期刊
PHYSICAL REVIEW MATERIALS
卷 2, 期 2, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevMaterials.2.024405
关键词
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资金
- US National Science Foundation [DMR-1610226]
- Air Force Office of Scientific Research (Asian Office of Aerospace Research and Development) [FA2386-17-1-4040]
- Italian Ministry of Education and Research (MIUR) though the PRIN Project [2015HYFSRT]
- Australian Research Council [DP15010325]
- National Science Foundation [DMR-1157490]
- State of Florida
- [ANR-13-BS10-0001-03 MolQuSpin]
- [DFG-TR 88]
Recent studies have highlighted the importance of organic ligands in the field of molecular spintronics, via which delocalized electron-spin density can mediate magnetic coupling to otherwise localized 4f moments of lanthanide ions, which show tremendous potential for single-molecule device applications. To this end, high-field/ high-frequency electron paramagnetic resonance (EPR) spectroscopy is employed to study a neutral terbium bis-phthalocyaninato metalorganic complex, [TbPc2](0), with the aim of understanding the magnetic interaction between the Ising-like moment of the lanthanide ion and the unpaired spin density on the coordinating organic radical ligand. The measurements were performed on a previously unknown[TbPc2](0) structural phase crystallizing in the Pnma space group. EPR measurements on powder samples of [TbPc2](0) reveal an anisotropic spectrum, which is attributed to the spin-1/2 radical coupled weakly to the EPR-silent Tb-III ion. Extensive double-axis rotation studies on a single crystal reveal two independent spin-1/2 signals with differently oriented (albeit identical) uniaxial g-tensors, in complete agreement with x-ray structural studies that indicate two molecular orientations within the unit cell. The easy-axis nature of the radical EPR spectra thus reflects the coupling to the Ising-like Tb-III moment. This is corroborated by studies of the isostructural [YPc2](0) analog (where Y is nonmagnetic yttrium), which gives a completely isotropic radical EPR signal. The experimental results for the terbium complex are well explained on the basis of an effective model that introduces a weak ferromagnetic Heisenberg coupling between an isotropic spin-1/2 and an anisotropic spin-orbital moment, J = 6, that mimics the known, strong easy-axis Tb . . . Pc-2-crystal-field interaction.
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