修订后的 M06 密度泛函用于主族和过渡金属化学。
Revised M06 density functional for main-group and transition-metal chemistry.
机构信息
School of Chemistry and Molecular Engineering, Shanghai Engineering Research Center of Molecular Therapeutics and New Drug Development, East China Normal University, 200062 Shanghai, China.
State Key Laboratory of Precision Spectroscopy, East China Normal University, 200062 Shanghai, China.
出版信息
Proc Natl Acad Sci U S A. 2018 Oct 9;115(41):10257-10262. doi: 10.1073/pnas.1810421115. Epub 2018 Sep 20.
Abstract
We present a hybrid metageneralized-gradient-approximation functional, revM06, which is based on adding Hartree-Fock exchange to the revM06-L functional form. Compared with the original M06 suite of density functionals, the resulting revM06 functional has significantly improved across-the-board accuracy for both main-group and transition-metal chemistry. The revM06 functional improves on the M06-2X functional for main-group and transition-metal bond energies, atomic excitation energies, isomerization energies of large molecules, molecular structures, and both weakly and strongly correlated atomic and molecular data, and it shows a clear improvement over M06 and M06-2X for noncovalent interactions, including smoother potential curves for rare-gas dimers. The revM06 functional also predicts more accurate results than M06 and M06-2X for most of the outside-the-training-set test sets examined in this study. Therefore, the revM06 functional is well-suited for a broad range of chemical applications for both main-group and transition-metal elements.
摘要
我们提出了一种混合泛函，即 revM06，它基于在 revM06-L 泛函形式中添加 Hartree-Fock 交换。与原始的 M06 密度泛函套件相比，所得的 revM06 泛函对主族和过渡金属化学具有全面显著提高的准确性。revM06 泛函改进了 M06-2X 泛函在主族和过渡金属键能、原子激发能、大分子的异构化能、分子结构、弱和强相关的原子和分子数据方面的性能，并且在非共价相互作用方面表现出明显优于 M06 和 M06-2X 的性能，包括稀有气体二聚体的更平滑的势能曲线。在本研究中检查的大多数训练集外测试集中，revM06 泛函也预测出比 M06 和 M06-2X 更准确的结果。因此，revM06 泛函非常适合主族和过渡金属元素的广泛化学应用。
相似文献
1
Revised M06 density functional for main-group and transition-metal chemistry.修订后的 M06 密度泛函用于主族和过渡金属化学。
Proc Natl Acad Sci U S A. 2018 Oct 9;115(41):10257-10262. doi: 10.1073/pnas.1810421115. Epub 2018 Sep 20.
2
Density functionals with broad applicability in chemistry.在化学领域具有广泛适用性的密度泛函。
Acc Chem Res. 2008 Feb;41(2):157-67. doi: 10.1021/ar700111a. Epub 2008 Jan 11.
3
Revised M06-L functional for improved accuracy on chemical reaction barrier heights, noncovalent interactions, and solid-state physics.修正的 M06-L 泛函，提高化学反应势垒高度、非共价相互作用和固态物理的准确性。
Proc Natl Acad Sci U S A. 2017 Aug 8;114(32):8487-8492. doi: 10.1073/pnas.1705670114. Epub 2017 Jul 24.
4
Exploring the Limit of Accuracy of the Global Hybrid Meta Density Functional for Main-Group Thermochemistry, Kinetics, and Noncovalent Interactions.探索全局杂化泛函对主族热化学、动力学和非共价相互作用的精度极限。
J Chem Theory Comput. 2008 Nov 11;4(11):1849-68. doi: 10.1021/ct800246v.
5
How Accurate Are the Minnesota Density Functionals for Noncovalent Interactions, Isomerization Energies, Thermochemistry, and Barrier Heights Involving Molecules Composed of Main-Group Elements?对于涉及主族元素组成的分子的非共价相互作用、异构化能量、热化学和势垒高度，明尼苏达密度泛函的准确性如何？
J Chem Theory Comput. 2016 Sep 13;12(9):4303-25. doi: 10.1021/acs.jctc.6b00637. Epub 2016 Sep 2.
6
M06-SX screened-exchange density functional for chemistry and solid-state physics.M06-SX screened-exchange 密度泛函理论用于化学和固态物理。
Proc Natl Acad Sci U S A. 2020 Feb 4;117(5):2294-2301. doi: 10.1073/pnas.1913699117. Epub 2020 Jan 17.
7
On the Performances of the M06 Family of Density Functionals for Electronic Excitation Energies.关于M06族密度泛函在电子激发能方面的性能
J Chem Theory Comput. 2010 Jul 13;6(7):2071-85. doi: 10.1021/ct100119e. Epub 2010 May 26.
8
Design of Density Functionals by Combining the Method of Constraint Satisfaction with Parametrization for Thermochemistry, Thermochemical Kinetics, and Noncovalent Interactions.通过将约束满足方法与热化学、热化学动力学和非共价相互作用的参数化相结合来设计密度泛函
J Chem Theory Comput. 2006 Mar;2(2):364-82. doi: 10.1021/ct0502763.
9
MN15-L: A New Local Exchange-Correlation Functional for Kohn-Sham Density Functional Theory with Broad Accuracy for Atoms, Molecules, and Solids.MN15-L：一种用于Kohn-Sham密度泛函理论的新型局域交换关联泛函，对原子、分子和固体具有广泛的准确性。
J Chem Theory Comput. 2016 Mar 8;12(3):1280-93. doi: 10.1021/acs.jctc.5b01082. Epub 2016 Feb 2.
10
Zn Coordination Chemistry: Development of Benchmark Suites for Geometries, Dipole Moments, and Bond Dissociation Energies and Their Use To Test and Validate Density Functionals and Molecular Orbital Theory.锌配合物化学：用于测试和验证密度泛函和分子轨道理论的基准套件的开发，包括几何形状、偶极矩和键离解能。
J Chem Theory Comput. 2008 Jan;4(1):75-85. doi: 10.1021/ct700205n.
引用本文的文献
1
On the aromaticity and photophysics of 1-arylbenzo[]imidazo[5,1,2-]indolizines as bicolor fluorescent molecules for barium tagging in the study of double-beta decay of Xe.关于1-芳基苯并[]咪唑并[5,1,2-]中氮茚作为双色荧光分子用于氙双β衰变研究中钡标记的芳香性和光物理性质
Beilstein J Org Chem. 2025 Aug 13;21:1627-1638. doi: 10.3762/bjoc.21.126. eCollection 2025.
2
DFT investigation of therapeutic potential of benzimidazolone capsule as a drug delivery vehicle for anticancer drug.苯并咪唑酮胶囊作为抗癌药物递送载体的治疗潜力的密度泛函理论研究
Sci Rep. 2025 Aug 4;15(1):28383. doi: 10.1038/s41598-025-12817-7.
3
Accurate and Efficient Description of Acidic Zeolites with Plane-Wave Density Functional Theory Using Range-Separated Hybrid Functionals.使用范围分离混合泛函通过平面波密度泛函理论对酸性沸石进行准确高效的描述
Chemphyschem. 2025 Jun 30:e2500147. doi: 10.1002/cphc.202500147.
4
An Unusual Friedel-Crafts Reaction and Violation of the Markovnikov Rule in the Formation of an Adamantyl Arene.一种不寻常的傅克反应以及在金刚烷基芳烃形成过程中对马氏规则的违背
J Org Chem. 2025 Apr 25;90(16):5546-5549. doi: 10.1021/acs.joc.5c00215. Epub 2025 Apr 14.
5
Molecular insight into the role of benzotriazole nanocapsule to deliver anticancer drug in smart drug delivery system.关于苯并三唑纳米胶囊在智能药物递送系统中递送抗癌药物作用的分子见解。
Sci Rep. 2025 Apr 12;15(1):12636. doi: 10.1038/s41598-025-91719-0.
6
DABCO-Catalyzed Synthesis of Thiazolidine-2-thiones: System Development and Mechanistic Insights.1,4-二氮杂双环[2.2.2]辛烷催化合成噻唑烷-2-硫酮：体系开发与机理研究
J Org Chem. 2025 Mar 28;90(12):4302-4312. doi: 10.1021/acs.joc.5c00020. Epub 2025 Mar 19.
7
Theoretical Insight into Antioxidant Mechanism of Caffeic Acid Against Hydroperoxyl Radicals in Aqueous Medium at Different pH-Thermodynamic and Kinetic Aspects.不同pH值下咖啡酸在水介质中对抗氢过氧自由基抗氧化机制的理论洞察——热力学和动力学方面
Int J Mol Sci. 2024 Nov 27;25(23):12753. doi: 10.3390/ijms252312753.
8
Cooperative Catalysis in Stereoselective - and -Glycosylations with Glycosyl Trichloroacetimidates Mediated by Singly Protonated Phenanthrolinium Salt and Trichloroacetamide.单质子化菲咯啉鎓盐和三氯乙酰胺介导的糖基三氯乙酰亚胺酯立体选择性 - 和 - 糖基化反应中的协同催化作用
J Am Chem Soc. 2024 Dec 18;146(50):34413-34426. doi: 10.1021/jacs.4c10633. Epub 2024 Dec 4.
9
Why is thiol unexpectedly less reactive but more selective than alcohol in phenanthroline-catalyzed 1,2-- and -furanosylations?为什么在菲咯啉催化的1,2 - 以及 - 呋喃糖基化反应中，硫醇的反应活性出人意料地比醇低，但选择性却更高？
Org Biomol Chem. 2025 Jan 2;23(2):328-342. doi: 10.1039/d4ob01593b.
10
Revisiting a classic carbocation - DFT, coupled-cluster, and molecular dynamics computations on barbaralyl cation formation and rearrangements.重温经典碳正离子——关于巴巴拉烯基阳离子形成和重排的密度泛函理论、耦合簇理论及分子动力学计算
Chem Sci. 2024 Aug 27;15(38):15577-87. doi: 10.1039/d4sc04829f.
本文引用的文献
1
MN15: A Kohn-Sham global-hybrid exchange-correlation density functional with broad accuracy for multi-reference and single-reference systems and noncovalent interactions.MN15：一种具有广泛准确性的Kohn-Sham全局杂化交换相关密度泛函，适用于多参考和单参考系统以及非共价相互作用。
Chem Sci. 2016 Aug 1;7(8):5032-5051. doi: 10.1039/c6sc00705h. Epub 2016 Apr 6.
2
Calculation of Ligand Dissociation Energies in Large Transition-Metal Complexes.计算大过渡金属配合物中的配体离解能。
J Chem Theory Comput. 2018 May 8;14(5):2456-2468. doi: 10.1021/acs.jctc.8b00061. Epub 2018 Apr 13.
3
A look at the density functional theory zoo with the advanced GMTKN55 database for general main group thermochemistry, kinetics and noncovalent interactions.借助用于一般主族热化学、动力学和非共价相互作用的先进GMTKN55数据库审视密度泛函理论体系。
Phys Chem Chem Phys. 2017 Dec 13;19(48):32184-32215. doi: 10.1039/c7cp04913g.
4
Revised M06-L functional for improved accuracy on chemical reaction barrier heights, noncovalent interactions, and solid-state physics.修正的 M06-L 泛函，提高化学反应势垒高度、非共价相互作用和固态物理的准确性。
Proc Natl Acad Sci U S A. 2017 Aug 8;114(32):8487-8492. doi: 10.1073/pnas.1705670114. Epub 2017 Jul 24.
5
MN15-L: A New Local Exchange-Correlation Functional for Kohn-Sham Density Functional Theory with Broad Accuracy for Atoms, Molecules, and Solids.MN15-L：一种用于Kohn-Sham密度泛函理论的新型局域交换关联泛函，对原子、分子和固体具有广泛的准确性。
J Chem Theory Comput. 2016 Mar 8;12(3):1280-93. doi: 10.1021/acs.jctc.5b01082. Epub 2016 Feb 2.
6
Exploring the Limit of Accuracy of the Global Hybrid Meta Density Functional for Main-Group Thermochemistry, Kinetics, and Noncovalent Interactions.探索全局杂化泛函对主族热化学、动力学和非共价相互作用的精度极限。
J Chem Theory Comput. 2008 Nov 11;4(11):1849-68. doi: 10.1021/ct800246v.
7
Electronic Transition Energies: A Study of the Performance of a Large Range of Single Reference Density Functional and Wave Function Methods on Valence and Rydberg States Compared to Experiment.电子跃迁能量：与实验相比，对大量单参考密度泛函和波函数方法在价态和里德堡态上的性能研究。
J Chem Theory Comput. 2010 Feb 9;6(2):370-83. doi: 10.1021/ct9005129. Epub 2010 Jan 22.
8
New Benchmark Set of Transition-Metal Coordination Reactions for the Assessment of Density Functionals.用于评估密度泛函的过渡金属配位反应新基准集
J Chem Theory Comput. 2014 Aug 12;10(8):3092-103. doi: 10.1021/ct500248h. Epub 2014 Jul 3.
9
Performance of Density Functionals for Activation Energies of Zr-Mediated Reactions.密度泛函对锆介导反应活化能的性能研究
J Chem Theory Comput. 2013 Nov 12;9(11):4735-43. doi: 10.1021/ct400432x. Epub 2013 Oct 10.
10
Performance of Density Functionals for Activation Energies of Re-Catalyzed Organic Reactions.再催化有机反应活化能的密度泛函性能
J Chem Theory Comput. 2014 Feb 11;10(2):579-88. doi: 10.1021/ct4010855. Epub 2014 Jan 7.
Zotero 插件