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DOE OSTI · 1899421

Strong Relativistic Effects in Lanthanide-Based Single-Molecule Magnets

Dergachev, Vsevolod D.·Nakritskaia, Daria D.·Varganov, Sergey A.
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Abstract

Lanthanide-based single-molecule magnets (SMMs) are promising building blocks for quantum memory and spintronic devices. Designing lanthanide-based SMMs with long spin relaxation time requires a detailed understanding of their electronic structure, including the crucial role of the spin-orbit coupling (SOC). While traditional calculations of SOC using the perturbation theory applied to a solution of the non-relativistic Schrödinger equation are valid for light atoms, this approach is questionable for systems containing heavy elements such as lanthanides. We investigate the accuracy of the perturbation estimates of SOC by variationally solving the Dirac equation for the [DyO] + molecule, a prototype of a lanthanide-based SMM. We show that the energy splittings between the M J states involved in spin relaxation depend on the interplay between strong SOC and dynamic electron correlations. Here, we demonstrate that this interplay affects the resonances between the spin and vibrational transitions, and, therefore, the spin relaxation time.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYDirac equationcrystal field splittingmagnetic anisotropyperturbation theoryspin-orbit couplingspin-vibrational coupling

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Dergachev, Vsevolod D., Nakritskaia, Daria D., Varganov, Sergey A.. 2022-07-19. Strong Relativistic Effects in Lanthanide-Based Single-Molecule Magnets. https://doi.org/10.1021/acs.jpclett.2c01627

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