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    Observation of Anisotropic Dispersive Dark-Exciton Dynamics in CrSBr

    J. Sears1, B. Zager1,2, W. He1,*, C. A. Occhialini2,3, Y. Shen1,†,∥, M. Lajer1, J. W. Villanova4,‡, T. Berlijn4, F. Yakhou-Harris5 et al.

    N. B. Brookes5, D. G. Chica6, X. Roy6, E. Baldini7, J. Pelliciari2, V. Bisogni2, S. Johnston8,9, M. Mitrano10, and M. P. M. Dean1,§

    • *Present address: Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
    • †Present address: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
    • ‡Present address: Department of Physics and Astronomy, Middle Tennessee State University, Murfreesboro, Tennessee 37132, USA.
    • §Contact author: mdean@bnl.gov
    • ∥School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.

    Phys. Rev. Lett. 135, 146503 – Published 1 October, 2025

    DOI: https://doi.org/10.1103/fz3h-6jdx

    Abstract

    Many-body excitons in CrSBr are attracting intense interest in view of their highly anisotropic magneto-optical coupling and their potential for novel optical interfaces within spintronic and magnonic devices. Characterizing the orbital character and propagation of these electronic excitations is crucial for understanding and controlling their behavior; however, this information is challenging to access. High resolution resonant inelastic x-ray scattering is a momentum-resolved technique that can address these crucial questions. We present measurements collected at the Cr L3-edge which show a rich spectrum of excitations with a variety of spin-orbital characters. While most of these excitations appear to be localized, the dispersion of the lowest energy dark exciton indicates that it is able to propagate along both the a and b directions within the planes of the crystal. This two-dimensional character is surprising as it contrasts with electrical conductivity and the behavior of the bright exciton, both of which are strongly one dimensional. The discovery of this propagating dark exciton highlights an unusual coexistence of one- and two-dimensional electronic behaviors in CrSBr.

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