QM/ELMO: A Multi-Purpose Fully Quantum Mechanical Embedding Scheme Based on Extremely Localized Molecular Orbitals,The Journal of Physical Chemistry A

当前位置： X-MOL 学术 › J. Phys. Chem. A › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

QM/ELMO: A Multi-Purpose Fully Quantum Mechanical Embedding Scheme Based on Extremely Localized Molecular Orbitals
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2021-03-05 , DOI: 10.1021/acs.jpca.0c11450
Giovanni Macetti ₁ , Erna K. Wieduwilt ₁ , Alessandro Genoni ₁

Affiliation

The development of computationally advantageous methods for the study of large systems is a long-standing research topic in theoretical chemistry. Among these techniques, a prominent place is certainly occupied by the multiscale embedding strategies, from the well-known QM/MM (quantum mechanics/molecular mechanics) methods to the latest and promising fully quantum mechanical approaches. In this Feature Article, we will briefly review the recently proposed QM/ELMO (quantum mechanics/extremely localized molecular orbital) scheme, namely a new multiscale embedding strategy in which the most chemically relevant region of the investigated system is treated at fully quantum chemical level, while the remaining part (namely, the environment) is described by means of transferred extremely localized molecular orbitals that remain frozen throughout the computation. Other than highlighting the theoretical bases, here we will also review the main results obtained through all the currently available variants of the novel method. In particular, we will show how the QM/ELMO embedding scheme has been successfully exploited to perform both ground and excited state calculations, reproducing the results of corresponding fully quantum mechanical computations but with a much lower computational cost. A first application to crystallography will be also discussed, and we will describe how the QM/ELMO approach has been recently coupled with the Hirshfeld atom refinement technique to accurately determine the positions of hydrogen atoms from X-ray diffraction data. Given the reliability and quality of the obtained results, future applications of the current versions of the QM/ELMO embedding strategy to different types of chemical problems are to be expected in the near future. Moreover, further algorithmic improvements and methodological developments are also envisaged, such as the development of a polarizable QM/ELMO scheme accounting for the effects of the QM region on the ELMO subsystem or the use of the new embedding approach in the context of quantum crystallography to perform unprecedented accurate refinements of macromolecular crystal structures.

中文翻译：

QM / ELMO：基于极端局部分子轨道的多功能全量子力学嵌入方案

大型系统研究中计算上有利的方法的发展是理论化学中一个长期存在的研究主题。在这些技术中，从众所周知的QM / MM（量子力学/分子力学）方法到最新且很有前途的全量子力学方法，多尺度嵌入策略无疑占据了突出的位置。在这篇专题文章中，我们将简要回顾一下最近提出的QM / ELMO（量子力学/极端局限分子轨道）方案，即一种新的多尺度嵌入策略，其中，所研究系统的化学相关性最强的区域在全量子化学水平上进行处理。，而其余部分（即，（环境）的描述是通过极度局限的分子轨道来进行的，这些轨道在整个计算过程中保持冻结。除了强调理论基础之外，在这里我们还将回顾通过该新颖方法的所有当前可用变体获得的主要结果。特别是，我们将展示如何成功利用QM / ELMO嵌入方案来执行基态和激发态计算，并重现相应的全量子力学计算的结果，但计算成本要低得多。还将讨论晶体学的第一个应用，并且我们将描述QM / ELMO方法最近如何与Hirshfeld原子精制技术结合使用，以根据X射线衍射数据准确确定氢原子的位置。考虑到所获得结果的可靠性和质量，预计在不久的将来会将当前版本的QM / ELMO嵌入策略应用于不同类型的化学问题。此外，还设想了进一步的算法改进和方法学发展，例如考虑到QM区域对ELMO子系统的影响的可极化QM / ELMO方案的开发，或者在量子晶体学的背景下使用新的嵌入方法对大分子晶体结构进行前所未有的精确精制。

更新日期：2021-04-08

点击分享查看原文

点击收藏

阅读更多本刊最新论文