水相化学密度泛函理论中数据驱动的多体势

IF 6.1 Q2 CHEMISTRY, PHYSICAL Chemical physics reviews Pub Date : 2023-03-01 DOI:10.1063/5.0129613
Etienne Palos, Saswata Dasgupta, Eleftherios Lambros, F. Paesani
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引用次数: 3

摘要

密度泛函理论(DFT)应用于水分子相互作用的建模已有三十多年的历史。水在化学和生物过程中无处不在,这要求我们对水的物理学有统一的理解,从单分子到热力学极限,再到两者之间的一切。数据驱动和机器学习潜力的最新发展加速了具有DFT精度的水和水系统的模拟。然而,在水的DFT模型中,对局部和非局部多体(MB)相互作用进行严格处理的凝聚态水的异常性质往往不能令人满意或部分缺失。在这篇综述中,我们讨论了基于DFT的水和水系统的建模,并提供了从DFT参考数据开发数据驱动的多体势的一般理论/计算框架的全面描述。这个框架,被称为MB-DFT,可以很容易地实现气相和凝聚态小分子的多体分子动力学(MD)模拟,同时保持底层DFT模型的准确性。强调了理论上的考虑,包括离域误差在水的MB-DFT电位中所起的作用,以及通过密度校正的形式主义将DFT和MB-DFT提高到接近化学精度的可能性。详细描述了MB- dft框架的发展,以及它在MB- md模拟中的应用,以及最近在量子力学/MB分子力学(QM/MB- mm)方案中对溶液中反应过程建模的扩展,该方案使用水作为原型溶剂。最后,我们确定了开放的挑战,并讨论了MB-DFT和QM/MB-MM凝聚相模拟的未来方向。
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Data-driven many-body potentials from density functional theory for aqueous phase chemistry
Density functional theory (DFT) has been applied to modeling molecular interactions in water for over three decades. The ubiquity of water in chemical and biological processes demands a unified understanding of its physics, from the single molecule to the thermodynamic limit and everything in between. Recent advances in the development of data-driven and machine-learning potentials have accelerated simulation of water and aqueous systems with DFT accuracy. However, anomalous properties of water in the condensed phase, where a rigorous treatment of both local and non-local many-body (MB) interactions is in order, are often unsatisfactory or partially missing in DFT models of water. In this review, we discuss the modeling of water and aqueous systems based on DFT and provide a comprehensive description of a general theoretical/computational framework for the development of data-driven many-body potentials from DFT reference data. This framework, coined MB-DFT, readily enables efficient many-body molecular dynamics (MD) simulations of small molecules, in both gas and condensed phases, while preserving the accuracy of the underlying DFT model. Theoretical considerations are emphasized, including the role that the delocalization error plays in MB-DFT potentials of water and the possibility to elevate DFT and MB-DFT to near-chemical-accuracy through a density-corrected formalism. The development of the MB-DFT framework is described in detail, along with its application in MB-MD simulations and recent extension to the modeling of reactive processes in solution within a quantum mechanics/MB molecular mechanics (QM/MB-MM) scheme, using water as a prototypical solvent. Finally, we identify open challenges and discuss future directions for MB-DFT and QM/MB-MM simulations in condensed phases.
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