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偶极极化率的四维标度:从单粒子模型到原子与分子

Four-Dimensional Scaling of Dipole Polarizability: From Single-Particle Models to Atoms and Molecules.

作者信息

Góger Szabolcs, Karimpour Mohammad Reza, Tkatchenko Alexandre

机构信息

Department of Physics and Materials Science, University of Luxembourg, L-1511 Luxembourg City, Luxembourg.

出版信息

J Chem Theory Comput. 2024 Aug 13;20(15):6621-6631. doi: 10.1021/acs.jctc.4c00582. Epub 2024 Jul 17.

DOI:10.1021/acs.jctc.4c00582
PMID:39015013
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11325554/
Abstract

Scaling laws enable the determination of physicochemical properties of molecules and materials as a function of their size, density, number of electrons or other easily accessible descriptors. Such relations can be counterintuitive and nonlinear, and ultimately yield much needed insight into quantum mechanics of many-particle systems. In this work, we show on the basis of single-particle models, multielectron atoms and molecules that the dipole polarizability of quantum systems is generally proportional to the fourth power of a characteristic length, computed from the ground-state wave function. This four-dimensional (4D) scaling is independent of the ratio of bound-to-bound and bound-to-continuum electronic transitions and applies to many-electron atoms when a correlated length metric is used. Finally, this scaling law is applied to predict the polarizability of molecules by electrostatically coupled atoms-in-molecules approach, obtaining approximately 8% absolute and relative accuracy with respect to hybrid density functional theory (DFT) on the QM7-X data set of organic molecules, providing an efficient and scalable model for the anisotropic polarizability tensors of extended (bio)molecules.

摘要

标度律能够根据分子和材料的大小、密度、电子数或其他易于获取的描述符来确定其物理化学性质。这类关系可能违反直觉且是非线性的,最终能为多粒子系统的量子力学提供急需的见解。在这项工作中,我们基于单粒子模型、多电子原子和分子表明,量子系统的偶极极化率通常与根据基态波函数计算出的特征长度的四次方成正比。这种四维(4D)标度与束缚态到束缚态以及束缚态到连续态电子跃迁的比率无关,并且当使用相关长度度量时适用于多电子原子。最后,通过静电耦合分子中的原子方法应用此标度律来预测分子的极化率,在有机分子的QM7-X数据集上相对于杂化密度泛函理论(DFT)获得了约8%的绝对和相对精度,为扩展(生物)分子的各向异性极化率张量提供了一个高效且可扩展的模型。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/a78470ef8a6f/ct4c00582_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/4a2ddc71be26/ct4c00582_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/8e0ac6aa958c/ct4c00582_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/43c571fbb417/ct4c00582_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/b0768f239300/ct4c00582_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/73fc8fb31aba/ct4c00582_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/931f1eb0a120/ct4c00582_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/aa14cdb48bfa/ct4c00582_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/a78470ef8a6f/ct4c00582_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/4a2ddc71be26/ct4c00582_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/8e0ac6aa958c/ct4c00582_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/43c571fbb417/ct4c00582_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/b0768f239300/ct4c00582_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/73fc8fb31aba/ct4c00582_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/931f1eb0a120/ct4c00582_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/aa14cdb48bfa/ct4c00582_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/893f/11325554/a78470ef8a6f/ct4c00582_0008.jpg

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本文引用的文献

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libMBD: A general-purpose package for scalable quantum many-body dispersion calculations.libMBD:用于可扩展量子多体色散计算的通用软件包。
J Chem Phys. 2023 Nov 7;159(17). doi: 10.1063/5.0170972.
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Data-driven tailoring of molecular dipole polarizability and frontier orbital energies in chemical compound space.
化合物空间中基于数据驱动的分子偶极极化率和前沿轨道能量的定制
Phys Chem Chem Phys. 2023 Aug 23;25(33):22211-22222. doi: 10.1039/d3cp02256k.
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Quantum Many-Body Theory from a Solution of the N-Representability Problem.量子多体理论源于 N 可表示性问题的解。
Phys Rev Lett. 2023 Apr 14;130(15):153001. doi: 10.1103/PhysRevLett.130.153001.
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Efficient and accurate density-based prediction of macromolecular polarizabilities.基于密度的大分子极化率高效准确预测
Phys Chem Chem Phys. 2023 Jan 18;25(3):2131-2141. doi: 10.1039/d2cp04690c.
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A new framework for frequency-dependent polarizable force fields.一种频率相关极化力场的新框架。
J Chem Phys. 2022 Sep 28;157(12):124106. doi: 10.1063/5.0115151.
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Exact Sum-Rule Approach to Polarizability and Asymptotic van der Waals Functionals─Derivation of Exact Single-Particle Benchmarks.极化率和渐近范德瓦尔斯泛函的精确求和规则方法——精确单粒子基准的推导
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