Modeling angle-resolved photoemission of graphene and black phosphorus nano structures

Angle-resolved photoemission spectroscopy (ARPES) data on electronic structure are difficult to interpret, because various factors such as atomic structure and experimental setup influence the quantum mechanical effects during the measurement. Therefore, we simulated ARPES of nano-sized molecules to corroborate the interpretation of experimental results. Applying the independent atomic-center approximation, we used density functional theory calculations and custom-made simulation code to compute photoelectron intensity in given experimental setups for every atomic orbital in poly-aromatic hydrocarbons of various size, and in a molecule of black phosphorus. The simulation results were validated by comparing them to experimental ARPES for highly-oriented pyrolytic graphite. This database provides the calculation method and every file used during the work flow.

角分辨光电子能谱（Angle-resolved photoemission spectroscopy, ARPES）数据在电子结构研究中的解读往往存在较大难度，这是因为原子结构、实验装置等诸多因素会在测量过程中对量子力学效应产生影响。为此，我们通过模拟纳米尺度分子的ARPES信号，以辅助验证实验结果的解读合理性。我们采用独立原子中心近似方法，结合密度泛函理论（density functional theory, DFT）计算与定制化模拟代码，针对不同尺寸的多环芳烃以及黑磷分子中的每个原子轨道，在给定实验装置条件下计算光电子强度。我们通过将模拟结果与高定向热解石墨的实验ARPES数据进行对比，完成了模拟结果的有效性验证。本数据集包含本次研究工作流程中使用的全部计算方法与相关文件。