Paramagnetic Electronic Structure of CrSBr: Comparison between Ab Initio GW Theory and Angle-Resolved Photoemission Spectroscopy

Abstract

We explore the electronic structure of paramagnetic CrSBr by comparative first principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent $GW$ theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QS$GW$ and QS$G\hat{W}$, respectively). Comparing the quasi-particle band structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of $\approx$ 2.1 eV.

arXiv comment11 pages, 12 figures

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Cited by in corpus (25)

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• Magnon-mediated exciton-exciton interaction in a van der Waals antiferromagnet
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• Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr
• Anisotropic effects in two-dimensional materials
• Charge transfer and asymmetric coupling of MoSe${}_2$ valleys to the magnetic order of CrSBr
• Raman Polarization Switching in CrSBr
• Charge transfer-induced Lifshitz transition and magnetic symmetry breaking in ultrathin CrSBr crystals
• Identifying band structure changes of FePS3 across the antiferromagnetic phase transition
• Distinct Magneto-Optical Response of Frenkel and Wannier Excitons in CrSBr
• Surface-Dominated Quantum Metric-Induced Nonlinear Transport in the Layered Antiferromagnet CrSBr
• Resonance Raman Scattering and Anomalous Anti-Stokes Phenomena in CrSBr
• Defect complexes in CrSBr revealed through electron microscopy and deep learning
• Magnetic Correlation Spectroscopy in CrSBr
• Excitons and trions in CrSBr bilayers
• Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets
• Exciton transport driven by spin excitations in an antiferromagnet
• An autoencoder for compressing angle-resolved photoemission spectroscopy data
• Intrinsic defects as a source of $\text{n}$-type conductivity in CrSBr
• Interplay of vibrational, electronic, and magnetic states in CrSBr
• Resonant X-ray spectroscopies on Chromium $3\text{d}$ orbitals in CrSBr
• Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition
• Theory of interaction-induced charge order in CrSBr
• Magneto-Excitonic Duality From Monolayer to Trilayer CrSBr
• Assessing Orbital Optimization in Variational and Diffusion Monte Carlo