Quantum chemical cluster models for chemi- and physisorption of chlorobenzene on Si(111)-7×7.
Quantum chemical cluster models for chemi- and physisorption of chlorobenzene on Si(111)-7×7.
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氯苯在 Si(111)-7×7 上化学和物理吸附的量子化学簇模型。
DOI：
10.1021/jp504208d
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发表时间：
2014
期刊：
影响因子：
--
通讯作者：
R. Palmer
中科院分区：
文献类型：
--
作者：
M. Utecht;Tianluo Pan;T. Klamroth;R. Palmer
受最近的原子操纵实验的启发，我们报告了氯苯在Si(111)-7×7表面的化学和物理吸附最小值的量子化学计算。采用密度泛函理论聚类方法，使用B3LYP混合泛函和Grimme的经验色散校正（D3）。我们能够确定结合能为1.6 eV和物理吸附能为0.6 eV的化学吸附位点，两者都与实验数据的趋势一致。集群方法开启了基于第一性原理的STM操作实验动态描述的可能性，其解释涉及化学和物理吸收状态。然而，我们发现在选择聚类、基集和评估离散校正时必须特别注意。
Motivated by recent atomic manipulation experiments, we report quantum chemical calculations for chemi- and physisorption minima of chlorobenzene on the Si(111)-7×7 surface. A density functional theory cluster approach is applied, using the B3LYP hybrid functional alongside Grimme's empirical dispersion corrections (D3). We were able to identify chemisorption sites of binding energies of 1.6 eV and physisorption energies of 0.6 eV, both in encouraging agreement with the trend of experimental data. The cluster approach opens up the possibility of a first-principles based dynamical description of STM manipulation experiments on this system, the interpretation of which involves both the chemi- and physisorbed states. However, we found that special care has to be taken regarding the choice of clusters, basis sets, and the evaluation of the dispersion corrections.