Balzaretti Filippo, Voss Johannes
SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.
Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.
J Chem Theory Comput. 2024 Aug 8. doi: 10.1021/acs.jctc.4c00345.
First-principles electronic structure simulations are an invaluable tool for understanding chemical bonding and reactions. While machine-learning models such as interatomic potentials significantly accelerate the exploration of potential energy surfaces, electronic structure information is generally lost. Particularly in the field of heterogeneous catalysis, simulated electron band structures provide fundamental insights into catalytic reactivity. This ab initio knowledge is preserved in semiempirical methods such as density functional tight binding (DFTB), which extend the accessible computational length and time scales beyond first-principles approaches. In this paper we present Shell-Optimized Atomic Confinement (SOAC) DFTB electronic-part-only parametrizations for bulk and surface band structures of all -block transition metals that enable efficient predictions of electronic descriptors for large structures or high-throughput studies on complex systems outside the computational reach of density functional theory.
第一性原理电子结构模拟是理解化学键合和反应的宝贵工具。虽然诸如原子间势等机器学习模型显著加速了势能面的探索，但电子结构信息通常会丢失。特别是在多相催化领域，模拟的电子能带结构为催化反应活性提供了基本见解。这种从头算知识保存在诸如密度泛函紧束缚（DFTB）等半经验方法中，这些方法将可及的计算长度和时间尺度扩展到超越第一性原理方法的范围。在本文中，我们提出了用于所有块体过渡金属的体相和表面能带结构的壳层优化原子限制（SOAC）DFTB仅电子部分的参数化方法，该方法能够对大型结构的电子描述符进行高效预测，或对密度泛函理论计算范围之外的复杂系统进行高通量研究。
