Strongly Correlated Electrons in the<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mo stretchy="false">[</mml:mo><mml:mi>Ni</mml:mi><mml:mo stretchy="false">(</mml:mo><mml:mi>hmp</mml:mi><mml:mo stretchy="false">)</mml:mo><mml:mo stretchy="false">(</mml:mo><mml:mi>R</mml:mi><mml:mi>OH</mml:mi><mml:mo stretchy="false">)</mml:mo><mml:mi mathvariant="normal">X</mml:mi><mml:msub><mml:mo stretchy="false">]</mml:mo><mml:mn>4</mml:mn></mml:msub></mml:math>Single Molecule Magnet: A<

Cao, Chao; Hill, Stephen; Cheng, Hai‐Ping

doi:10.1103/physrevlett.100.167206

Cited by 44 publications

(35 citation statements)

References 31 publications

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“…Such effects would results from self-consistent changes in the electronic wavefunctions. This observation is consistent with that of Chao et al [17] who found that inclusion of Hubbard U corrections for both Ni 3d and O 2p state are important in similar systems. Radon finds that the S = 2 (quintet) state is higher in energy by 0.8 eV if full Slater exchange is used in the B3LYP functional but lower in energy by 0.8 eV when full exact exchange is used instead.…”

Section: The S = 2 Porphyrin Structures: Flat Vs Bentsupporting

confidence: 82%

The Role of Self-Interaction Corrections, Vibrations, and Spin-Orbit in Determining the Ground Spin State in a Simple Heme

et al. 2017

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Without self-interaction corrections or the use of hybrid functionals, approximations to the density-functional theory (DFT) often favor intermediate spin systems over high-spin systems. In this paper, we apply the recently proposed Fermi-Löwdin-orbital self-interaction corrected density functional formalism to a simple tetra-coordinated Fe(II)-porphyrin molecule and show that the energetic orderings of the S = 1 and S = 2 spin states are changed qualitatively relative to the results of Generalized Gradient Approximation (developed by Perdew, Burke, and Ernzerhof, PBE-GGA) and Local Density Approximation (developed by Perdew and Wang, PW92-LDA). Because the energetics, associated with changes in total spin, are small, we have also calculated the second-order spin-orbit energies and the zero-point vibrational energies to determine whether such corrections could be important in metal-substituted porphins. Our results find that the size of the spin-orbit and vibrational corrections to the energy orderings are small compared to the changes due to the self-interaction correction. Spin dependencies in the Infrared (IR)/Raman spectra and the zero-field splittings are provided as a possible means for identifying the spin in porphyrins containing Fe(II).

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Section: The S = 2 Porphyrin Structures: Flat Vs Bentsupporting

confidence: 82%

The Role of Self-Interaction Corrections, Vibrations, and Spin-Orbit in Determining the Ground Spin State in a Simple Heme

et al. 2017

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“…al. [20] a Experimental data is taken from [28] b Experimental Data is taken from [29] c BSDFT calculation from ref [21] d BSDFT calculation from ref [16] Our calculated data agree with the experimental value to within 15%, for both molecule with and without Acetate Bridge, compare to 65% deviation given by broken symmetry Density Functional theory. …”

Section: Calculation Of J For Bimettalic Mn(iv) Complexes and Validatsupporting

confidence: 71%

“…al. [20] was used for the calculations. We applied Hubbard U parameter on Mn atom, as well on the ligand oxygen and nitrogen atoms, coordinating the Mn atom.…”

Section: Computational Detailsmentioning

confidence: 99%

Prediction of Exchange Coupling Constant for Mn12 Molecular Magnet Using Dft+U

Gangopadhyay

Masunov

Poalelungi

2009

Lecture Notes in Computer Science

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Abstract. Single-molecule magnets are perspective materials for molecular spintronic applications. Predictions of magnetic coupling in these systems have posed a long standing problem, as calculations of this kind require a balanced description of static and dynamic electron correlation. The large size of these systems limits the choice of theoretical methods used. Two methods feasible to predict the exchange coupling parameters are broken symmetry Density Functional Theory (BSDFT) and DFT with empirical Hubbard U parameter (DFT+U). In this contribution we apply DFT+U to study Mn-based molecular magnets using Vanderbilt Ultrasoft Pseudopotential plane wave DFT method, implemented in Quantum ESPRESSSO code. Unlike most previous studies, we adjust U parameters for both metal and ligand atoms using two dineuclear molecular magnets [

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“…Also, there are numerous evidences of the importance of the Hubbard term for oxygen [19][20][21] and nitrogen 22 atoms; the U value for oxygen ranging from 1.5 eV 22 to 8.5 eV. 19 C. Cao et al 20 found that increasing U for oxygen above 6 eV slightly effects on the magnetic coupling constant in single-molecule magnet Ni(hmp)(MeOH)Cl 4 . The corresponding Hubbard scheme accounting for U for 2p-electrons of oxygen was named DFT+U p+d (or DFT+U d +U p ).…”

Section: -mentioning

confidence: 99%

Exchange coupling transformations in Cu (II) heterospin complexes of “breathing crystals” under structural phase transitions

2015

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Family of "breathing crystals" is the polymer-chain complexes of Cu(hfac) 2 with nitroxides. The polymer chains consist of one-, two-or three-spin clusters. The "breathing crystals" experience simultaneous magnetic and Jahn-Teller type structural phase transitions with change of total cluster spin and drastic change of bond lengths (ca. 10-12%). For the first time the intra-cluster magnetic couplings in "breathing crystals" have been calculated both by band structure methods GGA+U and hybrid DFT (B3LYP and PBE0) for the isolated exchange clusters. The temperature dependence of the magnetic coupling constant was calculated for two polymer-chain compounds of the "breathing crystal" family -C 21 H 19 CuF 12 N 4 O 6 with the chains containing two-spin clusters and C 22 H 21 CuF 12 N 4 O 6 with the chains of alternating three-spin clusters and one-spin sites. It was found that adding a Hubbard-like parameter not only to the copper 3d electrons but also to the oxygen 2p electrons (GGA+U d +U p approach) results in an improved description of exchange coupling in the "breathing crystal" compounds. At the same time treatment of the isolated clusters by a large basis hybrid DFT with high computational cost provides a similar quality fit of the experimental magneto-chemical data as that for the GGA+U d +U p band structure calculation scheme. Our calculations also showed that in spite of the abrupt transformation of the magnetic coupling constant under the phase transition, the band gap in the "breathing crystals" remains about the same value with temperature decrease. C 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.

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Strongly Correlated Electrons in the[Ni(hmp)(ROH)X]4Single Molecule Magnet: A<

Cited by 44 publications

References 31 publications

The Role of Self-Interaction Corrections, Vibrations, and Spin-Orbit in Determining the Ground Spin State in a Simple Heme

The Role of Self-Interaction Corrections, Vibrations, and Spin-Orbit in Determining the Ground Spin State in a Simple Heme

Prediction of Exchange Coupling Constant for Mn12 Molecular Magnet Using Dft+U

Exchange coupling transformations in Cu (II) heterospin complexes of “breathing crystals” under structural phase transitions

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