Probing defects and spin-phonon coupling in CrSBr via resonant Raman scattering

Abstract

Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, we correlate defects in mono- to multilayer CrSBr with their structural, vibrational and magnetic properties. We use resonant Raman scattering to reveal distinct vibrational defect signatures. In pristine CrSBr, we show that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. We show that environmental exposure causes drastic degradation in monolayers, with the formation of intralayer defects. Through deliberate ion irradiation, we tune the formation of defect modes, which we show are strongly polarized and resonantly enhanced, reflecting the quasi-1D electronic character of CrSBr. Strikingly, we observe pronounced signatures of spin-phonon coupling of the intrinsic phonon modes and the ion beam induced defect modes throughout the magnetic transition temperature. Overall, we demonstrate that CrSBr shows air stability above the monolayer threshold, and provide further insight into the quasi-1D physics present. Moreover, we demonstrate defect engineering of magnetic properties and show that resonant Raman spectroscopy can serve as a direct fingerprint of magnetic phases and defects in CrSBr.

arXiv commentmain: 15 pages, 5 figures; SI: 16 pages, 15 figures

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• Paramagnetic Electronic Structure of CrSBr: Comparison between Ab Initio GW Theory and Angle-Resolved Photoemission Spectroscopy
• Ferromagnetic interlayer coupling in CrSBr crystals irradiated by ions
• Charge Density Wave and Ferromagnetism in Intercalated CrSBr
• Raman Polarization Switching in CrSBr
• Strain Engineering of Magnetoresistance and Magnetic Anisotropy in CrSBr
• Defect complexes in CrSBr revealed through electron microscopy and deep learning
• Magnetically Modulated Electrical Switching in an Antiferromagnetic Transistor
• Resonance Raman Scattering and Anomalous Anti-Stokes Phenomena in CrSBr
• Intrinsic defects as a source of $\text{n}$-type conductivity in CrSBr
• Interplay of vibrational, electronic, and magnetic states in CrSBr
• Magneto-Excitonic Duality From Monolayer to Trilayer CrSBr
• Excitonic optical absorption in strained monolayer CrSBr
• Magnetic field tuning of modulated magnetic orders in CrOCl at the two-dimensional limit