Emerging 2D magnetic heterojunctions attract substantial interest due to their potential applications in spintronics. Achieving magnetic phase engineering with structural integrity in 2D heterojunctions is of paramount importance for their magnetism manipulation. Herein, starting with chromium ditelluride (CrTe2) as the backbone framework, various lateral and vertical magnetic heterojunctions are obtained via self‐intercalated 2D chromium telluride (CrxTey). A Cr2Te3‐Cr5Te8 lateral heterojunction prototype is demonstrated for the manipulation of magnetic moments under different magnitudes of magnetic excitation, showing a sharply stepped hysteresis loop with a dual spin‐flip transition at high Curie temperatures up to 150 and 210 K by magneto‐optical Kerr measurement. High‐resolution scanning transmission electron microscopy and first‐principles calculations reveal a preferred random location of Cr intercalants at the phase boundary, allowing lowering energy associated with crystal field splitting. The overall structural rigidity of chromium‐telluride heterostructure with magnetic phase decoupled behaviors is promising for 2D spintronic devices.

Probing large-scale intrinsic structure of air-sensitive 2D materials with atomic resolution is so far challenging due to their rapid oxidization and contamination. Here, by keeping the whole experiment including growth, transfer, and characterizations in an interconnected atmosphere-control environment, the large-scale intact lattice structure of air-sensitive monolayer 1T'-WTe 2 is directly visualized by atom-resolved scanning transmission electron microscopy. Benefit from the large-scale atomic mapping, collective lattice distortions are further unveiled due to the presence of anisotropic rippling, which propagates perpendicular to only one of the preferential lattice planes in the same WTe 2 monolayer. Such anisotropic lattice rippling modulates the intrinsic point defect (Te vacancy) distribution, in which they aggregate at the constrictive inner side of the undulating structure, presumably due to the ripple-induced asymmetric strain as elaborated by density functional theory. The results pave the way for atomic characterizations and defect engineering of air-sensitive 2D layered materials.

Emerging functionalities in two-dimensional materials, such as ferromagnetism, superconductivity and ferroelectricity, open new avenues for promising nanoelectronic applications. Here, we report the discovery of intrinsic in-plane room-temperature ferroelectricity in two-dimensional Bi2TeO5 grown by chemical vapor deposition, where spontaneous polarization originates from Bi column displacements. We found an intercalated buffer layer consist of mixed Bi/Te column as 180° domain wall which enables facile polarized domain engineering, including continuously tunable domain width by pinning different concentration of buffer layers, and even ferroelectric-antiferroelectric phase transition when the polarization unit is pinned down to single atomic column. More interestingly, the intercalated Bi/Te buffer layer can interconvert to polarized Bi columns which end up with series terraced domain walls and unusual fan-shaped ferroelectric domain. The buffer layer induced size and shape tunable ferroelectric domain in two-dimensional Bi2TeO5 offer insights into the manipulation of functionalities in van der Waals materials for future nanoelectronics.

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