基于域的局部对自然轨道 (DLPNO) 结合集群理论的准确和高效的开源实现,使用t1转换的哈密尔顿式
Andy Jiang1, Zachary L Glick2, David Poole2
1Center for Computational Quantum Chemistry, Department of Chemistry, University of Georgia, Athens, Georgia 30602, USA.
The Journal of chemical physics
|August 22, 2024
概括
我们开发了一种高效的,开源的计算化学方法,基于域的局部对自然轨道结合集群理论通过扰动三倍数[DLPNO-CCSD(T) ],用于准确的分子能量计算. 这种方法在复杂的系统中实现了高精度,包括大型分子和非共价相互作用.
科学领域:
- 计算化学是一种计算化学.
- 量子化学是一种量子化学.
- 理论化学是一种理论化学.
背景情况:
- 合集群理论是一种高精度的量子化学方法.
- 计算大型分子系统在计算上要求很高.
- 局部对自然轨道 (PNO) 方法旨在降低计算成本.
研究的目的:
- 通过扰动三重组 [DLPNO-CCSD(T) ] 提出基于域的局部对自然轨道的高效,开源的公式,通过扰动三重组合集群理论.
- 为了证明开发的DLPNO-CCSD算法的准确性和效率.
- 为了验证该方法对具有挑战性的化学相互作用和大型系统进行验证.
主要方法:
- 实现一个线性缩放的DLPNO-CCSD (T) 算法.
- 使用t1转换的哈密尔顿子来简化能量评估.
- 优化参数 (TightPNO) 以获得高精度.
主要成果:
- 与正规CCSD (T) 相比,获得了相对能量的 sub-kJ mol-1 偏差.
- 已证明的典型误差大约为0.1 kcal mol-1.
- 成功建模了非共价相互作用和像胰岛素 (787个原子) 这样的大型系统.
结论:
- 开发的DLPNO-CCSD (T) 公式为电子结构计算提供了一种高效和准确的方法.
- 该方法在具有挑战性的系统中表现出色,包括非共价相互作用.
- 开源代码可以在计算化学研究中得到更广泛的应用.
相关概念视频
03:35Hybridization of Atomic Orbitals II
31.9K
sp3d and sp3d 2 Hybridization
31.9K
03:24Hybridization of Atomic Orbitals I
46.7K
The mathematical expression known as the wave function, ψ, contains information about each orbital and the wavelike properties of electrons in an isolated atom. When atoms are bound together in a molecule, the wave functions combine to produce new mathematical descriptions that have different shapes. This process of combining the wave functions for atomic orbitals is called hybridization and is mathematically accomplished by the linear combination of atomic orbitals. The new orbitals that...
46.7K
03:51Molecular Orbital Theory II
19.0K
Molecular Orbital Energy Diagrams
19.0K
02:35Molecular Orbital Theory I
31.9K
Overview of Molecular Orbital Theory
31.9K
02:38Valence Bond Theory and Hybridized Orbitals
19.1K
According to valence bond theory, a covalent bond results when: (1) an orbital on one atom overlaps an orbital on a second atom, and (2) the single electrons in each orbital combine to form an electron pair. The strength of a covalent bond depends on the extent of overlap of the orbitals involved. Maximum overlap is possible when the orbitals overlap on a direct line between the two nuclei.
A σ bond (single bond in a Lewis structure) is a covalent bond in which the electron density is...
A σ bond (single bond in a Lewis structure) is a covalent bond in which the electron density is...
19.1K
02:44Atomic Orbitals
33.4K
An atomic orbital represents the three-dimensional regions in an atom where an electron has the highest probability to reside. The radial distribution function indicates the total probability of finding an electron within the thin shell at a distance r from the nucleus. The atomic orbitals have distinct shapes which are determined by l, the angular momentum quantum number. The orbitals are often drawn with a boundary surface, enclosing densest regions of the cloud.
33.4K