Direct observation of anisotropic exciton dispersion in the 2D semiconductor CrSBr

Abstract

We report momentum-resolved measurements of exciton dispersion in multilayer CrSBr using defocus-engineered electron energy-loss spectroscopy, supported by first-principles calculations. A pronounced in-plane anisotropy is observed, with the exciton exhibiting a linear dispersion along $Γ$Y within $\lvert \boldsymbol{q} \rvert$ < 0.007 Å$^{-1}$, while remaining nearly dispersionless along $Γ$X. The slope reaches 7.02 eV Å, among the largest reported in low-dimensional systems. The calculations reproduce the experimentally observed linear dispersion, confirming its intrinsic origin. We attribute the anisotropic dispersion to the long-range electron--hole exchange interaction, enhanced by strong out-of-plane confinement and governed by the directional selection rules of the transition dipole moment. Comparative measurements across the magnetic phase transition from the paramagnetic to the A-type antiferromagnetic state show that the dispersion remains essentially unchanged, indicating negligible coupling between exciton propagation and magnetic order. These results establish CrSBr as a model system for investigating anisotropic exciton dynamics in low-symmetry layered semiconductors.