A New Family of Nonempirical Range-Separated Functionals: RSX-r2SCAN, RSX-r2SCAN0, and RSX-r2SCAN-QIDH

IF 5.8 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2026-10-15 DOI:10.1021/acs.jctc.6c01471

P. Maiz-Pastor,E. Brémond,A. J. Pérez-Jiménez,C. Adamo,J. C. Sancho-García

{"title":"A New Family of\nNonempirical Range-Separated Functionals:\nRSX-r2SCAN, RSX-r2SCAN0, and RSX-r2SCAN-QIDH","authors":"P. Maiz-Pastor,E. Brémond,A. J. Pérez-Jiménez,C. Adamo,J. C. Sancho-García","doi":"10.1021/acs.jctc.6c01471","DOIUrl":null,"url":null,"abstract":"Abstract We extend the restored-regularized Strongly Constrained and Appropriately Normed (r2SCAN) nonempirical exchange-correlation functional to the Range-Separation eXchange (RSX) scheme, RSX-r2SCAN, where the range-separation parameter (ω) is obtained by applying a first-principles constraint, thus not relying on any empirical fitting. The corresponding exchange-correlation hybrid (i.e., RSX-r2SCAN0) and double-hybrid (i.e., RSX-r2SCAN-QIDH) versions are also built following this procedure, concomitantly assessing all the models on relevant systems (e.g., increasingly larger clusters of noninteracting He atoms) and a large data set of ionization potentials (e.g., GW100). The assessment is also done using the GMTKN55 database for general main-group thermochemistry, kinetics, and noncovalent interactions, along with the WTMAD-2 error metric and a more recent one called WTMAD-4. The assessment is completed with a detailed analysis of some of the GMTKN55 subsets most affected by self-interaction errors. Finally, the models are coupled to the VV10 correlation energy functional (RSX-r2SCAN-NL, r2SCAN0-NL, and RSX-r2SCAN-QIDH-NL) for nonlocal and long-range electronic effects, to accurately address noncovalently bound systems as well.","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":"64 1","pages":""},"PeriodicalIF":5.8000,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.6c01471","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

Abstract We extend the restored-regularized Strongly Constrained and Appropriately Normed (r2SCAN) nonempirical exchange-correlation functional to the Range-Separation eXchange (RSX) scheme, RSX-r2SCAN, where the range-separation parameter (ω) is obtained by applying a first-principles constraint, thus not relying on any empirical fitting. The corresponding exchange-correlation hybrid (i.e., RSX-r2SCAN0) and double-hybrid (i.e., RSX-r2SCAN-QIDH) versions are also built following this procedure, concomitantly assessing all the models on relevant systems (e.g., increasingly larger clusters of noninteracting He atoms) and a large data set of ionization potentials (e.g., GW100). The assessment is also done using the GMTKN55 database for general main-group thermochemistry, kinetics, and noncovalent interactions, along with the WTMAD-2 error metric and a more recent one called WTMAD-4. The assessment is completed with a detailed analysis of some of the GMTKN55 subsets most affected by self-interaction errors. Finally, the models are coupled to the VV10 correlation energy functional (RSX-r2SCAN-NL, r2SCAN0-NL, and RSX-r2SCAN-QIDH-NL) for nonlocal and long-range electronic effects, to accurately address noncovalently bound systems as well.

查看原文本刊更多论文

一类新的非经验范围分离泛函：RSX-r2SCAN、RSX-r2SCAN0和RSX-r2SCAN- qidh

摘要将恢复正则化强约束适当赋范（r2SCAN）非经验交换相关泛函扩展到距离分离交换（RSX）格式RSX-r2SCAN，其中距离分离参数（ω）是通过应用第一原理约束获得的，因此不依赖于任何经验拟合。相应的交换相关杂化（即RSX-r2SCAN0）和双杂化（即RSX-r2SCAN-QIDH）版本也按照此程序构建，同时评估相关系统（例如，越来越大的非相互作用He原子簇）和大型电离势数据集（例如，GW100）上的所有模型。评估还使用GMTKN55数据库进行一般主群热化学，动力学和非共价相互作用，以及WTMAD-2误差度量和最近的WTMAD-4。通过对一些受自交互误差影响最大的GMTKN55子集的详细分析，完成了评估。最后，将模型与VV10相关能函数（RSX-r2SCAN-NL， r2SCAN0-NL和RSX-r2SCAN-QIDH-NL）耦合，用于非局部和远程电子效应，以准确地解决非共价结合系统。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Chemical Theory and Computation 化学-物理：原子、分子和化学物理

CiteScore

9.90

自引率

16.40%

发文量

568

审稿时长

1 months

期刊介绍： The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.