Automated Construction of Quantum-Classical Hybrid Models
Automated Construction of Quantum-Classical Hybrid Models
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DOI：
10.1021/acs.jctc.1c00178
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发表时间：
2021-05-12
影响因子：
5.5
通讯作者：
Reiher, Markus
中科院分区：
文献类型：
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作者：
Brunken, Christoph;Reiher, Markus
我们提出了一种用于全自动构建量子力学(QM)-经典混合模型的协议，通过扩展我们之前报道的自参数化系统聚焦原子模型(SFAM)的方法[Brunken，C.；Reiher，M.J.Chem]。理论计算。2020、16、3、1646-1665]。在这种QM/SfAM方法中，QM区域的大小和组成是基于第一性原理自动计算的，因此混合模型能够准确地描述QM区域中心的原子力。这需要自动构建和评估不同大小的QM区域，并且需要为自动验证程序支付可承受的计算开销。将SfAM应用于模型的经典部分，消除了由于其以系统为中心的量子力学派生的参数化而对先前存在的参数的任何依赖。因此，QM/SfAM能够提供高保真和完全自动化。此外，由于SfAM参数是为整个系统生成的，因此我们的ansatz允许在分子探索期间方便地重新定义QM区域。为此，引入了一种局部重参数方案，当新的共价键形成(或断裂)并移动到经典区域时，该方案有效地动态产生额外的经典参数。
We present a protocol for the fully automated construction of quantum mechanical (QM)-classical hybrid models by extending our previously reported approach on self-parametrizing system-focused atomistic models (SFAMs) [Brunken, C.; Reiher, M. J. Chem. Theory Comput. 2020, 16, 3, 1646-1665]. In this QM/SFAM approach, the size and composition of the QM region are evaluated in an automated manner based on first principles so that the hybrid model describes the atomic forces in the center of the QM region accurately. This entails the automated construction and evaluation of differently sized QM regions with a bearable computational overhead that needs to be paid for automated validation procedures. Applying SFAM for the classical part of the model eliminates any dependence on pre-existing parameters due to its system-focused quantum mechanically derived parametrization. Hence, QM/SFAM is capable of delivering high fidelity and complete automation. Furthermore, since SFAM parameters are generated for the whole system, our ansatz allows for a convenient redefinition of the QM region during a molecular exploration. For this purpose, a local reparametrization scheme is introduced, which efficiently generates additional classical parameters on the fly when new covalent bonds are formed (or broken) and moved to the classical region.