论文标题

精确的非经验范围分离的杂种范德华密度在复杂的分子问题,固体和表面上功能

Accurate non-empirical range-separated hybrid van der Waals density functional for complex molecular problems, solids, and surfaces

论文作者

Shukla, Vivekanand, Jiao, Yang, Lee, Jung-Hoon, Schroder, Elsebeth, Neaton, Jeffrey B., Hyldgaard, Per

论文摘要

我们在非经验VDW-DF方法[JPCM 32,393001(2020)]中引入了一种新的,通用的,范围分离的杂种范德华密度\ ph {功能,称为vdw-df-ahbr,}。它将VDW-DF2的相关性与由\ ph {ph {新的Exchange效果模型}固定的筛选的Fock交换相结合,在密度 - 显式VDW-DF2-B86R功能中的新模型[PRB 89,121103(R)(R)(2014)]。新的VDW-DF2-AHBR可防止虚假交换结合,并具有从多体扰动分析中设置的小密度梯度形式。它对于\ ph {块和分层材料}是准确的,并且系统地并显着提高了当前VDW-DF的性能,用于分子问题。重要的是,VDW-DF2-AHBR在广泛的非共价相互作用基准集上还胜过范围分离的范围分离杂种,同时成功缓解密度驱动的错误通常会影响分子过渡状态和异构化的描述。 VDW-DF2-AHBR进一步改善了艺术密度功能理论方法的改进1)通过1)正确预测PT(111),2)在PT(111)上均具有对co吸附的现场偏好,超过了现有的非经验的非经验VDW-DF,以对CO $ _2 $ co $ _2 $ accoration的描述,并在功能中的范围中进行了高度准确的框架,并在一个函数上的框架中,并且在且在一个函数上的框架中,并且在均具有良好的范围。 \ ph {用于DNA组装模型中的基本对相互作用集。

We introduce a new, general-purpose, range-separated hybrid van der Waals density \ph{functional, termed vdW-DF-ahbr,} within the non-empirical vdW-DF method [JPCM 32, 393001 (2020)]. It combines correlation from vdW-DF2 with a screened Fock exchange that is fixed by \ph{a new model of exchange effects} in the density-explicit vdW-DF2-b86r functional [PRB 89, 121103(R) (2014)]. The new vdW-DF2-ahbr prevents spurious exchange binding and has a small-density-gradient form set from many-body perturbation analysis. It is accurate for \ph{bulk as well as layered materials} and it systematically and significantly improves the performance of present vdW-DFs for molecular problems. Importantly, vdW-DF2-ahbr also outperforms present-standard (dispersion-corrected) range-separated hybrids on a broad collection of noncovalent-interaction benchmark sets, while at the same time successfully mitigating the density-driven errors that often affect the description of molecular transition states and isomerization calculations. vdW-DF2-ahbr furthermore improves on state of the art density functional theory approaches by 1) correctly predicting both the substrate structure and the site preference for CO adsorption on Pt(111), 2) outperforming existing non-empirical vdW-DFs for the description of CO$_2$ adsorption in both a functionalized and in a simple metal-organic framework, and 3) being highly accurate \ph{for the} set of base-pair interactions in a model of DNA assembly.

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