BOS-TMC数据集：159k个实验表征的过渡金属配合物的DFT性质，涵盖多种电荷和自旋状态
The BOS-TMC Dataset: DFT Properties of 159k Experimentally Characterized Transition Metal Complexes Spanning Multiple Charge and Spin States
AI总结：
BOS-TMC数据集包含159k个实验表征的过渡金属配合物的DFT性质，涵盖多种电荷和自旋状态，通过迭代方法确定电荷并计算自旋依赖的原子化能，为机器学习和DFT基准提供高保真基础。
摘要：
我们介绍了Boston Open-Shell Transition Metal Complex (BOS-TMC)数据集，包含159k个实验表征的单核过渡金属配合物（TMCs）的密度泛函理论（DFT）性质，这些配合物处于多种自旋状态，具有范围广泛的形式电荷，源自Cambridge Structural Database (CSD)。为了整理这个集合，我们进行了迭代过程以准确确定总体TMC电荷。从这些信息中，我们获得了多达三种自旋状态的性质，即对于3d金属低自旋、中间自旋和高自旋，对于4d和5d金属为低自旋和中间自旋，根据金属电子配置的兼容性，总计343.8k个TMC/自旋组合。与先前的集合不同，我们在优化过程中保留了实验重原子坐标。我们使用PBE0/def2-TZVP单点能报告所有性质。我们介绍了一种计算金属自旋依赖原子化能的方案，并为每个TMC报告这些能量。除了电子能量外，我们还报告了多达七个额外的属性，包括HOMO、LUMO、HOMO-LUMO间隙、原子部分电荷、偶极矩、原子化能和自旋分裂能，总计超过2.9M个TMC相关属性。对于基于大小选择的代表性子集超过10k个配合物，我们评估了计算属性对交换相关（xc）功能选择的敏感性，从十二种xc功能中选取，覆盖“Jacob's ladder”各阶，突出TMC空间中不确定性最大的热点区域。与先前的过渡金属数据集相比，BOS-TMC在电荷和自旋配置方面更大更多样，因此其属性范围也更广泛。该数据集预计为机器学习模型开发、DFT基准和探索提供高保真的基础。
英文摘要：
We present the Boston Open-Shell Transition Metal Complex (BOS-TMC) dataset, a set of density functional theory (DFT) properties for 159k experimentally characterized mononuclear transition metal complexes (TMCs) in multiple spin states with a range of formal charges derived from the Cambridge Structural Database (CSD). To curate this set, we carried out an iterative procedure to confidently assign overall TMC charge. From this information, we then obtained properties in up to three spin states, i.e., low-, intermediate-, and high-spin for 3d metals and low- and intermediate-spin for 4d and 5d metals, depending on compatibility with the metal electron configuration, for a total of 343.8k TMC/spin combinations. At odds with prior sets, we preserved experimental heavy-atom coordinates in these structures during optimization. We report all properties using PBE0/def2-TZVP single-point energies on these structures. We introduce a scheme for computing metal-spin-dependent atomization energies, which we report for each TMC. Alongside electronic energies, we report up to seven additional properties including: HOMO, LUMO, HOMO-LUMO gap, atomic partial charges, dipole moments, atomization energies, and spin-splitting energies for a total of over 2.9M TMC-associated properties. For a representative subset of over 10k complexes chosen based on size, we evaluate the sensitivity of computed properties to exchange-correlation (xc) functional choice from a set of twelve xcs spanning rungs of "Jacob's ladder", highlighting hotspots of TMC space that have the greatest uncertainty. In comparison to prior transition-metal datasets, BOS-TMC is both larger and more diverse in terms of charge and spin configurations and, as a result, more diverse in its range of properties. This dataset is expected to provide a high-fidelity foundation for machine-learning model development, DFT benchmarking, and exploration.
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