Intra- and Interatomic Spin Interactions by the Density Functional Theory plus U Approach: A Critical Assessment

doi:10.1021/ct200299s

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	Intra- and Interatomic Spin Interactions by the Density Functional Theory plus U Approach: A Critical Assessment
	Zhang, Yachao; Jiang, Hong
刊名	JOURNAL OF CHEMICAL THEORY AND COMPUTATION
	2011-09-01
卷号	7 期号:9 页码:2795-2803
ISSN号	1549-9618
DOI	10.1021/ct200299s
英文摘要	Accurate evaluation of the total energy difference between different spin states in molecular magnetic systems is currently a great challenge in theoretical chemistry. In this work we assess the performance of the density functional theory plus the Hubbard U (DFT+U) approach for the first-principles description of the high spin-low spin (HS-LS) Splitting and the exchange coupling constant, corresponding to the intra- and interatomic spin interactions, respectively. The former is investigated using a set of mononuclear ion complexes with different HS-LS splitting, including seven spin-crossover (SCO) compounds, while the latter is investigated in a series of binuclear copper complexes covering both ferromagnetic and antiferromagnetic interactions. We find that the DFT+U approach can reproduce experimental data as accurately as the hybrid functionals approach but with much lower computational efforts. We further analyze the effect of U in. terms of spin density on magnetic centers, and we find that the main effect of the U correction can be attributed to the enhanced localization of magnetic orbitals. Even taking the uncertainty related to the determination of U into account, we think the DFT+U approach is an efficient and predictive first-principles method for the SCO phenomenon and interatomic magnetic interactions.
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000294790400017
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/71949]
专题	中国科学院化学研究所
通讯作者	Jiang, Hong
作者单位	Peking Univ, State Key Lab Rare Earth Mat Chem & Applicat, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Yachao,Jiang, Hong. Intra- and Interatomic Spin Interactions by the Density Functional Theory plus U Approach: A Critical Assessment[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2011,7(9):2795-2803.
APA	Zhang, Yachao,&Jiang, Hong.(2011).Intra- and Interatomic Spin Interactions by the Density Functional Theory plus U Approach: A Critical Assessment.JOURNAL OF CHEMICAL THEORY AND COMPUTATION,7(9),2795-2803.
MLA	Zhang, Yachao,et al."Intra- and Interatomic Spin Interactions by the Density Functional Theory plus U Approach: A Critical Assessment".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 7.9(2011):2795-2803.