It is accepted that only three elements are ferromagnetic at room temperature, the transition metals iron, cobalt and nickel. The Stoner criterion explains why, for example, iron is ferromagnetic but manganese is not, even though both elements have an unfilled 3d shell and are adjacent in the periodic table: the product of the density of states with the exchange integral must be greater than unity for spontaneous ordering to emerge.1,2 Here, we demonstrate that it is possible to alter the electronic states of nonferromagnetic materials, such as diamagnetic copper and paramagnetic manganese, in 2 order to drive them ferromagnetic at room temperature. This remarkable effect is achieved via interfaces between metallic thin films and C 60 molecular layers. The emergent ferromagnetic state can exist over several layers of the metal before being quenched at large sample thicknesses by the material's bulk properties. While the induced magnetisation is easily measurable by magnetometry, low energy muon spin spectroscopy 3 provides insight into its magnetic distribution by studying the depolarisation process of low energy muons implanted in the sample. This technique indicates localized spin-ordered states at and close to the metallo-molecular interface.Density functional theory simulations suggest a mechanism based on magnetic hardening of the metal atoms due to electron transfer. 4,5 This opens a path for the exploitation of molecular coupling to design magnetic metamaterials using abundant, non-toxic elements such as organic semiconductors. Charge transfer at molecular interfaces can then be used to control spin polarisation or magnetisation, with far reaching consequences in the design of devices for electronic, power or computing applications. 6,7 Multifunctional materials with the spin degree of freedom such as multiferroics, magnetic semiconductors and molecular magnets have all aroused huge interest as potentially transformative components in quantum technologies. [8][9][10][11][12] Strategies used to bring magnetic ordering to these materials typically rely on the inclusion of magnetic transition metals, heavy elements with a large atomic moment or rare earths. In thin film structures, proximity effects and coupling at interfaces play an essential role. 13,14 This is especially the case for molecular spintronics, 15,16 where organic thin films grown on copper have demonstrated spin filtering. 17The organic magnetic coupling can propagate for long distances in systems such as nanoscale vortex-like configurations or nanoskyrmion lattices. 183We choose C 60 as a model molecule due to its structural simplicity and robustness as well as its high electron affinity. C 60 /transition metal complexes exhibit strong interfacial coupling between metal 3d z electrons and molecular π-bonded p electrons. The potential created by the mismatch of molecular and metal work functions leads to a partial filling of the interface states. [19][20][21] Other molecules with close electron affinity and the potential for 3d z /p coupling ...
A facile one-pot method is described for the formation of novel heterostructures in which inorganic nanoparticles are homogeneously distributed throughout an inorganic single crystal matrix. Our strategy uses nanoparticles functionalised with a poly(sodium 4-styrenesulphonate)-poly(methacrylic acid) [PNaStS-PMAA] diblock copolymer as a soluble crystal growth additive. This copolymer plays a number of essential roles. The PMAA anchor block is physically adsorbed onto the inorganic nanoparticles, while the PNaStS block acts as an electrosteric stabiliser and ensures that the nanoparticles retain their colloidal stability in the crystal growth solution. In addition, this strong acid block promotes binding to both the nanoparticles and the host crystal, which controls nanoparticle incorporation within the host crystal lattice. We show that this approach can be used to achieve encapsulation loadings of at least 12 wt% copolymer-coated magnetite particles within calcite single crystals. Transmission electron microscopy shows that these nanoparticles are uniformly distributed throughout the calcite, and that the crystal lattice retains its continuity around the embedded magnetite particles. Characterisation of these calcite/magnetite nanocomposites confirmed their magnetic properties. This new experimental approach is expected to be quite general, such that a small family of block copolymers could be used to drive the incorporation of a wide range of pre-prepared nanoparticles into host crystals, giving intimate mixing of phases with contrasting properties, while limiting nanoparticle aggregation and migration.
Iron sulfur (Fe–S) phases have been implicated in the emergence of life on early Earth due to their catalytic role in the synthesis of prebiotic molecules. Similarly, Fe–S phases are currently of high interest in the development of green catalysts and energy storage. Here we report the synthesis and structure of a nanoparticulate phase (FeSnano) that is a necessary solid-phase precursor to the conventionally assumed initial precipitate in the iron sulfide system, mackinawite. The structure of FeSnano contains tetrahedral iron, which is compensated by monosulfide and polysulfide sulfur species. These together dramatically affect the stability and enhance the reactivity of FeSnano.
. Solid (R)-3·MeNO 2 exhibits an unusualv ery gradual, but discontinuoust hermals pin-crossover with an approximate T1 = 2 of 350 K. The discontinuity around 240 Kl ies well below T1 = 2 , and is unconnected to ac rystallographic phase change occurring at 170 K. Rather,i tc an be correlated with ag radual ordering of the ligand conformation as the temperature is raised. The other solid compounds either exhibit spin-cross-
Evidence is presented to show that carbon nanotubes can become magnetized when they are in contact with magnetic material. Spin-polarized charge transfer at the interface between a flat ferromagnetic metal substrate and a multiwalled carbon nanotube leads to a spin transfer of about 0.1 μB per contact carbon atom. The corresponding magnetization is detected by using magnetic force microscopy to probe the stray field in the neighbourhood of the nanotube. Magnetic contrast is observed for carbon nanotubes placed on cobalt or magnetite substrates, but it is absent on silicon, copper or gold substrates. This observation of contact-induced magnetism opens a new avenue for implementing spin-electronics at the molecular level, where the current leads can be separated from the electrodes producing spin polarization.
The synthesis of 4-methyl-2,6-di(pyrazol-1-yl)pyridine (L) and four salts of [FeL 2 Torr pressure inside the powder diffractometer causes a reversible transformation back to the high-temperature crystal phase. Consideration of thermodynamic data implies this cannot be accompanied by a low high spin state change, however. Both compounds also exhibit the LIESST effect, with 2 exhibiting an unusually high T(LIESST) of 112 K. The salts 3 and 4 are respectively high-spin and low-spin between 3-300 K, with crystalline 3 exhibiting a more pronounced version of the same Jahn-Teller distortion.3
A novel magnetic SO4/Fe-Al-TiO2 solid acid catalyst was synthesized for biodiesel production via the (trans)esterification of waste cooking oil (WCO). The nanocomposite catalyst was prepared by the sequential functionalisation of commercial rutile/anatase mixed phase TiO2 nanoparticles (NPs) with alumina as a buffer layer, and subsequently hematite to impart magnetic character, prior to sulfation with chlorosulfonic acid to introduce Brønsted acidity. XRD showed that the SO4/Fe-Al-TiO2 catalyst comprised titania (rutile and anatase phases), aluminium sulphate, and hematite nanoparticles, while electron microscopy revealed the layer-by-layer assembly of these components within the SO4/Fe-Al-TiO2 catalyst. FTIR confirmed the presence of surface sulphate groups SO4 2and S2O7 2-/S3O10 2-, creating a predominantly Brønsted acid catalyst with high acid loading. The catalyst achieved 96 % fatty acid methyl ester (FAME) yield from WCO after 2.5 h of reaction at 90 °C, using 3 wt% of the magnetic catalyst, and a methanol:oil molar ratio of 10:1. SO4/Fe-Al-TiO2 was also effective for feedstocks containing up to 20 wt% of free fatty acid (FFA), and showed excellent stability for WCO (trans)esterification over 10 recycles.
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