First-Principles Statistical Mechanics Studies of Doped Silicon Clusters: From Isolated Cages to Clusters in Complex Environments

本项目的目的是建立一个基本的理解，即如何利用简单气相分子的吸附和掺杂之间的相互作用来微调小硅团簇的功能。由于亚纳米尺寸范围内团簇的几何结构和电子结构之间的复杂关系，可靠地确定相应的基态几何结构是先决条件。因此，该项目的一个主要方面是为这类系统开发和使用基于密度泛函理论的有效无偏抽样技术。主要目的是利用获得的详细的几何、能量和电子结构数据来建立对具有感兴趣的材料性质的稳定的吸附/掺杂组合的趋势的理解。特别是通过计算振动指纹和X射线吸收光谱来寻求与实验的联系，也是为了方法验证。

The aim of the present project is to establish a fundamental understanding of how the interplay between adsorption of simple gas-phase molecules and doping may be employed to fine-tune the function of small silicon clusters. Due to the intricate relationship between the geometric and electronic structure of clusters in the sub-nm size range a reliable determination of the corresponding ground-state geometric structures is a prerequisite. A major aspect of the project is therefore to develop and employ efficient unbiased sampling techniques based on density-functional theory for this class of systems. The main objective is to use the obtained detailed geometric, energetic and electronic structure data to establish a trend understanding of stable adsorbate/dopant combinations with interesting materials properties. Contact to experiment, also for method validation, is particularly sought through the computation of vibrational fingerprints and X-ray absorption spectra.