Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 123, Issue 45, Pages 27802-27810Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.9b08868
Keywords
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Funding
- MINECO of Spain [MAT2016-80762-R, PGC2018-101334-A-C22, PGC2018-101334-B-C21]
- MECD through the FPU grant [FPU16/02572]
- European Commission through the Marie Sklodowska-Curie IEF project SUPER2D [GA-748971]
- Spanish MINECO [MAT2017-82074-ERC]
- ERC Starting grant LINKSPM [758558]
- IKERBASQUE
- European Research Council (ERC) [758558] Funding Source: European Research Council (ERC)
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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 VSe2, both experimentally and ab initio. Magnetometry, X-ray magnetic circular dichrosim (XMCD), and ab initio calculations demonstrate that the charge density wave in bulk stoichiometric VSe2.0 causes a structural distortion with a strong reduction in the density of states at the Fermi level, prompting the system toward a nonmagnetic 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 VSe2-delta single crystals show a breakdown of magnetism, discarding vacancies as a possible origin of magnetic order in VSe2.
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