Structural and optical properties of single- and few-layer magnetic semiconductor CrPS4

Abstract

Atomically thin binary 2-dimensional (2D) semiconductors exhibit diverse physical properties depending on their composition, structure and thickness. By adding another element in those materials, which will lead to formation of ternary 2D materials, the property and structure would greatly change and significantly expanded applications could be explored. In this work, we report structural and optical properties of atomically thin chromium thiophosphate (CrPS4), a ternary antiferromagnetic semiconductor. Its structural details were revealed by X-ray and electron diffractions. Transmission electron microscopy showed that preferentially-cleaved edges are parallel to diagonal Cr atom rows, which readily identified their crystallographic orientations. Strong in-plane optical anisotropy induced birefringence that also enabled efficient determination of crystallographic orientation using polarized microscopy. The lattice vibrations were probed by Raman spectroscopy for the first time and exhibited significant dependence on thickness of crystals exfoliated down to single layer. Optical absorption determined by reflectance contrast was dominated by d-d type transitions localized at Cr3+ ions, which was also responsible for the major photoluminescence peak at 1.31 eV. The spectral features in the absorption and emission spectra exhibited noticeable thickness-dependence and hinted a high photochemical activity for single layer CrPS4. The current structural and optical investigation will provide a firm basis for future study and application of this novel magnetic semiconductor.

arXiv comment32 pages, 5 figures

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• Ultrasensitive, Ultrafast and Gate-Tunable Two-Dimensional Photodetectors in Ternary Rhombohedral ZnIn2S4 for Optical Neural Networks
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• Electronic Correlations in Multiferroic van der Waals CuCrP${}_2$S6: Insights From X-Ray Spectroscopy and DFT
• Quantum Spin Hall Effect in Magnetic Graphene
• Configurable antiferromagnetic domains and lateral exchange bias in atomically thin CrPS4
• Resonant Raman Scattering of Few Layers CrBr${}_3$
• Magnetoresistance oscillations in vertical junctions of 2D antiferromagnetic semiconductor CrPS${}_4$
• Anomalous Tunneling Magnetoresistance Oscillation and Electrically Tunable Tunneling Anisotropic Magnetoresistance in Few-layer CrPS4
• Brightened Optical Transition as Indicator of Multiferroicity in a Layered Antiferromagnet
• Parameter free treatment of a layered correlated van der Waals magnet: CrPS${}_4$
• Optically Facet-Resolved Reaction Anisotropy in Two-Dimensional Transition Metal Dichalcogenides
• Tunable linear and nonlinear anomalous Hall transport in two-dimensional CrPS${}_4$
• Spin-flip optical excitations in van der Waals antiferromagnet CrPS${}_4$
• Growth of Large Crystals of Janus Phase RhSeCl Using Self-Selecting Vapour Growth
• Momentum-Resolved Electronic Structure and Orbital Hybridization in the Layered Antiferromagnet CrPS${}_4$
• Room Temperature Anisotropic Photoresponse in Low-Symmetry van der Waals Semiconductor CrPS${}_4$
• Activated Migration of Localized Ligand-Field Excitons in Atomically Thin CrCl3
• Spin Seebeck in the weak exchange coupled van der Waals antiferromagnet