The discovery of magnetism in 2D materials offers new opportunities for exploring novel quantum states and developing spintronic devices. In this work, using field-effect transistors with solid ion conductors as the gate dielectric (SIC-FETs), we have observed a significant enhancement of ferromagnetism associated with magnetic easy-axis switching in few-layered Cr 2 Ge 2 Te 6 . The easy axis of the magnetization, inferred from the anisotropic magnetoresistance, can be uniformly tuned from the out-of-plane direction to an in-plane direction by electric field in the few-layered Cr 2 Ge 2 Te 6 . Additionally, the Curie temperature, obtained from both the Hall resistance and magnetoresistance measurements, increases from 65 to 180 K in the few-layered sample by electric gating. Moreover, the surface of the sample is fully exposed in the SIC-FET device configuration, making further heterostructure-engineering possible. This work offers an excellent platform for realizing electrically controlled quantum phenomena in a single device.
Magnetism in the two-dimensional limit has become an intriguing topic for exploring new physical phenomena and potential applications. Especially, the two-dimensional magnetism is often associated with novel intrinsic spin fluctuations and versatile electronic structures, which provides vast opportunities in 2D material research. However, it is still challenging to verify candidate materials hosting two-dimensional magnetism, since the prototype systems have to be realized by using mechanical exfoliation or atomic layer deposition. Here, an alternative manipulation of two-dimensional magnetic properties via electrochemical intercalation of organic molecules is reported. Using tetrabutyl ammonium (TBA+), we synthesized a (TBA)Cr2Ge2Te6 hybrid superlattice with metallic behavior, and the Curie temperature is significantly increased from 67 K in pristine Cr2Ge2Te6 to 208 K in (TBA)Cr2Ge2Te6. Moreover, the magnetic easy axis changes from the ⟨001⟩ direction in Cr2Ge2Te6 to the ab-plane in (TBA)Cr2Ge2Te6. Theoretical calculations indicate that the drastic increase of the Curie temperature can be attributed to the change of magnetic coupling from a weak superexchange interaction in pristine Cr2Ge2Te6 to a strong double-exchange interaction in (TBA)Cr2Ge2Te6. These findings are the first demonstration of manipulation of magnetism in magnetic van der Waals materials by means of intercalating organic ions, which can serve as a convenient and efficient approach to explore versatile magnetic and electronic properties in van der Waals crystals.
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