On the calculation of second-order magnetic properties using subsystem approaches in the relativistic framework

Malgorzata Olejniczak 1 Radovan Bast 2 Andre Severo Pereira Gomes 1, *
* Auteur correspondant
1 PCMT - Physico-Chimie Moléculaire Théorique
PhLAM - Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523
2 High performance Computing Group
UiT - University of Tromsø
Abstract : We report an implementation of the nuclear magnetic resonance (NMR) shielding (σ), isotope-independent indirect spin-spin coupling (K) and the magnetizability (χ) tensors in the frozen density embedding (FDE) scheme using the four-component (4c) relativistic Dirac--Coulomb (DC) Hamiltonian and the non-collinear spin density functional theory (SDFT). The formalism takes into account the magnetic balance between the large and the small components of molecular spinors and assures the gauge-origin independence of NMR shielding and magnetizability results. This implementation has been applied to hydrogen-bonded HXH⋯OH2 complexes (X = Se, Te, Po) and compared with the supermolecular calculations and with the approach based on the integration of the magnetically induced current density vector. A comparison with the approximate Zeroth-Order Regular Approximation (ZORA) Hamiltonian indicates non-negligible differences in σ and K in the HPoH⋯OH2 complex, and calls for a thourough comparison of ZORA and DC in the description of environment effects on NMR parameters for molecular systems with heavy elements.
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Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2017, 19, pp.8400-8415. 〈10.1039/C6CP08561J〉
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Soumis le : samedi 21 janvier 2017 - 12:19:47
Dernière modification le : jeudi 6 septembre 2018 - 15:12:04

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Malgorzata Olejniczak, Radovan Bast, Andre Severo Pereira Gomes. On the calculation of second-order magnetic properties using subsystem approaches in the relativistic framework. Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2017, 19, pp.8400-8415. 〈10.1039/C6CP08561J〉. 〈hal-01442808〉

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