 84 anion sites) being elusive. Here, we report the so-far largest supertetrahedral cluster (T6, [Zn25In31S84]25-). New T6 clusters can serve as the host matrix for optically active centers. Mn-doped variants of T4 and T6 have also been made, allowing the investigation of site-dependent Mn emission. The results lead to the elucidation of the mechanism regulating Mn emission via size-dependent crystal lattice strain and provide new insight into Mn-doping chemistry in cluster-based chalcogenides at the atomic level.

中文翻译:

提高金属硫属化物超四面体纳米团簇的尺寸极限

立方 ZnS 结构类型和相关纳米粒子的尺寸相关特性具有基础和技术重要性。然而,合成这种结构类型的大原子精确簇仍然是一个挑战。目前,只有具有 4、10、20 和 35 个金属位点(分别表示为 T2、T3、T4 和 T5)的超四面体簇是已知的。由于 2002 年 T5 的合成,许多针对较大簇的合成努力仅导致 T2-T5 簇具有不同的组成和簇间连接,而 T6(56 个金属和 84 个阴离子位点)难以捉摸。在这里,我们报告了迄今为止最大的超四面体簇(T6,[Zn25In31S84]25-)。新的 T6 簇可以作为光学活性中心的宿主矩阵。还制造了 T4 和 T6 的 Mn 掺杂变体,允许调查与场地有关的 Mn 排放。结果导致阐明了通过尺寸依赖性晶格应变调节 Mn 发射的机制,并在原子水平上提供了对基于簇的硫属元素化物中 Mn 掺杂化学的新见解。
更新日期:2018-01-16
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