While density functional theory (DFT) serves as a prevalent computational approach in electronic structure calculations, its computational demands and scalability limitations persist. Recently, leveraging neural networks to parameterize the Kohn-Sham DFT Hamiltonian has emerged as a promising avenue for accelerating electronic structure computations. Despite advancements, challenges such as the necessity for computing extensive DFT training data to explore each new system and the complexity of establishing accurate ML models for multi-elemental materials still exist. Addressing these hurdles, this study introduces a universal electronic Hamiltonian model trained on Hamiltonian matrices obtained from first-principles DFT calculations of nearly all crystal structures on the Materials Project. We demonstrate its generality in predicting electronic structures across the whole periodic table, including complex multi-elemental systems, solid-state electrolytes, Moir\'e twisted bilayer heterostructure, and metal-organic frameworks (MOFs). Moreover, we utilize the universal model to conduct high-throughput calculations of electronic structures for crystals in GeNOME datasets, identifying 3,940 crystals with direct band gaps and 5,109 crystals with flat bands. By offering a reliable efficient framework for computing electronic properties, this universal Hamiltonian model lays the groundwork for advancements in diverse fields, such as easily providing a huge data set of electronic structures and also making the materials design across the whole periodic table possible.

翻译：尽管密度泛函理论（DFT）作为电子结构计算中的一种主流计算方法，但其计算需求与可扩展性限制依然存在。近年来，利用神经网络参数化Kohn-Sham DFT哈密顿量已成为加速电子结构计算的一个有前景的方向。尽管取得了进展，但仍面临挑战，例如需要为探索每个新体系计算大量DFT训练数据，以及为多元素材料建立精确机器学习模型的复杂性。针对这些难题，本研究引入了一个通用电子哈密顿量模型，该模型基于对Materials Project中几乎所有晶体结构进行第一性原理DFT计算所得的哈密顿量矩阵进行训练。我们展示了其在预测整个元素周期表内电子结构方面的通用性，包括复杂多元素体系、固态电解质、Moiré扭曲双层异质结构以及金属有机框架（MOFs）。此外，我们利用该通用模型对GeNOME数据集中的晶体进行了高通量电子结构计算，识别出3,940个具有直接带隙的晶体和5,109个具有平带的晶体。通过提供一个可靠且高效的计算电子性质的框架，这一通用哈密顿量模型为各个领域的进展奠定了基础，例如轻松提供庞大的电子结构数据集，并使得在整个元素周期表内进行材料设计成为可能。