Electronic structure calculations of sub-nanometer oxide-supported transition metal particles

该项目旨在增加我们对支持在技术上重要的氧化物衬底（如Mg0， Al203， TiO2和SiO2）表面上的小亚纳米级过渡金属的结构，键合和电子性能的理解。为此目的，将使用申请人小组开发的并行计算机代码PARAGAUSS，对充分嵌入的表面簇模型进行高密度泛函计算。该程序提供了各种有利于项目目标的功能，例如氧化物衬底团簇的一致嵌入，标量相对论和自旋轨道效应的自一致处理，计算激发能和电子g张量的选项。这项理论工作将补充优先项目中的实验项目，例如乌尔姆大学的海兹大学和汉堡大学的伍尔特大学。在第一个资助期内，工作将侧重于两种类型的支撑金属系统的几何和电子结构以及各种光谱参数，这些系统表现出明显的量子尺寸效应：(i)在表征良好的基体MgO上由Fe、Co和Ni亚群的高自旋原子组成的低核团簇，强调表面不规则性的影响；（ii）在不同载体上的铸币金属的小颗粒，追踪氧化物载体与沉积物相互作用的特异性。

The project aims at increasing our understanding of the structure, bonding and electronic properties of small sub-nanoscale transition metal species supported on surfaces of technologically important oxide substrates, like Mg0, Al203, TiO2 und SiO2. For this purpose, high-level density functional calculations of adequately embedded surface cluster models will be carried out, using the parallel computer code PARAGAUSS developed in the group of the applicant. This program provides various features, advantageous for the goals of the project, e.g. a consistent embedding for oxide substrate clusters, self-consistent treatment of scalar relativistic and spin-orbit effects, options for calculating excitation energies and electronic g tensors. This theoretical effort will supplement experimental projects within the priority program, e.g. by U. Heiz, University of Ulm, and W. Wurth, University of Hamburg. During the first funding period, work will focus on the geometric and electronic structure as well as various spectroscopic parameters of two types of supported metal systems that exhibit pronounced quantum size effects: (i) low nuclearity clusters of high-spin atoms of the Fe, Co and Ni subgroups on the well-characterized substrate MgO, emphasizing the influence of surface irregularities; (ii) small particles of the coinage metals on varying supports, tracing the specificity of the oxide support for interactions with the deposits.