Absence of ferromagnetism in VSe${}_2$ caused by its charge density wave phase

Abstract

How magnetism emerges in low-dimensional materials such as transition metal dichalcogenides at the monolayer limit is still an open question. Herein, we present a comprehensive study of the magnetic properties of single crystal and monolayer VSe${}_2$, both experimentally and \emph{ab initio}. Magnetometry, X-ray magnetic circular dichrosim (XMCD) and \emph{ab initio} calculations demonstrate that the charge density wave in bulk stoichiometric VSe${}_{2.0}$ causes a structural distortion with a strong reduction in the density of sates at the Fermi level, prompting the system towards a non-magnetic state but on the verge of a ferromagnetic instability. In the monolayer limit, the structural rearrangement induces a Peierls distortion with the opening of an energy gap at the Fermi level and the absence of magnetic order. Control experiments on defect-induced VSe${}_{2-\delta }$ single crystals show a breakdown of magnetism, discarding vacancies as a possible origin of magnetic order in VSe${}_2$.

polished version, updated acknowledgments

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• Ultrafast triggering of insulator-metal transition in two-dimensional VSe${}_2$
• Anharmonicity reveals the tunability of the charge density wave orders in monolayer VSe${}_2$
• Nontrivial doping evolution of electronic properties in Ising-superconducting alloys
• Controllable phase transitions between multiple charge density waves in monolayer 1T-VSe${}_2$ via doping and strain engineering
• Atomically sharp 1D interfaces in 2D lateral heterostructures of VSe${}_2$-NbSe${}_2$ monolayers
• Tunable magnetism in bilayer transition metal dichalcogenides
• Quantum Monte Carlo and density functional theory study of strain and magnetism in 2D 1T-VSe${}_2$ with charge density wave states
• Generating Two-dimensional Ferromagnetic Charge Density Waves via External Fields
• Moiré induced electronic structure modifications in monolayer V${}_2$S${}_3$ on Au(111)
• Self-doped flat band and spin-triplet superconductivity in monolayer 1T-TaSe${}_{2-x}$Te${}_x$
• Identification of a Low Energy Metastable 1$T$-Type Phase for Monolayer VSe2
• Alloying 2D VSe2 with Pt: from a charge density wave state to a disordered insulator
• Comparative study of Kondo effect in Vanadium dichalcogenides VX${}_2$ (X=Se & Te)
• Structure dependent and strain tunable magnetic ordering in ultrathin chromium telluride
• Anomalous amplitude mode dynamics below the expected charge-density-wave transition in 1$T$-VSe${}_2$
• An ab initio description of the family of Cr selenides: structure, magnetism and electronic structure from bulk to the single-layer limit
• Electronic structure and charge-density wave transition in monolayer VS_{2}