Spin-forbidden transitions in the molecular nanomagnet V-15

Gysler M, Schlegel C, Mitra T, Müller A, Krebs B, van Slageren J. Spin-forbidden transitions in the molecular nanomagnet V-15. Physical Review B. 2014;90(14): 144405.We performed electron spin-resonance measurements on single crystals of the molecular nanomagnet V-15 using a novel broadband spectrometer, both in parallel and in perpendicular modes, we see (B-1 parallel to B-0, B-1 perpendicular to B-0). Measurements were carried out in proximity of the spin level crossing at B-0 = 2.75 T. We observed spin-forbidden transitions from the S = 1/2 zero-field ground state to the S = 3/2 excited state in parallel mode spectra. Spin-forbidden transitions are employed for switching of coherent interactions between qubits in recent quantum simulator proposals. Our theoretical investigations showed that the mixing of spin states can result from either an antisymmetric exchange interaction or a combination of static distortion and hyperfine interaction

Multitechnique investigation of Dy 3 – implications for coupled lanthanide clusters

International audienc

Multitechnique investigation of Dy3-implications for coupled lanthanide clusters

In-depth investigations of the low energy electronic structures of mononuclear lanthanide complexes, including single molecule magnets, are challenging at the best of times. For magnetically coupled polynuclear systems, the task seems well nigh impossible. However, without detailed understanding of the electronic structure, there is no hope of understanding their static and dynamic magnetic properties in detail. We have been interested in assessing which techniques are most appropriate for studying lanthanide single-molecule magnets. Here we present a wide ranging theoretical and experimental study of the archetypal polynuclear lanthanide single-molecule magnet Dy3 and derive the simplest model to describe the results from each experimental method, including high-frequency electron paramagnetic resonance and far-infrared spectroscopies and cantilever torque magnetometry. We conclude that a combination of these methods together with ab initio calculations is required to arrive at a full understanding of the properties of this complex, and potentially of other magnetically coupled lanthanide complexes.crosscheck: This document is CrossCheck deposited related_data: Supplementary Information identifier: Liviu Ungur (ORCID) identifier: Liviu Ungur (ResearcherID) copyright_licence: The Royal Society of Chemistry has an exclusive publication licence for this journal copyright_licence: This article is freely available. This article is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported Licence (CC BY-NC 3.0) history: Received 22 January 2016; Accepted 16 March 2016; Accepted Manuscript published 16 March 2016; Advance Article published 29 March 2016; Version of Record published 21 June 2016status: publishe

Multitechnique investigation of Dy3-implications for coupled lanthanide clusters

10.1039/c6sc00318dCHEMICAL SCIENCE774347-435

Determination of the electronic structure of a dinuclear dysprosium single molecule magnet without symmetry idealization

International audienc

Comprehensive Spectroscopic Determination of the Crystal Field Splitting in an Erbium Single-Ion Magnet

The electronic structure of a novel lanthanide-based single-ion magnet, {C­(NH₂)₃}₅[Er­(CO₃)₄]·11H₂O, was comprehensively studied by means of a large number of different spectroscopic techniques, including far-infrared, optical, and magnetic resonance spectroscopies. A thorough analysis, based on crystal field theory, allowed an unambiguous determination of all relevant free ion and crystal field parameters. We show that inclusion of methods sensitive to the nature of the lowest-energy states is essential to arrive at a correct description of the states that are most relevant for the static and dynamic magnetic properties. The spectroscopic investigations also allowed for a full understanding of the magnetic relaxation processes occurring in this system. Thus, the importance of spectroscopic studies for the improvement of single-molecule magnets is underlined

Determination of the electronic structure of a dinuclear dysprosium single molecule magnet without symmetry idealization

We present the in-depth determination of the magnetic properties and electronic structure of the luminescent and volatile dysprosium-based single molecule magnet [Dy2(bpm)(fod)6] (Hfod = 6,6,7,7,8,8,8-heptafluoro-2,2-dimethyl-3,5-octanedione, bpm = 2,2'-bipyrimidine). Ab initio calculations were used to obtain a global picture of the electronic structure and to predict possible single molecule magnet behaviour, confirmed by experiments. The orientation of the susceptibility tensor was determined by means of cantilever torque magnetometry. An experimental determination of the electronic structure of the lanthanide ion was obtained combining Luminescence, Far Infrared and Magnetic Circular Dichroism spectroscopies. Fitting these energies to the full single ion plus crystal field Hamiltonian allowed determination of the eigenstates and crystal field parameters of a lanthanide complex without symmetry idealization. We then discuss the impact of a stepwise symmetry idealization on the modelling of the experimental data. This result is particularly important in view of the misleading outcomes that are often obtained when the symmetry of lanthanide complexes is idealized.status: publishe