Development of Linear-Scaling Methods for Calculating Energy Gradients and NMR Chemical Shifts at the Second-Order Møller-Plesset Perturbation Level

开发用于计算二阶 Mäller-Plesset 扰动水平的能量梯度和 NMR 化学位移的线性标度方法

• 批准号: 244944579
• 负责人: Professor Dr. Christian Ochsenfeld
• 金额: --
• 依托单位: Department Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2013
• 资助国家: 德国
• 起止时间: 2012-12-31 至 2016-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/244944579?language=en
• 关键词: Development; Linear; Scaling; Methods; Calculating

The reliable quantum-chemical calculation of NMR chemical shieldings represents an important link between theory and experiment, where second-order Møller-Plesset perturbation theory (MP2) can provide reliable data for many molecular systems. However, for large molecular systems the steep fifth-order scaling of the computational effort with molecular size prohibits such calculations. Therefore, the project aims to reduce this scaling and to develop a fast, linear-scaling atomic-orbital (AO) based MP2 NMR method that opens the way to compute systems with 1000 and more atoms. At the same time, the closely related linear-scaling AO-MP2 energy gradients important for structure determination or direct Born-Oppenheimer molecular dynamics will be developed. Moreover, for computing the MP2 NMR shielding tensor for selected nuclei, a suitable method will be devised that reduces the fifth-order scaling to sublinear scaling (i.e., asymptotically independently) with molecular size. In this way, the project is expected to substantially increase the possibilities for reliable quantum-chemical assignments of NMR spectra.

NMR化学屏蔽的可靠量子化学计算是理论和实验之间的重要联系，其中二阶Møller-Plesset微扰理论（MP2）可以为许多分子系统提供可靠的数据。然而，对于大分子系统的陡峭的五阶标度的计算工作与分子大小禁止这样的计算。 因此，该项目的目标是减少这种缩放，并开发一种快速，线性缩放的基于原子轨道（AO）的MP2 NMR方法，为计算具有1000个或更多原子的系统开辟了道路。 与此同时，密切相关的线性标度AO-MP2能量梯度的结构确定或直接玻恩-奥本海默分子动力学的重要性将被开发。此外，为了计算所选核的MP2 NMR屏蔽张量，将设计将五阶标度降低到次线性标度（即，渐近独立地）与分子大小。通过这种方式，该项目预计将大大增加可靠的NMR光谱量子化学分配的可能性。

项目成果

Communication: Almost error-free resolution-of-the-identity correlation methods by null space removal of the particle-hole interactions.

通信：通过零空间去除粒子-空穴相互作用来几乎无错误地解析身份相关方法

• DOI: 10.1063/1.4985085
• 发表时间: 2017
• 期刊: The Journal of chemical physics
• 作者: H. F. Schurkus;A. Luenser;C. Ochsenfeld
• 通讯作者: C. Ochsenfeld

Communication: A reduced scaling J-engine based reformulation of SOS-MP2 using graphics processing units.

• DOI: 10.1063/1.4891797
• 发表时间: 2014-08
• 期刊: The Journal of chemical physics
• 作者: S. Maurer;J. Kussmann;C. Ochsenfeld

Nuclear Magnetic Shieldings of Stacked Aromatic and Antiaromatic Molecules.

堆叠芳香族和反芳香族分子的核磁屏蔽

• DOI: 10.1021/acs.jctc.6b01250
• 发表时间: 1962
• 期刊: Journal of chemical theory and computation
• 影响因子: 5.5
• 作者: D. Sundholm;M. Rauhalahti;N. Özcan;R. Mera-Adasme;J. Kussmann;C. Ochsenfeld
• 通讯作者: C. Ochsenfeld

Vanishing-Overhead Linear-Scaling Random Phase Approximation by Cholesky Decomposition and an Attenuated Coulomb-Metric.

通过 Cholesky 分解和衰减库仑度量进行消失开销线性缩放随机相位近似

• DOI: 10.1021/acs.jctc.6b01235
• 发表时间: 2017
• 期刊: Journal of chemical theory and computation
• 影响因子: 5.5
• 作者: A. Luenser;H. F. Schurkus;C. Ochsenfeld
• 通讯作者: C. Ochsenfeld

Computation of indirect nuclear spin-spin couplings with reduced complexity in pure and hybrid density functional approximations.

• DOI: 10.1063/1.4962260
• 发表时间: 2016-09
• 期刊: The Journal of chemical physics
• 作者: A. Luenser;J. Kussmann;C. Ochsenfeld