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The layered, air-stable van der Waals antiferromagnetic compound CrSBrexhibits pronounced coupling between its optical, electronic, and magneticproperties. As an example, exciton dynamics can be significantly influenced bylattice vibrations through exciton-phonon coupling. Using low-temperaturephotoluminescence spectroscopy, we demonstrate the effective coupling betweenexcitons and phonons in nanometer-thick CrSBr. By careful analysis, we identifythat the satellite peaks predominantly arise from the interaction between theexciton and an optical phonon with a frequency of 118 cm-1 (~14.6 meV) due tothe out-of-plane vibration of Br atoms. Power-dependent andtemperature-dependent photoluminescence measurements support exciton-phononcoupling and indicate a coupling between magnetic and optical properties,suggesting the possibility of carrier localization in the material. Thepresence of strong coupling between the exciton and the lattice may haveimportant implications for the design of light-matter interactions in magneticsemiconductors and provides new insights into the exciton dynamics in CrSBr.This highlights the potential for exploiting exciton-phonon coupling to controlthe optical properties of layered antiferromagnetic materials.

Strong Exciton-Phonon Coupling as a Fingerprint of Magnetic Ordering in van der Waals Layered CrSBr