<p>Chromium ditelluride, CrTe<sub>2</sub>, is an attractive candidate van der Waals material for hosting 2D magnetism. However, how the room-temperature ferromagnetism of the bulk evolves as the sample is thinned to the single-layer limit has proved controversial. This, in part, reflects its metastable nature, vs. a series of more stable self-intercalation compounds with higher relative Cr:Te stoichiometry. Here, exploiting a recently developed method for enhancing nucleation in molecular-beam epitaxy growth of transition-metal chalcogenides, we demonstrate the selective stabilisation of high-coverage CrTe<sub>2</sub> and Cr<sub>2+<i>ε</i></sub>Te<sub>3</sub> epitaxial monolayers. Combining X-ray magnetic circular dichroism, scanning tunnelling microscopy, and temperature-dependent angle-resolved photoemission, we demonstrate that both compounds order magnetically with a similar <i>T</i><sub>C</sub>. We find, however, that monolayer CrTe<sub>2</sub> forms as an antiferromagnetic metal, while monolayer Cr<sub>2+<i>ε</i></sub>Te<sub>3</sub> hosts an intrinsic ferromagnetic semiconducting state. This work thus demonstrates that control over the self-intercalation of metastable Cr-based chalcogenides provides a powerful route for tuning both their metallicity and magnetic structure, establishing the Cr<sub>x</sub>Te<sub>y</sub> system as a flexible materials class for future 2D spintronics.</p>

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From ferromagnetic semiconductor to antiferromagnetic metal in epitaxial CrxTey monolayers

  • Naina Kushwaha,
  • Olivia Armitage,
  • Brendan Edwards,
  • Liam Trzaska,
  • Jennifer Rigden,
  • Peter Bencok,
  • Deepnarayan Biswas,
  • Tien-Lin Lee,
  • Charlotte Sanders,
  • Gerrit van der Laan,
  • Peter Wahl,
  • Phil D. C. King,
  • Akhil Rajan

摘要

Chromium ditelluride, CrTe2, is an attractive candidate van der Waals material for hosting 2D magnetism. However, how the room-temperature ferromagnetism of the bulk evolves as the sample is thinned to the single-layer limit has proved controversial. This, in part, reflects its metastable nature, vs. a series of more stable self-intercalation compounds with higher relative Cr:Te stoichiometry. Here, exploiting a recently developed method for enhancing nucleation in molecular-beam epitaxy growth of transition-metal chalcogenides, we demonstrate the selective stabilisation of high-coverage CrTe2 and Cr2+εTe3 epitaxial monolayers. Combining X-ray magnetic circular dichroism, scanning tunnelling microscopy, and temperature-dependent angle-resolved photoemission, we demonstrate that both compounds order magnetically with a similar TC. We find, however, that monolayer CrTe2 forms as an antiferromagnetic metal, while monolayer Cr2+εTe3 hosts an intrinsic ferromagnetic semiconducting state. This work thus demonstrates that control over the self-intercalation of metastable Cr-based chalcogenides provides a powerful route for tuning both their metallicity and magnetic structure, establishing the CrxTey system as a flexible materials class for future 2D spintronics.