q-AQUA: A Many-Body CCSD(T) Water Potential, Including Four-Body Interactions, Demonstrates the Quantum Nature of Water from Clusters to the Liquid Phase.
q-AQUA: A Many-Body CCSD(T) Water Potential, Including Four-Body Interactions, Demonstrates the Quantum Nature of Water from Clusters to the Liquid Phase.
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q-AQUA：多体 CCSD(T) 水势，包括四体相互作用，展示了水从簇到液相的量子性质。
DOI：
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发表时间：
2022
影响因子：
5.7
通讯作者：
J. Bowman
中科院分区：
文献类型：
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作者：
Qi Yu;Chen Qu;P. Houston;R. Conte;Apurba Nandi;J. Bowman
已报道了许多水模型势能面 (PES)；然而，没有一个是严格遵循“第一原则”的。在这里，我们基于 CCSD(T) 理论水平的多体表示直至四体相互作用报告了这种潜力。新的 PES 以水六聚体异构体的解离能、谐波频率以及棱镜、书形和笼形异构体零点能量的无限制扩散蒙特卡罗 (DMC) 计算为基准。 20 聚体的几种异构体的解离能与最近的基准能量非常吻合。对该簇的探索性 DMC 计算验证了新 PES 对于量子模拟的鲁棒性。新 PES 的精度和速度针对标准凝聚相特性（即径向分布函数和自扩散常数）进行了验证。事实证明，量子效应对于这些可观察到的现象是显着的，并且还需要使理论与实验完全一致。
Many model potential energy surfaces (PESs) have been reported for water; however, none are strictly from "first-principles". Here we report such a potential, based on a many-body representation at the CCSD(T) level of theory up to the four-body interaction. The new PES is benchmarked for the isomers of the water hexamer for dissociation energies, harmonic frequencies, and unrestricted diffusion Monte Carlo (DMC) calculations of the zero-point energies of the Prism, Book, and Cage isomers. Dissociation energies of several isomers of the 20-mer agree well with recent benchmark energies. Exploratory DMC calculations on this cluster verify the robustness of the new PES for quantum simulations. The accuracy and speed of the new PES are demonstrated for standard condensed phase properties, i.e., the radial distribution function and the self-diffusion constant. Quantum effects are shown to be substantial for these observables and also needed to bring theory into excellent agreement with experiment.
影响因子：
6.3
作者：
Kapil, Venkat;Rossi, Mariana;Ceriotti, Michele
通讯作者：
Ceriotti, Michele
影响因子：
4.4
作者：
Habershon, Scott;Markland, Thomas E.;Manolopoulos, David E.
通讯作者：
Manolopoulos, David E.