New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy.
New scaling relations to compute atom-in-material polarizabilities and dispersion coefficients: part 1. Theory and accuracy.
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作者：
极化率和伦敦色散力对许多化学过程都很重要。经典原子模拟的力场可以使用原子在材料中的极化率和Cn（n = 6，8，9，10.）色散系数来构造。本文解决了如何有效地将这些参数分配给材料中的组成原子的关键问题，以便更好地再现整个材料的性能。我们开发了一套新的标度律和计算算法（称为MCLF），以便在不同的材料类型中以准确和计算效率高的方式做到这一点。我们引入了传导极限上限和m标度来描述表面和掩埋原子的不同行为。我们通过将结果与孤立的中性和带电原子、各种双原子分子、各种多原子分子（例如，聚并苯、富勒烯和小的有机和无机分子）和致密固体（包括金属的、共价的和离子的）。我们还展示了与抑制剂分子复合的HIV逆转录酶的结果。MCLF提供了构建力场所需的非定向屏蔽极化率、定向屏蔽静态极化率张量分量和本征值以及环境屏蔽C6系数。总体而言，与TS-SCS方法相比，MCLF的准确性有所提高。对于TS-SCS，我们比较了电荷分区方法，并显示DDEC 6分区比Hirshfeld分区产生更准确的结果。MCLF还给出了C8，C9和C10色散系数和量子德鲁德振荡器参数的近似。这种方法应该找到广泛的应用参数化经典力场和密度泛函理论（DFT）+色散方法。提出了一种计算不同材料类型的原子极化率和色散系数的新方法。
Polarizabilities and London dispersion forces are important to many chemical processes. Force fields for classical atomistic simulations can be constructed using atom-in-material polarizabilities and Cn (n = 6, 8, 9, 10…) dispersion coefficients. This article addresses the key question of how to efficiently assign these parameters to constituent atoms in a material so that properties of the whole material are better reproduced. We develop a new set of scaling laws and computational algorithms (called MCLF) to do this in an accurate and computationally efficient manner across diverse material types. We introduce a conduction limit upper bound and m-scaling to describe the different behaviors of surface and buried atoms. We validate MCLF by comparing results to high-level benchmarks for isolated neutral and charged atoms, diverse diatomic molecules, various polyatomic molecules (e.g., polyacenes, fullerenes, and small organic and inorganic molecules), and dense solids (including metallic, covalent, and ionic). We also present results for the HIV reverse transcriptase enzyme complexed with an inhibitor molecule. MCLF provides the non-directionally screened polarizabilities required to construct force fields, the directionally-screened static polarizability tensor components and eigenvalues, and environmentally screened C6 coefficients. Overall, MCLF has improved accuracy compared to the TS-SCS method. For TS-SCS, we compared charge partitioning methods and show DDEC6 partitioning yields more accurate results than Hirshfeld partitioning. MCLF also gives approximations for C8, C9, and C10 dispersion coefficients and quantum Drude oscillator parameters. This method should find widespread applications to parameterize classical force fields and density functional theory (DFT) + dispersion methods. A new method was developed to compute atom-in-material polarizabilities and dispersion coefficients for diverse material types.
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DOI：
10.1021/ci00015a015
发表时间：
1993-09-01
期刊：
JOURNAL OF CHEMICAL INFORMATION AND COMPUTER SCIENCES
影响因子：
--
作者：
BUSH, BL;SHERIDAN, RP
通讯作者：
SHERIDAN, RP
影响因子：
1.7
作者：
BADER, RFW;KEITH, TA;LAIDIG, KE
通讯作者：
LAIDIG, KE
影响因子：
15
作者：
APPLEQUIST, J;CARL, JR;FUNG, KK
通讯作者：
FUNG, KK
影响因子：
4.4
作者：
Axilrod, BM;Teller, E
通讯作者：
Teller, E
DOI：
10.1107/s0108768102006948
发表时间：
2002-06-01
期刊：
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE
影响因子：
--
作者：
Belsky, A;Hellenbrandt, M;Luksch, P
通讯作者：
Luksch, P