Excitonic optical interface for GHz-THz collective excitations in a van der Waals magnet

Abstract

Collective spin and lattice excitations in quantum materials span energy scales from GHz to THz, yet establishing a unified optical interface for these modes remains a central challenge. Here we show that excitonic resonances in the van der Waals antiferromagnet CrSBr provide a broadband optical interface for such excitations. Using femtosecond broadband transient reflectivity, we resolve coherent GHz magnon and THz phonon modes that modulate the dielectric response over a wide spectral range. Despite their distinct microscopic origin and frequency scales, both excitations give rise to the same emergent optical signature: a resonance at 1.46 eV that is absent in steady-state spectra and exhibits a characteristic π-phase inversion, identifying it as a discrete excitonic transition. We attribute this behaviour to boson-driven modulation of the dielectric response, which transiently transfers spectral weight from a nominally dark exciton into an observable channel without requiring a finite equilibrium oscillator strength. Supported by many-body calculations, we assign this feature to a higher-energy exciton with distinct momentum and orbital character and strongly suppressed optical matrix elements. These results establish excitonic resonances in van der Waals magnets as a platform for interfacing collective excitations across GHz, THz and optical frequency scales.