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1.
ACS Nano ; 15(1): 387-395, 2021 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-33119252

RESUMO

Nanoscopic lamellae of centrosymmetric ferromagnetic alloys have recently been reported to host the biskyrmion spin texture; however, this has been disputed as the misidentication of topologically trivial type-II magnetic bubbles. Here we demonstrate resonant soft X-ray holographic imaging of topological magnetic states in lamellae of the centrosymmetric alloy (Mn1-xNix)0.65Ga0.35 (x = 0.5), showing the presence of magnetic stripes evolving into single core magnetic bubbles. We observe rotation of the stripe phase via the nucleation and destruction of disclination defects. This indicates the system behaves as a conventional uniaxial ferromagnet. By utilizing the holography with extended reference by autocorrelation linear differential operator (HERALDO) method, we show tilted holographic images at 30° incidence confirming the presence of type-II magnetic bubbles in this system. This study demonstrates the utility of X-ray imaging techniques in identifying the topology of localized structures in nanoscale magnetism.

2.
Sci Rep ; 10(1): 16485, 2020 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-32999347

RESUMO

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

3.
Sci Rep ; 10(1): 9813, 2020 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-32555354

RESUMO

The GaV4S8-ySey (y = 0 to 8) family of materials have been synthesized in both polycrystalline and single crystal form, and their structural and magnetic properties thoroughly investigated. Each of these materials crystallizes in the F[Formula: see text][Formula: see text]3m space group at ambient temperature. However, in contrast to the end members GaV4S8 and GaV4Se8, that undergo a structural transition to the R3m space group at 42 and 41 K respectively, the solid solutions (y = 1 to 7) retain cubic symmetry down to 1.5 K. In zero applied field the end members of the family order ferromagnetically at 13 K (GaV4S8) and 18 K (GaV4Se8), while the intermediate compounds exhibit a spin-glass-like ground state. We demonstrate that the magnetic structure of GaV4S8 shows localization of spins on the V cations, indicating that a charge ordering mechanism drives the structural phase transition. We conclude that the observation of both structural and ferromagnetic transitions in the end members of the series in zero field is a prerequisite for the stabilization of a skyrmion phase, and discuss how the absence of these transitions in the y = 1 to 7 materials can be explained by their structural properties.

4.
Adv Mater ; 31(16): e1806598, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-30844122

RESUMO

The intense research effort investigating magnetic skyrmions and their applications for spintronics has yielded reports of more exotic objects including the biskyrmion, which consists of a bound pair of counter-rotating vortices of magnetization. Biskyrmions have been identified only from transmission electron microscopy images and have not been observed by other techniques, nor seen in simulations carried out under realistic conditions. Here, quantitative Lorentz transmission electron microscopy, X-ray holography, and micromagnetic simulations are combined to search for biskyrmions in MnNiGa, a material in which they have been reported. Only type-I and type-II magnetic bubbles are found and images purported to show biskyrmions can be explained as type-II bubbles viewed at an angle to their axes. It is not the magnetization but the magnetic flux density resulting from this object that forms the counter-rotating vortices.

5.
Nat Chem ; 9(7): 635-643, 2017 07.
Artigo em Inglês | MEDLINE | ID: mdl-28644474

RESUMO

Molecular solids with cooperative electronic properties based purely on π electrons from carbon atoms offer a fertile ground in the search for exotic states of matter, including unconventional superconductivity and quantum magnetism. The field was ignited by reports of high-temperature superconductivity in materials obtained by the reaction of alkali metals with polyaromatic hydrocarbons, such as phenanthrene and picene, but the composition and structure of any compound in this family remained unknown. Here we isolate the binary caesium salts of phenanthrene, Cs(C14H10) and Cs2(C14H10), to show that they are multiorbital strongly correlated Mott insulators. Whereas Cs2(C14H10) is diamagnetic because of orbital polarization, Cs(C14H10) is a Heisenberg antiferromagnet with a gapped spin-liquid state that emerges from the coupled highly frustrated Δ-chain magnetic topology of the alternating-exchange spiral tubes of S = ½ (C14H10)•- radical anions. The absence of long-range magnetic order down to 1.8 K (T/J ≈ 0.02; J is the dominant exchange constant) renders the compound an excellent candidate for a spin-½ quantum-spin liquid (QSL) that arises purely from carbon π electrons.

6.
Dalton Trans ; 46(10): 3338-3346, 2017 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-28230220

RESUMO

The reactivity of antimony trifluoride, SbF3, in non-polar aprotic solvents has been unexplored due to its negligible solubility. The reaction of the [SbF3(tmen)] complex (2) with the N-heterocyclic carbene, 1,3-bis(2,6-diisopropylphenyl)imidazole-2-ylidene, (LDipp), probably leads to the formation of a neutral [(LDipp)SbF3] intermediate (3) in non-polar solvents. Mild heat treatment of the reaction mixture unexpectedly activates the SbF3 molecules to undergo the auto-ionization reaction. In this process, one of the (LDipp) ligands undergoes rearrangement into the mesoionic carbene (MIC) and further coordinates to the cation to form [(LDipp)2SbF2]+[SbF4]-, product (4). Studies have confirmed that N,N,N',N'-tetramethylethane-1,2-diamine (tmen) present in the solution is not involved in the conversion mechanism and serves solely as an auxiliary ligand to increase the solubility of SbF3. The compound (4) shows a rare pnictogen(iii) halide auto-ionization process with the first mesoionic NHC rearrangement on any metal/metalloid fluoride compound and the first reported reaction system where a N-heterocyclic carbene ligand facilitates the auto-ionization process on a fluorido substrate.

7.
Dalton Trans ; 44(47): 20609-17, 2015 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-26556764

RESUMO

AlF3-based aerogels, a new class of inorganic aerogels, are prepared in a novel direct process that combines fluoride sol-gel synthesis with high temperature supercritical drying. The bulk structure of the solid products depends decisively on the applied solvent(s); very voluminous bulk aerogels are obtained only with MeOH that is used either alone or in combination with some other polar solvents. MeOH acts as a methoxylation agent; and formed methoxy (MeO) species are remarkably stable and deactivate the surface acidic sites. Removal of MeO species under moderate conditions results in catalytically active fluorides with a preserved nanostructure. In preparations with MeOH, preferential growth of anisotropic nanoparticles (nanorods) is the key step that leads to the formation of very open aerogel structures. Another process, dehydration of alcohols, results in some hydroxylation and hydration that lead to the formation of distinctive surface and bulk OH/H2O species. The structure of AlF3-based aerogels is consistent with the hexagonal tungsten bronze (HTB) ß-AlF3 although their composition corresponds to a formula AlF3-x(OH, OMe)x·yH2O (x = 0.1 ± 0.05). Some other characteristics of the fluoride nanoparticles, like crystallinity, particle size, and uniformity, can be effectively controlled by the temperature of the solvothermal process. The described methodology allows a controllable preparation of catalytically active fluorides in the form of regularly shaped and uniformly sized nanoparticles.

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