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Electronic Transport In Mesoscopic Systems

Materials research has driven the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices1,2 because identifying new magnetic materials is key to better device performance and design. Van der Waals crystals retain their chemical stability and structural integrity down to the monolayer and, being atomically thin, are readily tuned by various kinds of gate modulation3,4. Recent experiments have demonstrated that it is possible to obtain two-dimensional ferromagnetic order in insulating Cr2Ge2Te6 (ref. 5) and CrI3 (ref. 6) at low temperatures. Here we develop a device fabrication technique and isolate monolayers from the layered metallic magnet Fe3GeTe2 to study magnetotransport. We find that the itinerant ferromagnetism persists in Fe3GeTe2 down to the monolayer with an out-of-plane magnetocrystalline anisotropy. The ferromagnetic transition temperature, Tc, is suppressed relative to the bulk Tc of 205 kelvin in pristine Fe3GeTe2 thin flakes. An ionic gate, however, raises Tc to room temperature, much higher than the bulk Tc. The gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2 opens up opportunities for potential voltage-controlled magnetoelectronics7-11 based on atomically thin van der Waals crystals.

Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe 3 GeTe 2

Lower olefins-generally referring to ethylene, propylene and butylene-are basic carbon-based building blocks that are widely used in the chemical industry, and are traditionally produced through thermal or catalytic cracking of a range of hydrocarbon feedstocks, such as naphtha, gas oil, condensates and light alkanes. With the rapid depletion of the limited petroleum reserves that serve as the source of these hydrocarbons, there is an urgent need for processes that can produce lower olefins from alternative feedstocks. The 'Fischer-Tropsch to olefins' (FTO) process has long offered a way of producing lower olefins directly from syngas-a mixture of hydrogen and carbon monoxide that is readily derived from coal, biomass and natural gas. But the hydrocarbons obtained with the FTO process typically follow the so-called Anderson-Schulz-Flory distribution, which is characterized by a maximum C2-C4 hydrocarbon fraction of about 56.7 per cent and an undesired methane fraction of about 29.2 per cent (refs 1, 10, 11, 12). Here we show that, under mild reaction conditions, cobalt carbide quadrangular nanoprisms catalyse the FTO conversion of syngas with high selectivity for the production of lower olefins (constituting around 60.8 per cent of the carbon products), while generating little methane (about 5.0 per cent), with the ratio of desired unsaturated hydrocarbons to less valuable saturated hydrocarbons amongst the C2-C4 products being as high as 30. Detailed catalyst characterization during the initial reaction stage and theoretical calculations indicate that preferentially exposed {101} and {020} facets play a pivotal role during syngas conversion, in that they favour olefin production and inhibit methane formation, and thereby render cobalt carbide nanoprisms a promising new catalyst system for directly converting syngas into lower olefins.

Cobalt carbide nanoprisms for direct production of lower olefins from syngas

In this paper, we review some of the key concepts in ultrathin film magnetism which underpin nanomagnetism. We survey the results of recent experimental and theoretical studies of well characterized epitaxial structures based on Fe, Co and Ni to illustrate how intrinsic fundamental properties such as the magnetic exchange interactions, magnetic moment and magnetic anisotropies change markedly in ultrathin films as compared with their bulk counterparts, and to emphasize the role of atomic scale structure, strain and crystallinity in determining the magnetic properties. After introducing the key length scales in magnetism, we describe the 2D magnetic phase transition and survey studies of the thickness dependent Curie temperature and the critical exponents which characterize the paramagnetic–ferromagnetic phase transition. We next discuss recent experimental and theoretical results on the determination of the exchange constant, followed by an overview of measurements of the magnetic moment in the elemental 3d transition metal thin films in the various crystal phases that have been successfully stabilized, thereby illustrating the sensitivity of the magnetic moment to the local symmetry and to the atomic environment. Finally, we discuss briefly the magnetic anisotropies of Fe, Co and Ni in the fcc crystalline phase, to emphasize the role of structure and the details of the interface in influencing the magnetic properties. The dramatic effect that adsorbates can have on the magnetic anisotropies of thin magnetic films is also discussed. Our survey demonstrates that the fundamental properties, namely, the magnetic moment and magnetic anisotropies of ultrathin films have dramatically different behaviour compared with those of the bulk while the comparable size of the structural and magnetic contributions to the total energy of ultrathin structures results in an exquisitely sensitive dependence of the magnetic properties on the film structure.

https://iopscience.iop.org/article/10.1088/0034-4885/71/5/056501/pdf

Magnetism in ultrathin film structures

The direct synthesis of lower (C2 to C4) olefins, key building-block chemicals, from syngas (H2/CO), which can be derived from various nonpetroleum carbon resources, is highly attractive, but the selectivity for lower olefins is low because of the limitation of the Anderson-Schulz-Flory distribution. We report that the coupling of methanol-synthesis and methanol-to-olefins reactions with a bifunctional catalyst can realize the direct conversion of syngas to lower olefins with exceptionally high selectivity. We demonstrate that the choice of two active components and the integration manner of the components are crucial to lower olefin selectivity. The combination of a Zr-Zn binary oxide, which alone shows higher selectivity for methanol and dimethyl ether even at 673 K, and SAPO-34 with decreased acidity offers around 70% selectivity for C2-C4 olefins at about 10% CO conversion. The micro- to nanoscale proximity of the components favors the lower olefin selectivity.

Direct and Highly Selective Conversion of Synthesis Gas into Lower Olefins: Design of a Bifunctional Catalyst Combining Methanol Synthesis and Carbon–Carbon Coupling

Fischer–Tropsch synthesis (FTS) is a classical topic of great significance because of the approach of post-petroleum times. For decades, people have attempted to develop iron-based FTS catalysts with high selectivity for lower olefins. By means of the anchoring effect and the intrinsic basicity of nitrogen-doped carbon nanotubes (NCNTs), iron nanoparticles were conveniently immobilized on NCNTs without surface premodification. The so-constructed Fe/NCNTs catalyst presents superb catalytic performance in FTS with high selectivity for lower olefins of up to 46.7% as well as high activity and stability. The excellent performance is well-correlated with enhanced dissociative CO adsorption, inhibition of secondary hydrogenation of lower olefins, and promoted formation of the active phase of χ-Fe5C2. All of these merits result from participation of the nitrogen, as revealed by our experimental characterization. These results may lead to a new strategy for exploring advanced FTS catalysts with abundant N-doped c...

Promotion Effects of Nitrogen Doping into Carbon Nanotubes on Supported Iron Fischer–Tropsch Catalysts for Lower Olefins

Using both broadband ferromagnetic resonance (FMR) spectroscopy and ab initio calculations, we study the magnetodynamic properties of permalloy (Py, Ni80Fe20) and Py100-x M-x films with M as platin ...

Tunable permalloy-based films for magnonic devices

For spintronics application, which requires fast field switching, it is important to have a kind of soft magnetic material with large damping coefficient. Here, we present the studies of the Nd dopant-level-dependent damping coefficient of Nd${}_{x}$-Py${}_{(1\ensuremath{-}x)}$ thin films (30 nm) in a dilute region utilizing ferromagnetic resonance (FMR). With the Nd content increasing, the film structure was found to be changing from polycrystalline to amorphous when the Nd content is around 3.4%. Meanwhile, the magnetization decreases linearly. Interestingly, we find that along the easy axis, both low coercivity and high hysteresis squareness are simultaneously maintained in the system; i.e., the magnetic softness has been well kept. By theoretical fitting of the angular dependence of the FMR field, the first- and second-order magnetic anisotropy constants, ${K}_{1}$ and ${K}_{2}$, and the Lande $g$ factor are obtained and discussed quantitatively. The measurements of angular and frequency dependence of the ferromagnetic resonance linewidth, as well as the theoretical fitting by considering the contributions of Gilbert damping, two-magnon scattering, and inhomogeneous broadening, show that the damping coefficient $\ensuremath{\alpha}$ increases rapidly (about 25-fold) as the Nd content increases to 11.6%, which is mainly due to the enhanced spin-orbit coupling by the Nd additives, supported by x-ray magnetic circular dichroism measurements.

Enhancement of magnetization damping coefficient of permalloy thin films with dilute Nd dopants

Exchange bias is a physical phenomenon whereby the spins of a ferromagnet are pinned by those of an antiferromagnet, and this phenomenon has played an undisputed role in magnetic data storage. Over the past few decades, this effect has been observed in a variety of antiferromagnet/ferromagnet systems. New aspects of this phenomenon are being discovered. With the increasing interest in van der Waals (vdW) magnets, we address the question whether the effect can exist in magnetic vdW heterostructures. Here, we report exchange-bias fields of over 50 mT in mechanically exfoliated CrCl3/Fe3GeTe2 heterostructures at 2.5 K, the value of which is highly tunable by the field-cooling process and the heterostructure thickness. We postulate an intuitive picture explaining how the effect arises in this vdW heterostructure, as well as explaining the practical difficulty associated with capturing the effect. This work opens up new routes toward designing spintronic devices made of atomically thin vdW magnets.

Exchange Bias in van der Waals CrCl3/Fe3GeTe2 Heterostructures.

A series of Fe3O4 particle chains with an average particle diameter of 150 nm and different lengths were synthesized by using the self-assembly method at reduced temperature in different synthesizing magnetic fields. The influence of synthesizing magnetic field on the properties of the magnetite particle chains was studied by structural analyses, magnetometry measurement, and ferromagnetic resonance. A uniaxial magnetic anisotropy in the saturation field (Hs), hysteresis loop, and ferromagnetic resonance were observed to increase with increasing synthesizing field. The saturation magnetization and g-factor were found to increase slightly with increasing synthesizing field. The demagnetizing fields and demagnetizing factors were determined from the experimental data of magnetometry measurement, ferromagnetic resonance, and also numerical calculation, which agreed reasonably well. It was found that the magnetization non-uniformity in the chains and the magnetostatic interaction among the chains have an impo...

Ya Zhai

Papers

Promotion Effects of Nitrogen Doping into Carbon Nanotubes on Supported Iron Fischer–Tropsch Catalysts for Lower Olefins

Tunable permalloy-based films for magnonic devices

Enhancement of magnetization damping coefficient of permalloy thin films with dilute Nd dopants

Exchange Bias in van der Waals CrCl3/Fe3GeTe2 Heterostructures.

The Shape Anisotropy in the Magnetic Field-Assisted Self-Assembly Chain-like Structure of Magnetite