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All van der Waals Fe 3 GeTe 2 /Cr 2 Ge 2 Te 6 /graphite magnetic heterojunctions have been fabricated via mechanical exfoliation and stacking, and their magnetotransport properties are studied in detail. At low bias voltages, large negative junction magnetoresistances have been observed and are attributed to spin-conserving tunneling transport across an insulating Cr 2 Ge 2 Te 6 layer. With increasing bias, a crossover to Fowler–Nordheim tunneling takes place. The negative sign of the tunneling magnetoresistance suggests that the bottom of a conduction band in Cr 2 Ge 2 Te 6 belongs to minority spins, opposite to the findings of some first-principles calculations. This work shows that the vdW heterostructures based on 2D magnetic insulators are a valuable platform to gain further insight into spin polarized tunneling transport, which is the basis for pursuing high performance spintronic devices and a large variety of quantum phenomena.

Alloy materials such as Si and Ge are attractive as high‐capacity anodes for rechargeable batteries, but such anodes undergo severe capacity degradation during discharge–charge processes. Compared to the over‐emphasized efforts on the electrode structure design to mitigate the volume changes, understanding and engineering of the solid‐electrolyte interphase (SEI) are significantly lacking. This work demonstrates that modifying the surface of alloy‐based anode materials by building an ultraconformal layer of Sb can significantly enhance their structural and interfacial stability during cycling. Combined experimental and theoretical studies consistently reveal that the ultraconformal Sb layer is dynamically converted to Li₃Sb during cycling, which can selectively adsorb and catalytically decompose electrolyte additives to form a robust, thin, and dense LiF‐dominated SEI, and simultaneously restrain the decomposition of electrolyte solvents. Hence, the Sb‐coated porous Ge electrode delivers much higher initial Coulombic efficiency of 85% and higher reversible capacity of 1046 mAh g⁻¹after 200 cycles at 500 mA g⁻¹, compared to only 72% and 170 mAh g⁻¹for bare porous Ge. The present finding has indicated that tailoring surface structures of electrode materials is an appealing approach to construct a robust SEI and achieve long‐term cycling stability for alloy‐based anode materials.