We investigate the Cr electronic structure and excitations in CrSBr, a layered magnetic semiconductor, using a combination of resonant x-ray spectroscopic techniques. X-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) spectra collected at the Cr L2,3 edges reveal significant linear dichroism, which arises from the distorted octahedral environment surrounding the Cr3+ ions. The origin of the bright excitons observed in this compound is examined through a comparison of the d-d excitations identified in the RIXS spectra, the x-ray excited optical luminescence (XEOL) spectra, and previously reported optical spectroscopic and theoretical studies. To further understand these phenomena, we develop a multiplet model based on a crystal electric field (CEF) approach that accounts for the local environment of Cr ions. This model successfully reproduces several experimental features, while also suggesting strong hybridization effects between Cr 3d orbitals and ligands that are not fully captured by the present framework. These findings advance our understanding of the electronic structure and excitonic behavior in CrSBr and provide a foundation for future in-situ and operando studies of CrSBr-based devices for spintronic and optoelectronic applications.
@article{arxiv.2501.04751,
title = {Resonant X-ray spectroscopies on Chromium $3\textit{d}$ orbitals in CrSBr},
author = {Victor Porée and Alberto Zobelli and Amit Pawbake and Jakub Regner and Zdenĕk Sofer and Clément Faugeras and Alessandro Nicolaou},
journal= {arXiv preprint arXiv:2501.04751},
year = {2025}
}