Heterometal doping is a promising avenue toward tailoring properties of ligand-protected metal nanoclusters for specific applications. Though successful doping has been demonstrated in several structures, the underlying reasons for the dopant preference on occupying specific locations on the nanocluster with different concentrations remain unclear. In this study we apply our thermodynamic stability model, originally developed for ligand-protected monometallic nanoclusters, to rationalize the synthetic accessibility, dopant location, and concentrations of various heterometals on ligand-protected Au nanoclusters. Importantly, we demonstrate that the thermodynamic stability theory is a significant step forward in accurately describing doping effects on nanoclusters using first-principles calculations. With our computational predictions being in excellent agreement with a series of experiments, we introduce the thermodynamic stability theory as a new method for bimetallic nanocluster prediction.

中文翻译：

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对配体保护的金属纳米团簇中的杂金属掺杂的反思

杂金属掺杂是针对特定应用定制配体保护的金属纳米簇的特性的有前途的途径。尽管已经在几种结构中证明了成功的掺杂，但是尚不清楚掺杂剂偏爱以不同浓度占据纳米簇上特定位置的根本原因。在这项研究中，我们应用了最初为配体保护的单金属纳米团簇开发的热力学稳定性模型，以使在配体保护的Au纳米团簇上的合成可及性，掺杂剂位置和各种杂金属的浓度合理化。重要的是，我们证明了热力学稳定性理论是使用第一性原理计算准确描述纳米团簇上掺杂效应的重要一步。