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Room Temperature Intrinsic Ferromagnetism in Epitaxial Manganese Selenide Films in the Monolayer Limit

Published 22 Feb 2018 in cond-mat.mtrl-sci and cond-mat.mes-hall | (1802.08152v1)

Abstract: Monolayer van der Waals (vdW) magnets provide an exciting opportunity for exploring two-dimensional (2D) magnetism for scientific and technological advances, but the intrinsic ferromagnetism has only been observed at low temperatures. Here, we report the observation of room temperature ferromagnetism in manganese selenide (MnSe$_x$) films grown by molecular beam epitaxy (MBE). Magnetic and structural characterization provides strong evidence that in the monolayer limit, the ferromagnetism originates from a vdW manganese diselenide (MnSe$_2$) monolayer, while for thicker films it could originate from a combination of vdW MnSe$_2$ and/or interfacial magnetism of $\alpha$-MnSe(111). Magnetization measurements of monolayer MnSe$_x$ films on GaSe and SnSe$_2$ epilayers show ferromagnetic ordering with large saturation magnetization of ~ 4 Bohr magnetons per Mn, which is consistent with density functional theory calculations predicting ferromagnetism in monolayer 1T-MnSe$_2$. Growing MnSe$_x$ films on GaSe up to high thickness (~ 40 nm) produces $\alpha$-MnSe(111), and an enhanced magnetic moment (~ 2x) compared to the monolayer MnSe$_x$ samples. Detailed structural characterization by scanning transmission electron microscopy (STEM), scanning tunneling microscopy (STM), and reflection high energy electron diffraction (RHEED) reveal an abrupt and clean interface between GaSe(0001) and $\alpha$-MnSe(111). In particular, the structure measured by STEM is consistent with the presence of a MnSe$_2$ monolayer at the interface. These results hold promise for potential applications in energy efficient information storage and processing.

Citations (571)

Summary

  • The paper demonstrates that epitaxial monolayer MnSe films exhibit robust intrinsic ferromagnetism with a saturation magnetization of approximately 4 Bohr magnetons per Mn atom.
  • It employs molecular beam epitaxy along with advanced characterization techniques, including STEM, STM, XRD, and AFM, to detail structural and magnetic properties.
  • The findings pave the way for integrating 2D magnetic materials into spintronic applications such as low-energy non-volatile memory and sensor systems.

Room Temperature Intrinsic Ferromagnetism in Epitaxial Manganese Selenide Films in the Monolayer Limit

The experimental observation and theoretical understanding of two-dimensional (2D) magnetism have been topics of intense research. In the pursuit of practical 2D magnetic materials viable at room temperature, the study of epitaxial manganese selenide (MnSe) films, especially in monolayer form, presents significant implications. This paper focuses on the synthesis and characterization of MnSe films grown by molecular beam epitaxy (MBE), demonstrating room-temperature intrinsic ferromagnetism.

The core achievement of the study is the successful demonstration of room-temperature ferromagnetism in monolayer MnSe films. Previous forays into 2D van der Waals (vdW) magnets revealed ferromagnetism only at cryogenic temperatures, hence the current findings significantly advance the field. The research utilized an array of characterization techniques, including SQUID magnetometry for magnetic behavior analysis and a combination of scanning transmission electron microscopy (STEM), scanning tunneling microscopy (STM), x-ray diffraction (XRD), and atomic force microscopy (AFM) for structural insights.

The MnSe monolayers, when deposited on GaSe or SnSe substrates, exhibited a saturation magnetization consistent with density functional theory predictions of approximately 4 Bohr magnetons per Mn atom. This supports the assertion of intrinsic ferromagnetism in these 2D systems. Further, this saturation magnetization remained notably robust across different substrates, indicating a strong intrinsic property rather than an artifact of the substrate interaction.

Structurally, the research identified a clean, abrupt interface between the monolayers and the GaSe substrate, with the MnSe monolayers forming a vdW-bonded structure as evidenced by STEM and XRD analyses. As the thickness of MnSe increased, an α-MnSe(111) phase emerged. Notably, the presence of this bulk phase, which traditionally is not ferromagnetic, suggests complex interfacial or vdW-layer derived magnetic phenomena.

The implications of these findings are multi-faceted. On a theoretical level, they support existing predictions about high-temperature ferromagnetism in vdW materials with particular attention to lattice structure and electronic states. Practically, the integration of room-temperature magnetic materials into electronic and spintronic devices is greatly facilitated, opening possibilities for low energy spintronic applications, such as proximity-coupled non-volatile memory and logic devices, and magnetic sensor systems.

Future research trajectories might involve exploring other vdW ferromagnetic materials and furthering the understanding of interfacial effects between different vdW layers. Moreover, direct examination of magnetic properties through techniques like spin-polarized STM could unveil richer physics underpinning the observed ferromagnetism. Additionally, exploring electric-field manipulations and heterostructure engineering could tailor these 2D magnets for specific technological applications.

In conclusion, the confirmation of room-temperature ferromagnetism in monolayer MnSe marks a significant development, potentially catalyzing advancements across both fundamental research and applied technology utilizing 2D materials. The study expands the horizons for future explorations into novel materials and underscores the complex interplay of atomic structure and magnetic properties in defining the next generation of electronic materials.

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