量子激发的SIBFA多体极化力场的发展：实现凝聚相分子动力学模拟
Development of the Quantum Inspired SIBFA Many-Body Polarizable Force Field: Enabling Condensed Phase Molecular Dynamics Simulations
摘要：
本文将从头计算的多体极化力场方法推广到凝聚相分子动力学模拟。量子激发的SIBFA程序是基于从局域分子轨道理论获得的简化积分，并实现其分子间势的完全分离。它体现了远程多极静电（高达四极）耦合到一个短程渗透校正（高达电荷四极），交换排斥，多体极化，多体电荷转移/离域，交换色散和色散（高达C10）。这使得从头算对称适应微扰理论（SAPT（DFT））气相参考计算的所有能量贡献的再现。SIBFA方法已集成在Tinker-HP大规模并行MD包中。为了做到这一点，所有的SIBFA能量梯度已被导出，该方法已被扩展到使用平滑粒子网格埃瓦尔德使周期性边界条件模拟。这种新颖的实现方式还特别包括计算上易于处理的多体电荷转移/离域贡献的简化。作为概念的证明，我们进行了第一次计算实验，定义了一个水模型拟合有限的（SAPT（DFT））数据集。SIBFA显示，使一个令人满意的再现气相充满活力的贡献和凝聚相的属性突出其物理动机的功能形式的重要性。
英文摘要：
We present the extension of the SIBFA (Sum of Interactions Between Fragments Ab initio Computed many-body polarizable force field to condensed phase Molecular Dynamics (MD) simulations. The Quantum-Inspired SIBFA procedure is grounded on simplified integrals obtained from localized molecular orbital theory and achieves full separability of its intermolecular potential. It embodies long-range multipolar electrostatics (up to quadrupole) coupled to a short-range penetration correction (up to charge-quadrupole), exchange-repulsion, many-body polarization, many-body charge transfer/delocalization, exchange-dispersion and dispersion (up to C10). This enables the reproduction of all energy contributions of ab initio Symmetry-Adapted Perturbation Theory (SAPT(DFT)) gas phase reference computations. The SIBFA approach has been integrated within the Tinker-HP massively parallel MD package. To do so all SIBFA energy gradients have been derived and the approach has been extended to enable periodic boundary conditions simulations using Smooth Particle Mesh Ewald. This novel implementation also notably includes a computationally tractable simplification of the many-body charge transfer/delocalization contribution. As a proof of concept, we perform a first computational experiment defining a water model fitted on a limited set of (SAPT(DFT)) data. SIBFA is shown to enable a satisfactory reproduction of both gas phase energetic contributions and condensed phase properties highlighting the importance of its physically-motivated functional form.
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