TY  - DATA
AU  - Garcia-Fernandez, Pablo
AU  - Antonio Aramburu, Jose
AU  - Moreno, Miguel
AU  - Zlatar, Matija
AU  - Gruden-Pavlović, Maja
PY  - 2014
UR  - https://cherry.chem.bg.ac.rs/handle/123456789/3667
PB  - Amer Chemical Soc, Washington
T2  - Journal of Chemical Theory and Computation
T1  - Supplementary data for the article: García-Fernández, P.; Aramburu, J. A.; Moreno, M.; Zlatar, M.; Gruden-Pavlović, M. A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. Journal of Chemical Theory and Computation 2014, 10 (4), 1824–1833. https://doi.org/10.1021/ct4011097
UR  - https://hdl.handle.net/21.15107/rcub_cherry_3667
ER  - 

@misc{
author = "Garcia-Fernandez, Pablo and Antonio Aramburu, Jose and Moreno, Miguel and Zlatar, Matija and Gruden-Pavlović, Maja",
year = "2014",
publisher = "Amer Chemical Soc, Washington",
journal = "Journal of Chemical Theory and Computation",
title = "Supplementary data for the article: García-Fernández, P.; Aramburu, J. A.; Moreno, M.; Zlatar, M.; Gruden-Pavlović, M. A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. Journal of Chemical Theory and Computation 2014, 10 (4), 1824–1833. https://doi.org/10.1021/ct4011097",
url = "https://hdl.handle.net/21.15107/rcub_cherry_3667"
}

Garcia-Fernandez, P., Antonio Aramburu, J., Moreno, M., Zlatar, M.,& Gruden-Pavlović, M.. (2014). Supplementary data for the article: García-Fernández, P.; Aramburu, J. A.; Moreno, M.; Zlatar, M.; Gruden-Pavlović, M. A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. Journal of Chemical Theory and Computation 2014, 10 (4), 1824–1833. https://doi.org/10.1021/ct4011097. in Journal of Chemical Theory and Computation
Amer Chemical Soc, Washington..
https://hdl.handle.net/21.15107/rcub_cherry_3667

Garcia-Fernandez P, Antonio Aramburu J, Moreno M, Zlatar M, Gruden-Pavlović M. Supplementary data for the article: García-Fernández, P.; Aramburu, J. A.; Moreno, M.; Zlatar, M.; Gruden-Pavlović, M. A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. Journal of Chemical Theory and Computation 2014, 10 (4), 1824–1833. https://doi.org/10.1021/ct4011097. in Journal of Chemical Theory and Computation. 2014;.
https://hdl.handle.net/21.15107/rcub_cherry_3667 .

Garcia-Fernandez, Pablo, Antonio Aramburu, Jose, Moreno, Miguel, Zlatar, Matija, Gruden-Pavlović, Maja, "Supplementary data for the article: García-Fernández, P.; Aramburu, J. A.; Moreno, M.; Zlatar, M.; Gruden-Pavlović, M. A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. Journal of Chemical Theory and Computation 2014, 10 (4), 1824–1833. https://doi.org/10.1021/ct4011097" in Journal of Chemical Theory and Computation (2014),
https://hdl.handle.net/21.15107/rcub_cherry_3667 .

TY  - JOUR
AU  - Garcia-Fernandez, Pablo
AU  - Antonio Aramburu, Jose
AU  - Moreno, Miguel
AU  - Zlatar, Matija
AU  - Gruden-Pavlović, Maja
PY  - 2014
UR  - https://cherry.chem.bg.ac.rs/handle/123456789/1765
AB  - Vibronic coupling theory shows that the cause for spontaneous instability in systems presenting a nondegenerate ground state is the so-called pseudo-Jahn-Teller effect, and thus its study can be extremely helpful to understand the structure of many molecules. While this theory, based on the mixing of the ground and excited states with a distortion, has been long studied, there are two obscure points that we try to clarify in the present work. First, the operators involved in both the vibronic and nonvibronic parts of the force constant take only into account electron nuclear and nuclear nuclear interactions, apparently leaving electron electron repulsions and the electron's kinetic energy out of the chemical picture. Second, a fully quantitative computational appraisal of this effect has been up to now problematic. Here, we present a reformulation of the pseudo-Jahn-Teller theory that explicitly shows the contributions of all operators in the molecular Hamiltonian and allows connecting the results obtained with this model to other chemical theories relating electron distribution and geometry. Moreover, we develop a practical approach based on Hartree-Fock and density functional theory that allows quantification of the pseudo-Jahn-Teller effect. We demonstrate the usefulness of our method studying the pyramidal distortion in ammonia and its absence in borane, revealing the strong importance of the kinetic energy of the electrons in the lowest a(2)'' orbital to trigger this instability. The present tool opens a window for exploring in detail the actual microscopic origin of structural instabilities in molecules and solids.
PB  - Amer Chemical Soc, Washington
T2  - Journal of Chemical Theory and Computation
T1  - A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect
VL  - 10
IS  - 4
SP  - 1824
EP  - 1833
DO  - 10.1021/ct4011097
ER  - 

@article{
author = "Garcia-Fernandez, Pablo and Antonio Aramburu, Jose and Moreno, Miguel and Zlatar, Matija and Gruden-Pavlović, Maja",
year = "2014",
abstract = "Vibronic coupling theory shows that the cause for spontaneous instability in systems presenting a nondegenerate ground state is the so-called pseudo-Jahn-Teller effect, and thus its study can be extremely helpful to understand the structure of many molecules. While this theory, based on the mixing of the ground and excited states with a distortion, has been long studied, there are two obscure points that we try to clarify in the present work. First, the operators involved in both the vibronic and nonvibronic parts of the force constant take only into account electron nuclear and nuclear nuclear interactions, apparently leaving electron electron repulsions and the electron's kinetic energy out of the chemical picture. Second, a fully quantitative computational appraisal of this effect has been up to now problematic. Here, we present a reformulation of the pseudo-Jahn-Teller theory that explicitly shows the contributions of all operators in the molecular Hamiltonian and allows connecting the results obtained with this model to other chemical theories relating electron distribution and geometry. Moreover, we develop a practical approach based on Hartree-Fock and density functional theory that allows quantification of the pseudo-Jahn-Teller effect. We demonstrate the usefulness of our method studying the pyramidal distortion in ammonia and its absence in borane, revealing the strong importance of the kinetic energy of the electrons in the lowest a(2)'' orbital to trigger this instability. The present tool opens a window for exploring in detail the actual microscopic origin of structural instabilities in molecules and solids.",
publisher = "Amer Chemical Soc, Washington",
journal = "Journal of Chemical Theory and Computation",
title = "A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect",
volume = "10",
number = "4",
pages = "1824-1833",
doi = "10.1021/ct4011097"
}

Garcia-Fernandez, P., Antonio Aramburu, J., Moreno, M., Zlatar, M.,& Gruden-Pavlović, M.. (2014). A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. in Journal of Chemical Theory and Computation
Amer Chemical Soc, Washington., 10(4), 1824-1833.
https://doi.org/10.1021/ct4011097

Garcia-Fernandez P, Antonio Aramburu J, Moreno M, Zlatar M, Gruden-Pavlović M. A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect. in Journal of Chemical Theory and Computation. 2014;10(4):1824-1833.
doi:10.1021/ct4011097 .

Garcia-Fernandez, Pablo, Antonio Aramburu, Jose, Moreno, Miguel, Zlatar, Matija, Gruden-Pavlović, Maja, "A Practical Computational Approach to Study Molecular Instability Using the Pseudo-Jahn-Teller Effect" in Journal of Chemical Theory and Computation, 10, no. 4 (2014):1824-1833,
https://doi.org/10.1021/ct4011097 . .

TY  - JOUR
AU  - Gruden-Pavlović, Maja
AU  - Perić, Marko
AU  - Zlatar, Matija
AU  - Garcia-Fernandez, Pablo
PY  - 2014
UR  - https://cherry.chem.bg.ac.rs/handle/123456789/1512
AB  - Magnetic molecules that present a slow decay of their magnetization (molecular magnets) are very interesting both from a fundamental and applied points of view. While many approaches focus strongly on finding systems with strong magnetic anisotropy giving rise to large spin-reversal barriers, less is known on the behavior of magnetic tunnelling, which is also a fundamental component of molecular magnet behavior. In this work, we propose a model to describe both the spin-reversal barrier and magnetic tunnelling in Ni(II) trigonal bipyramidal complexes, which could be easily extended to other transitionmetal systems. Based on this model, we show the criteria that lead to the optimal complexes to find molecular magnet behavior. We test our proposal with multi-reference configuration-interaction (MRCI) and ligand-field-density-functional-theory (LF-DFT) first-principles calculations applied over several families of mononuclear Ni(II) complexes. As a salient result, we find that the complex [NiCl3(Hdabco)(2)](+) (dabco is 1,4-diazabicyclo[2.2.2]-octane) displays both a very large magnetic anisotropy energy, 524 cm(-1), and a small tunnelling splitting, 0.2 cm(-1), when compared to other systems containing the same metal. We expect molecular magnet behaviour to be observed when small magnetic fields are employed to disrupt tunnelling. These values are reached due to the choice of ligands that favor a complete destruction of the Jahn-Teller distortions through spin-orbit coupling and an unquenched orbital momentum.
PB  - Royal Soc Chemistry, Cambridge
T2  - Chemical Science
T1  - Theoretical study of the magnetic anisotropy and magnetic tunnelling in mononuclear Ni(II) complexes with potential molecular magnet behavior
VL  - 5
IS  - 4
SP  - 1453
EP  - 1462
DO  - 10.1039/c3sc52984c
ER  - 

@article{
author = "Gruden-Pavlović, Maja and Perić, Marko and Zlatar, Matija and Garcia-Fernandez, Pablo",
year = "2014",
abstract = "Magnetic molecules that present a slow decay of their magnetization (molecular magnets) are very interesting both from a fundamental and applied points of view. While many approaches focus strongly on finding systems with strong magnetic anisotropy giving rise to large spin-reversal barriers, less is known on the behavior of magnetic tunnelling, which is also a fundamental component of molecular magnet behavior. In this work, we propose a model to describe both the spin-reversal barrier and magnetic tunnelling in Ni(II) trigonal bipyramidal complexes, which could be easily extended to other transitionmetal systems. Based on this model, we show the criteria that lead to the optimal complexes to find molecular magnet behavior. We test our proposal with multi-reference configuration-interaction (MRCI) and ligand-field-density-functional-theory (LF-DFT) first-principles calculations applied over several families of mononuclear Ni(II) complexes. As a salient result, we find that the complex [NiCl3(Hdabco)(2)](+) (dabco is 1,4-diazabicyclo[2.2.2]-octane) displays both a very large magnetic anisotropy energy, 524 cm(-1), and a small tunnelling splitting, 0.2 cm(-1), when compared to other systems containing the same metal. We expect molecular magnet behaviour to be observed when small magnetic fields are employed to disrupt tunnelling. These values are reached due to the choice of ligands that favor a complete destruction of the Jahn-Teller distortions through spin-orbit coupling and an unquenched orbital momentum.",
publisher = "Royal Soc Chemistry, Cambridge",
journal = "Chemical Science",
title = "Theoretical study of the magnetic anisotropy and magnetic tunnelling in mononuclear Ni(II) complexes with potential molecular magnet behavior",
volume = "5",
number = "4",
pages = "1453-1462",
doi = "10.1039/c3sc52984c"
}

Gruden-Pavlović, M., Perić, M., Zlatar, M.,& Garcia-Fernandez, P.. (2014). Theoretical study of the magnetic anisotropy and magnetic tunnelling in mononuclear Ni(II) complexes with potential molecular magnet behavior. in Chemical Science
Royal Soc Chemistry, Cambridge., 5(4), 1453-1462.
https://doi.org/10.1039/c3sc52984c

Gruden-Pavlović M, Perić M, Zlatar M, Garcia-Fernandez P. Theoretical study of the magnetic anisotropy and magnetic tunnelling in mononuclear Ni(II) complexes with potential molecular magnet behavior. in Chemical Science. 2014;5(4):1453-1462.
doi:10.1039/c3sc52984c .

Gruden-Pavlović, Maja, Perić, Marko, Zlatar, Matija, Garcia-Fernandez, Pablo, "Theoretical study of the magnetic anisotropy and magnetic tunnelling in mononuclear Ni(II) complexes with potential molecular magnet behavior" in Chemical Science, 5, no. 4 (2014):1453-1462,
https://doi.org/10.1039/c3sc52984c . .