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Abstract The van der Waals magnets CrX3(X = I, Br, and Cl) exhibit highly tunable magnetic properties and are promising candidates for developing novel two‐dimensional (2D) spintronic devices such as magnetic tunnel junctions and spin tunneling transistors. Previous studies of the antiferromagnetic CrCl3have mainly focused on mechanically exfoliated samples. Controlled synthesis of high quality atomically thin flakes is critical for their technological implementation but has not been achieved to date. This work reports the growth of large CrCl3flakes down to monolayer thickness via the physical vapor transport technique. Both isolated flakes with well‐defined facets and long stripe samples with the trilayer portion exceeding 60 µm have been obtained. High‐resolution transmission electron microscopy studies show that the CrCl3flakes are single crystalline in the monoclinic structure, consistent with the Raman results. The room temperature stability of the CrCl3flakes decreases with decreasing thickness. The tunneling magnetoresistance of graphite/CrCl3/graphite tunnel junctions confirms that few‐layer CrCl3possesses in‐plane magnetic anisotropy and Néel temperature of 17 K. This study paves the path for developing CrCl3‐based scalable 2D spintronic applications.
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Controlling Magnetic and Optical Properties of the van der Waals Crystal CrCl 3− x Br x via Mixed Halide Chemistry
Abstract Magnetic van der Waals (vdW) materials are the centerpiece of atomically thin devices with spintronic and optoelectronic functions. Exploring new chemistry paths to tune their magnetic and optical properties enables significant progress in fabricating heterostructures and ultracompact devices by mechanical exfoliation. The key parameter to sustain ferromagnetism in 2D is magnetic anisotropy—a tendency of spins to align in a certain crystallographic direction known as easy‐axis. In layered materials, two limits of easy‐axis are in‐plane (XY) and out‐of‐plane (Ising). Light polarization and the helicity of topological states can couple to magnetic anisotropy with promising photoluminescence or spin‐orbitronic functions. Here, a unique experiment is designed to control the easy‐axis, the magnetic transition temperature, and the optical gap simultaneously in a series of CrCl3−xBrxcrystals between CrCl3withXYand CrBr3with Ising anisotropy. The easy‐axis is controlled between the two limits by varying spin–orbit coupling with the Br content in CrCl3−xBrx. The optical gap, magnetic transition temperature, and interlayer spacing are all tuned linearly withx. This is the first report of controlling exchange anisotropy in a layered crystal and the first unveiling of mixed halide chemistry as a powerful technique to produce functional materials for spintronic devices.
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- PAR ID:
- 10060636
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 30
- Issue:
- 25
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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