<p>Dimensionality and magnetic anisotropy jointly determine whether long-range magnetic order survives in low-dimensional magnets. Although theory predicts that perpendicular magnetic anisotropy can stabilize ferromagnetism in two-dimensional systems, an experimental realization of a continuous crossover from a three-dimensional Heisenberg-type system to a two-dimensional Ising-type ferromagnet has remained challenging. Here we demonstrate such a crossover in thin layers of the van der Waals ferromagnet Fe<sub>3</sub>GeTe<sub>2</sub>. Counterintuitively, the monolayer—one quintuple layer, where no van der Waals gap exists—exhibits three-dimensional Heisenberg-like behaviour. We reveal that this arises from substantial structural modifications relative to bulk-like quintuple layers. Bilayers and thicker films revert to the bulk-like structure, which, together with substantial self-intercalation of Fe in the van der Waals gaps, stabilizes perpendicular magnetic anisotropy and drives the system into a two-dimensional Ising-like regime. Our findings emphasize the critical role of self-intercalation and provide insights into how subtle atomic-scale structural evolution, rather than nominal thickness alone, governs magnetic ordering in low-dimensional materials.</p>

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Anomalous crossover from three-dimensional Heisenberg to two-dimensional Ising magnetism in a van der Waals magnet

  • Ke Xiao,
  • Ruifeng Wang,
  • Yicheng Guan,
  • Jae-Chun Jeon,
  • Tingting Jiang,
  • Kajal Tiwari,
  • Yung-Cheng Li,
  • Ilya Kostanovski,
  • Katayoon Mohseni,
  • Holger L. Meyerheim,
  • Stuart S. P. Parkin

摘要

Dimensionality and magnetic anisotropy jointly determine whether long-range magnetic order survives in low-dimensional magnets. Although theory predicts that perpendicular magnetic anisotropy can stabilize ferromagnetism in two-dimensional systems, an experimental realization of a continuous crossover from a three-dimensional Heisenberg-type system to a two-dimensional Ising-type ferromagnet has remained challenging. Here we demonstrate such a crossover in thin layers of the van der Waals ferromagnet Fe3GeTe2. Counterintuitively, the monolayer—one quintuple layer, where no van der Waals gap exists—exhibits three-dimensional Heisenberg-like behaviour. We reveal that this arises from substantial structural modifications relative to bulk-like quintuple layers. Bilayers and thicker films revert to the bulk-like structure, which, together with substantial self-intercalation of Fe in the van der Waals gaps, stabilizes perpendicular magnetic anisotropy and drives the system into a two-dimensional Ising-like regime. Our findings emphasize the critical role of self-intercalation and provide insights into how subtle atomic-scale structural evolution, rather than nominal thickness alone, governs magnetic ordering in low-dimensional materials.