Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr

Abstract

We present the evolution of the electronic structure of CrSBr from its antiferromagnetic ground state to the paramagnetic phase above T_N=132 K, in both experiment and theory. Low temperature angle-resolved photoemission spectroscopy (ARPES) results are obtained using a novel method to overcome sample charging issues, revealing quasi-2D valence bands in the ground state. The results are very well reproduced by our QSGŴ calculations, which further identify certain bands at the X points to be exchange-split pairs of states with mainly Br and S character. By tracing band positions as a function of temperature, we show the splitting disappears above T_N. The energy splitting is interpreted as an effective exchange splitting in individual layers in which the Cr moments all align, within the so-called A-type antiferromagnetic arrangement. Our results lay firm foundations for the interpretation of the many other intriguing physical and optical properties of CrSBr.

Published open access at https://doi.org/10.1038/s41699-024-00492-7 including supplementary information

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• Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets
• Directional Flow of Confined Polaritons in CrSBr
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• Intrinsic defects as a source of $\text{n}$-type conductivity in CrSBr
• Interplay of vibrational, electronic, and magnetic states in CrSBr
• Observation of anisotropic dispersive dark exciton dynamics in CrSBr
• Quasiparticle Description of Angle-Resolved Photoemission Spectroscopy for SrCuO2
• Magneto-Excitonic Duality From Monolayer to Trilayer CrSBr
• Momentum-Resolved Electronic Structure and Orbital Hybridization in the Layered Antiferromagnet CrPS${}_4$