Journal
CHEMICAL SCIENCE
Volume 5, Issue 4, Pages 1650-1660Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3sc53044b
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Funding
- Swiss National Science Foundation
- Danish Ministry of Science, Innovation and Higher Education
- Danish Research Council FNU [12-125226]
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We study the ligand-field splittings and magnetic properties of three Er-III single-ion magnets which differ in the peripheral ligand sphere but exhibit similar first coordination spheres by inelastic neutron scattering (INS) and SQUID magnetometry. The INS spectra of the three compounds are profoundly different pointing at a strong response of the magnetic behavior tominor structural changes, as they are e. g. encountered when depositing molecules on surfaces. The observation of several magnetic excitations within the J = 15/2 ground multiplet together with single-crystal magnetic measurements allows for the extraction of the sign and magnitude of all symmetry-allowed Stevens parameters. The parameter values and the energy spectrum derived from INS are compared to the results of state-of-the-art ab initio CASSCF calculations. Temperature-dependent alternating current (ac) susceptibility measurements suggest that the magnetisation relaxation in the investigated temperature range of 1.9 K < T < 5 K is dominated by quantum tunnelling of magnetisation and two-phonon Raman processes. The possibility of observing electron paramagnetic resonance transitions between the ground-state doublet states, which can be suppressed in perfectly axial single-ion magnets, renders the studied systems interesting as representations of quantum bits.
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