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Evidence of Spin Frustration in a Vanadium Diselenide Monolayer Magnet.

  • Author(s): Wong, Ping Kwan Johnny;
  • Zhang, Wen;
  • Bussolotti, Fabio;
  • Yin, Xinmao;
  • Herng, Tun Seng;
  • Zhang, Lei;
  • Huang, Yu Li;
  • Vinai, Giovanni;
  • Krishnamurthi, Sridevi;
  • Bukhvalov, Danil W;
  • Zheng, Yu Jie;
  • Chua, Rebekah;
  • N'Diaye, Alpha T;
  • Morton, Simon A;
  • Yang, Chao-Yao;
  • Ou Yang, Kui-Hon;
  • Torelli, Piero;
  • Chen, Wei;
  • Goh, Kuan Eng Johnson;
  • Ding, Jun;
  • Lin, Minn-Tsong;
  • Brocks, Geert;
  • de Jong, Michel P;
  • Castro Neto, Antonio H;
  • Wee, Andrew Thye Shen
  • et al.
Abstract

Monolayer VSe2 , featuring both charge density wave and magnetism phenomena, represents a unique van der Waals magnet in the family of metallic 2D transition-metal dichalcogenides (2D-TMDs). Herein, by means of in situ microscopy and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, direct spectroscopic signatures are established, that identify the metallic 1T-phase and vanadium 3d1 electronic configuration in monolayer VSe2 grown on graphite by molecular-beam epitaxy. Element-specific X-ray magnetic circular dichroism, complemented with magnetic susceptibility measurements, further reveals monolayer VSe2 as a frustrated magnet, with its spins exhibiting subtle correlations, albeit in the absence of a long-range magnetic order down to 2 K and up to a 7 T magnetic field. This observation is attributed to the relative stability of the ferromagnetic and antiferromagnetic ground states, arising from its atomic-scale structural features, such as rotational disorders and edges. The results of this study extend the current understanding of metallic 2D-TMDs in the search for exotic low-dimensional quantum phenomena, and stimulate further theoretical and experimental studies on van der Waals monolayer magnets.

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