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1.
Chem Mater ; 36(14): 7056-7068, 2024 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-39070667

RESUMO

Neodymium tritelluride is a layered van der Waals material, with correlated electronic properties including high electronic mobility, charge density waves, and antiferromagnetism. We developed a solution synthesis method to form free-standing nanosheets of NdTe3, with nanosheet lateral dimensions of 200-400 nm. The morphology of the nanosheet was influenced by the neodymium precursor. When Nd[(N(SiMe3)2]3 was used as the metal source the nanosheet thickness average was 12 ± 2.5 nm, alternatively the combination of NdCl3 and Li(N(SiMe3)2) led to thicker nanosheets, approximately 19 ± 2.4 nm. We believe that the difference in thickness and changes in surface chemistry point to the role of chloride in accelerating nanocrystal growth for the synthesis with NdCl3 (and Li(N(SiMe3)2). Both types of nanosheets exhibit charge density wave (CDW) distortions as measured using electron diffraction and investigated using variable temperature Raman scattering. Interestingly, the magnetic studies suggest a distinct change in properties between 12 and 19 nm thickness in antiferromagnetic NdTe3.

2.
Phys Chem Chem Phys ; 25(43): 29516-29530, 2023 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-37901907

RESUMO

We present a theoretical and experimental study of two tetracoordinate Co(II)-based complexes with semi-coordination interactions, i.e., non-covalent interactions involving the central atom. We argue that such interactions enhance the thermal and structural stability of the compounds, making them appropriate for deposition on substrates, as demonstrated by their successful deposition on graphene. DC magnetometry and high-frequency electron spin resonance (HF-ESR) experiments revealed an axial magnetic anisotropy and weak intermolecular antiferromagnetic coupling in both compounds, supported by theoretical predictions from complete active space self-consistent field calculations complemented by N-electron valence state second-order perturbation theory (CASSCF-NEVPT2), and broken-symmetry density functional theory (BS-DFT). AC magnetometry demonstrated that the compounds are field-induced single-ion magnets (SIMs) at applied static magnetic fields, with slow relaxation of magnetization governed by a combination of quantum tunneling, Orbach, and direct relaxation mechanisms. The structural stability under ambient conditions and after deposition was confirmed by X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Theoretical modeling by DFT of different configurations of these systems on graphene revealed n-type doping of graphene originating from electron transfer from the deposited molecules, confirmed by electrical transport measurements and Raman spectroscopy.

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