Intrinsic Negative Magnetoresistance in Van Der Waals FeNbTe₂ Single Crystals

Abstract Magnetoresistance, the dependence of resistivity on the applied magnetic field, provides the opportunity to manipulate and utilize the electronic spin degree of freedom, which is not only a long‐term frontier field of solid‐state physics but also the cornerstone of information storage technology. However, the negative magnetoresistance (nMR) is a relatively rare case of magnetoresistance in which the microscopic origin is still elusive and for which it is difficult to define a general interpretation. Herein, an experimental case of an intrinsic unsaturated nMR is demonstrated in van der Waals FeNbTe₂ single crystal. The clear‐cut evidence in angle‐resolved photoemission spectroscopy (ARPES), the electronic transport measurement, and DC/AC magnetic susceptibility confirms that the intrinsic unsaturated nMR is derived from the comprehensive effect of Anderson localization and a spin glass state. Taking into consideration that intrinsic unsaturated nMR has so far been rarely reported, especially in van der Waals structures, it is anticipated that this work will not only lead to a deep understanding of the inherent microcosmic mechanism but will also serve as a guide to broaden the research of spintronics and information storage based on magnetoresistance.