Strongly correlated electrons in the [Ni(hmp)(ROH)X]4 single molecule magnet:: A DFT+U study

被引：40

作者：

Cao, Chao ^{[1
,2
]}

Hill, Stephen ^{[1
]}

Cheng, Hai-Ping ^{[1
,2
]}

机构：

[1] Univ Florida, Dept Phys, Gainesville, FL 32611 USA

[2] Univ Florida, Quantum Theory Project, Gainesville, FL 32611 USA

来源：

PHYSICAL REVIEW LETTERS | 2008年 / 100卷 / 16期

基金：

美国国家科学基金会;

关键词：

D O I：

10.1103/PhysRevLett.100.167206

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

The single-molecule magnet [Ni(hmp)(MeOH)Cl](4) (hmp denotes the anion of 2-hydroxymethylpyridine and Me denotes methyl) is studied using both density functional theory (DFT) and the DFT+U method, and the results are compared. By incorporating a Hubbard-U like term for both the nickel and oxygen atoms, the experimentally determined ground state is successfully obtained, and the exchange coupling constants derived from the DFT+U calculation agree with experiment very well. The results show that the nickel 3d and oxygen 2p electrons in this molecule are strongly correlated, and thus the inclusion of on site Coulomb energies is crucial to obtaining the correct results.

引用

页数：4

共 34 条

[1] BAND THEORY AND MOTT INSULATORS - HUBBARD-U INSTEAD OF STONER-I [J].

ANISIMOV, VI ;

ZAANEN, J ;

ANDERSEN, OK .

PHYSICAL REVIEW B, 1991, 44 (03) :943-954

[2] Understanding the electronic structure, optical, and vibrational properties of the Fe8Br8 single-molecule magnet -: art. no. 214410 [J].

Baruah, T ;

Kortus, J ;

Pederson, MR ;

Wesolowski, R ;

Haraldsen, JT ;

Musfeldt, JL ;

North, JM ;

Zipse, D ;

Dalal, NS .

PHYSICAL REVIEW B, 2004, 70 (21) :1-9

[3] Electronic structure and magnetic anisotropy of the [Co4(hmp)4(CH3OH)4Cl4] molecule [J].

Baruah, T ;

Pederson, MR .

CHEMICAL PHYSICS LETTERS, 2002, 360 (1-2) :144-148

[4] Implementation of the projector augmented-wave LDA+U method:: Application to the electronic structure of NiO [J].

Bengone, O ;

Alouani, M ;

Blöchl, P ;

Hugel, J .

PHYSICAL REVIEW B, 2000, 62 (24) :16392-16401

[5] Electronic structure of a Mn12 molecular magnet:: Theory and experiment [J].

Boukhvalov, D. W. ;

Al-Saqer, M. ;

Kurmaev, E. Z. ;

Moewes, A. ;

Galakhov, V. R. ;

Finkelstein, L. D. ;

Chiuzbaian, S. ;

Neumann, M. ;

Dobrovitski, V. V. ;

Katsnelson, M. I. ;

Lichtenstein, A. I. ;

Harmon, B. N. ;

Endo, K. ;

North, J. M. ;

Dalal, N. S. .

PHYSICAL REVIEW B, 2007, 75 (01)

[6] ALTERNATING-CURRENT SUSCEPTIBILITY, HIGH-FIELD MAGNETIZATION, AND MILLIMETER BAND EPR EVIDENCE FOR A GROUND S = 10 STATE IN [MN12O12(CH3COO)16(H2O)4].2CH3COOH.4H2O [J].

CANESCHI, A ;

GATTESCHI, D ;

SESSOLI, R ;

BARRA, AL ;

BRUNEL, LC ;

GUILLOT, M .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1991, 113 (15) :5873-5874

[7] Linear response approach to the calculation of the effective interaction parameters in the LDA+U method [J].

Cococcioni, M ;

de Gironcoli, S .

PHYSICAL REVIEW B, 2005, 71 (03)

[8] Quantum superposition of high spin states in the single molecule magnet Ni4 -: art. no. 157202 [J].

del Barco, E ;

Kent, AD ;

Yang, EC ;

Hendrickson, DN .

PHYSICAL REVIEW LETTERS, 2004, 93 (15) :157202-1

[9] High-frequency electron paramagnetic resonance investigations of tetranuclear nickel-based single-molecule magnets [J].

Edwards, RS ;

Maccagnano, S ;

Yang, EC ;

Hill, S ;

Wernsdorfer, W ;

Hendrickson, D ;

Christou, G .

JOURNAL OF APPLIED PHYSICS, 2003, 93 (10) :7807-7809

[10]

*EPAPS, EPRLTAO100034815 EPA

← 1 2 3 4 →