We report the synthesis, characterization,
and magnetic properties
of eight neutral functionalized trigonal lanthanide coordination complexes
LnL with Ln = Gd (1), Tb (2), Dy (3), Ho (4), Er (5), Tm (6), Yb (7), Lu (8). These were prepared
through a one-pot synthesis where, first, the ligand H3L was synthesized in situ through a Schiff base
reaction of tris(2-aminoethyl)amine with 2,6-diformyl-p-cresol. Following addition of Ln(OTf)3·xH2O and base, LnL was obtained. Powder X-ray diffraction
confirms that all complexes are isostructural. LnL contain pendant,
noncoordinating carbonyl functions that are reactive and represent
direct anchoring points to appropriately functionalized surfaces.
Furthermore, these reactive carbonyl functions can be used to postfunctionalize
LnL: for example, with aromatic π systems. We present herein
the Schiff base condensation of 7 with benzylamine to
yield 9 as well as the characterization and magnetic
properties of 9. Our study establishes LnL as a truly
versatile module for the surface deposition of Ln-based single-ion
magnets.
Vibronic coupling, the interaction between molecular vibrations and electronic states, is a fundamental effect that profoundly affects chemical processes. In the case of molecular magnetic materials, vibronic, or spin-phonon, coupling leads to magnetic relaxation, which equates to loss of magnetic memory and loss of phase coherence in molecular magnets and qubits, respectively. The study of vibronic coupling is challenging, and most experimental evidence is indirect. Here we employ far-infrared magnetospectroscopy to directly probe vibronic transitions in [Yb(trensal)] (where H3trensal = 2,2,2-tris(salicylideneimino)trimethylamine). We find intense signals near electronic states, which we show arise due to an “envelope effect” in the vibronic coupling Hamiltonian, which we calculate fully ab initio to simulate the spectra. We subsequently show that vibronic coupling is strongest for vibrational modes that simultaneously distort the first coordination sphere and break the C3 symmetry of the molecule. With this knowledge, vibrational modes could be identified and engineered to shift their energy towards or away from particular electronic states to alter their impact. Hence, these findings provide new insights towards developing general guidelines for the control of vibronic coupling in molecules.
We report the synthesis, characterisation and magnetic properties of six novel neutral lanthanide cryptate coordination complexes. Reaction of 2,6-diformyl-4-methylphenol, tris(2-aminoethyl)amine and Ln(OTf)39H2O in the ratio 3:2:1, respectively, and in the...
Nuclear spins are candidates to encode qubits or qudits due to their isolation from magnetic noise and potentially long coherence times. However, their weak coupling to external stimuli makes them hard to integrate into circuit quantum electrodynamics architectures, the leading technology for solid-state quantum processors. Here, we study the coupling of 173Yb(III) nuclear spin states in an [Yb(trensal)] molecule to superconducting cavities. Experiments have been performed on magnetically dilute single crystals placed on the inductors of lumped-element LC superconducting resonators with characteristic frequencies spanning the range of nuclear and electronic spin transitions. We achieve a high cooperative coupling to all electronic and most nuclear [173Yb(trensal)] spin transitions, a necessary ingredient for the implementation of qudit protocols with molecular spins using a hybrid architecture.
Magnetochiral Dichroism of chiral mononuclear lanthanoid complexes is for the first time detected by X-ray absorption measurements on single crystals of Holmium oxydiacetate, at the Ho L3-edge. The effect is of opposite sign for the two enantiomers.
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