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Interfacial Charge Transfer and Morphology Govern Magnetism in Ultrathin VOx/MoSe2 Heterostructures

Abstract

Engineering magnetism in two-dimensional semiconductors through interfacial interactions offers an attractive alternative to substitutional doping and provides opportunities for integrating magnetic and optoelectronic functionality within the same heterostructure. Here, we investigate ultrathin VOx films deposited on monolayer MoSe2 and demonstrate a pronounced enhancement of the magnetic response upon formation of the VOx/MoSe2 interface. Combined structural, spectroscopic, magnetic, and first-principles analyses support a consistent picture in which finite VOx clusters possess intrinsic magnetic moments that are further enhanced by electron transfer from MoSe2 to the oxide. The predicted charge transfer is also consistent with the increased trion contribution observed in the photoluminescence response of the heterostructure. Beyond this interfacial enhancement, the magnetic behavior is strongly governed by the morphology of the ultrathin oxide. A crossover from discontinuous clusters to more continuous films produces qualitatively different temperature dependences: the continuous-film regime exhibits conventional thermal demagnetization and coercive softening, whereas the clustered regime displays an unusual increase in magnetization and nonmonotonic coercivity with increasing temperature. These contrasting responses are captured by a phenomenological model in which morphology determines the collective magnetic dynamics through a distribution of effective reversal barriers and their thermally activated accessibility. Together, the results establish a unified picture in which interfacial charge transfer enhances the local magnetic moments of VOx, while nanoscale morphology governs their collective magnetic dynamics, providing complementary routes for controlling magnetism in oxide/transition-metal dichalcogenide heterostructures.

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BibTeX
@misc{wadumesthri2026interfacial,
  title = {{Interfacial Charge Transfer and Morphology Govern Magnetism in Ultrathin VOx/MoSe2 Heterostructures}},
  author = {Yasinthara Wadumesthri and Nalaka Kapuruge and Raphael B. de Oliveira and Bruno Ipaves and Guilherme S. L. Fabris and Kinga Lasek and Florence A. Nugera and Jianjun Pan and Xiaomei Jiang and Douglas S. Galvão and Humberto Rodríguez Gutiérrez},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.08494},
  eprint = {2610.08494},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.08494},
}
RIS
TY  - UNPB
TI  - Interfacial Charge Transfer and Morphology Govern Magnetism in Ultrathin VOx/MoSe2 Heterostructures
AU  - Yasinthara Wadumesthri
AU  - Nalaka Kapuruge
AU  - Raphael B. de Oliveira
AU  - Bruno Ipaves
AU  - Guilherme S. L. Fabris
AU  - Kinga Lasek
AU  - Florence A. Nugera
AU  - Jianjun Pan
AU  - Xiaomei Jiang
AU  - Douglas S. Galvão
AU  - Humberto Rodríguez Gutiérrez
PY  - 2026
DA  - 2026/10/06
PB  - arXiv
DO  - 10.48550/arxiv.2610.08494
UR  - https://arxiv.org/abs/2610.08494
AB  - Engineering magnetism in two-dimensional semiconductors through interfacial interactions offers an attractive alternative to substitutional doping and provides opportunities for integrating magnetic and optoelectronic functionality within the same heterostructure. Here, we investigate ultrathin VOx films deposited on monolayer MoSe2 and demonstrate a pronounced enhancement of the magnetic response upon formation of the VOx/MoSe2 interface. Combined structural, spectroscopic, magnetic, and first-principles analyses support a consistent picture in which finite VOx clusters possess intrinsic magnetic moments that are further enhanced by electron transfer from MoSe2 to the oxide. The predicted charge transfer is also consistent with the increased trion contribution observed in the photoluminescence response of the heterostructure. Beyond this interfacial enhancement, the magnetic behavior is strongly governed by the morphology of the ultrathin oxide. A crossover from discontinuous clusters to more continuous films produces qualitatively different temperature dependences: the continuous-film regime exhibits conventional thermal demagnetization and coercive softening, whereas the clustered regime displays an unusual increase in magnetization and nonmonotonic coercivity with increasing temperature. These contrasting responses are captured by a phenomenological model in which morphology determines the collective magnetic dynamics through a distribution of effective reversal barriers and their thermally activated accessibility. Together, the results establish a unified picture in which interfacial charge transfer enhances the local magnetic moments of VOx, while nanoscale morphology governs their collective magnetic dynamics, providing complementary routes for controlling magnetism in oxide/transition-metal dichalcogenide heterostructures.
ER  -