Mononuclear Lanthanide Complexes: Use of the Crystal Field Theory to Design Single‐Ion Magnets and Spin Qubits

Clemente‐Juan, Juan M.; Coronado, Eugenio; Gaita‐Ariño, Alejandro

doi:10.1002/9783527673476.ch2

Cited by 18 publications

(11 citation statements)

References 83 publications

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“…Indeed, the ability to tune the spatial arrangement of more than one non-identical SIM qubit (in the present example three structurally distinguishable SIMs are present) is precisely what is currently needed to advance in the global control paradigm of quantum computing. 78 On the other hand, the incorporation of functional molecular species into the pores can provide a convenient way for introducing a second property into these hybrid materials. …”

Section: Mofs With Single-molecule Magnets At the Inorganic Nodesmentioning

confidence: 99%

Magnetic functionalities in MOFs: from the framework to the pore

2018

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In this review, we show the different approaches developed so far to prepare metal-organic frameworks (MOFs) presenting electronic functionalities, with particular attention to magnetic properties. We will cover the chemical design of frameworks necessary for the incorporation of different magnetic phenomena, as well as the encapsulation of functional species in their pores leading to hybrid multifunctional MOFs combining an extended lattice with a molecular lattice.

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Section: Mofs With Single-molecule Magnets At the Inorganic Nodesmentioning

confidence: 99%

Magnetic functionalities in MOFs: from the framework to the pore

2018

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“…From simple yet powerful electrostatic methods, 3,35 to computationally inexpensive CF approaches, 24,[36][37][38] to more computationally demanding ab initio CASSCF/RASSI methods, [39][40][41] there is a vibrant debate regarding the theoretical approaches to rationalizing -or predicting -the magnetic properties of Ln-SMMs. 8,[42][43][44] Ab initio CASSCF/RASSI methods have an intrinsically higher heuristic value as they aim for an accurate description of the wavefunctions, relying on virtually no empirical data beyond the atomic positions obtained from crystal structure determination.…”

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confidence: 99%

“…The energy barrier to magnetization reversal determined by an Arrhenius plot is reported to be . 4.8 meV 36,42,54,55.…”

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confidence: 99%

Magnetic Excitations in Polyoxotungstate-Supported Lanthanoid Single-Molecule Magnets: An Inelastic Neutron Scattering and ab Initio Study

et al. 2016

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Inelastic neutron scattering (INS) has been used to investigate the crystal field (CF) magnetic excitations of the analogs of the most representative lanthanoid-polyoxometalate single-molecule magnet family: Na[Ln(WO)] (Ln = Nd, Tb, Ho, Er). Ab initio complete active space self-consistent field/restricted active space state interaction calculations, extended also to the Dy analog, show good agreement with the experimentally determined low-lying CF levels, with accuracy better in most cases than that reported for approaches based only on simultaneous fitting to CF models of magnetic or spectroscopic data for isostructural Ln families. In this work we demonstrate the power of a combined spectroscopic and computational approach. Inelastic neutron scattering has provided direct access to CF levels, which together with the magnetometry data, were employed to benchmark the ab initio results. The ab initio determined wave functions corresponding to the CF levels were in turn employed to assign the INS transitions allowed by selection rules and interpret the observed relative intensities of the INS peaks. Ultimately, we have been able to establish the relationship between the wave function composition of the CF split Ln ground multiplets and the experimentally measured magnetic and spectroscopic properties for the various analogs of the Na[Ln(WO)] family.

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“…This can be successful for describing low-temperature properties, but inevitably fails for understanding the magnetic susceptibility, or the relaxation properties of SMMs [11,37,52]. Alternatively, semi-empirical models such as the point-charge model or improved versions of it [17,24,53] can be used, which promise fewer parameters, but introduce hard to control approximations. They thus typically need to be "calibrated" by a large data set, which may not be available [24].…”

Section: Challenges Of Analysismentioning

confidence: 99%

“…Alternatively, semi-empirical models such as the point-charge model or improved versions of it [17,24,53] can be used, which promise fewer parameters, but introduce hard to control approximations. They thus typically need to be "calibrated" by a large data set, which may not be available [24].…”

Section: Challenges Of Analysismentioning

confidence: 99%

Perspectives on Neutron Scattering in Lanthanide-Based Single-Molecule Magnets and a Case Study of the Tb2(μ-N2) System

et al. 2016

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Single-molecule magnets (SMMs) based on lanthanide ions display the largest known blocking temperatures and are the best candidates for molecular magnetic devices. Understanding their physical properties is a paramount task for the further development of the field. In particular, for the poly-nuclear variety of lanthanide SMMs, a proper understanding of the magnetic exchange interaction is crucial. We discuss the strengths and weaknesses of the neutron scattering technique in the study of these materials and particularly for the determination of exchange. We illustrate these points by presenting the results of a comprehensive inelastic neutron scattering study aimed at a radical-bridged diterbium(III) cluster, Tb 2 (µ-N 2 3−), which exhibits the largest blocking temperature for a poly-nuclear SMM. Results on the Y III analogue Y 2 (µ-N 2 3−) and the parent compound Tb 2 (µ-N 2 2−) (showing no SMM features) are also reported. The results on the parent compound include the first direct determination of the lanthanide-lanthanide exchange interaction in a molecular cluster based on inelastic neutron scattering. In the SMM compound, the resulting physical picture remains incomplete due to the difficulties inherent to the problem.

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Mononuclear Lanthanide Complexes: Use of the Crystal Field Theory to Design Single‐Ion Magnets and Spin Qubits

Cited by 18 publications

References 83 publications

Magnetic functionalities in MOFs: from the framework to the pore

Magnetic functionalities in MOFs: from the framework to the pore

Magnetic Excitations in Polyoxotungstate-Supported Lanthanoid Single-Molecule Magnets: An Inelastic Neutron Scattering and ab Initio Study

Perspectives on Neutron Scattering in Lanthanide-Based Single-Molecule Magnets and a Case Study of the Tb2(μ-N2) System

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