Evidence of Spin Frustration in Vanadium Diselenide Monolayer Magnet

Authors:
  • PWPing Kwan Johnny Wong
    Ping Kwan Johnny Wong
  • WZWen Zhang
    Wen Zhang
  • FBFabio Bussolotti
    Fabio Bussolotti
  • XYXinmao Yin
    Xinmao Yin
  • THTun Seng Herng
    Tun Seng Herng
  • LZLei Zhang
    Lei Zhang
  • YHYu Li Huang
    Yu Li Huang
  • GVGiovanni Vinai
    Giovanni Vinai
  • SKSridevi Krishnamurthi
    Sridevi Krishnamurthi
  • DBDanil W Bukhvalov
    Danil W Bukhvalov
  • YZYu Jie Zheng
    Yu Jie Zheng
  • RCRebekah Chua
    Rebekah Chua
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Abstract
Monolayer VSe2, featuring both charge density wave and magnetism phenomena, represents a unique van der Waals magnet in the family of metallic two-dimensional transition-metal dichalcogenides (2D-TMDs). Herein, by means of in-situ microscopic 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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