Elevating density functional theory to chemical accuracy for water simulations through a density-corrected many-body formalism

被引:74
作者
Dasgupta, Saswata [1 ]
Lambros, Eleftherios [1 ]
Perdew, John P. [2 ,3 ]
Paesani, Francesco [1 ,4 ,5 ]
机构
[1] Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA
[2] Temple Univ, Dept Phys, Philadelphia, PA 19122 USA
[3] Temple Univ, Dept Chem, Philadelphia, PA 19122 USA
[4] Univ Calif San Diego, Mat Sci & Engn, La Jolla, CA 92093 USA
[5] Univ Calif San Diego, San Diego Supercomp Ctr, La Jolla, CA 92093 USA
基金
美国国家科学基金会;
关键词
POTENTIAL-ENERGY SURFACE; MOLECULAR-DYNAMICS SIMULATION; 1ST PRINCIPLES; LIQUID WATER; ELECTRON-AFFINITIES; BASIS-SETS; DIFFUSION-COEFFICIENTS; SELF-DIFFUSION; CLOSED-SHELL; HARTREE-FOCK;
D O I
10.1038/s41467-021-26618-9
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
No existing density functional correctly describes the properties of water across the entire phase diagram. The authors report a data-driven many-body potential energy function based on density-corrected SCAN functional that quantitatively reproduces the energetics of gas-phase water clusters, and correctly predicts the properties of liquid water. Density functional theory (DFT) has been extensively used to model the properties of water. Albeit maintaining a good balance between accuracy and efficiency, no density functional has so far achieved the degree of accuracy necessary to correctly predict the properties of water across the entire phase diagram. Here, we present density-corrected SCAN (DC-SCAN) calculations for water which, minimizing density-driven errors, elevate the accuracy of the SCAN functional to that of "gold standard" coupled-cluster theory. Building upon the accuracy of DC-SCAN within a many-body formalism, we introduce a data-driven many-body potential energy function, MB-SCAN(DC), that quantitatively reproduces coupled cluster reference values for interaction, binding, and individual many-body energies of water clusters. Importantly, molecular dynamics simulations carried out with MB-SCAN(DC) also reproduce the properties of liquid water, which thus demonstrates that MB-SCAN(DC) is effectively the first DFT-based model that correctly describes water from the gas to the liquid phase.
引用
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页数:12
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