Exciton dressing by extreme nonlinear magnons in a layered semiconductor

Abstract

Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency-mixing processes are central to communication and attosecond science, and extreme (>sixth-order) harmonic generation provides broad wavelength conversion. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear optomagnonic coupling. In the layered antiferromagnetic semiconductor CrSBr, we observe exciton states dressed by up to 20 harmonics of magnons, resulting from their extreme nonlinearities. We also create tunable optical sidebands via sum- and difference-frequency generation between two optically bright magnon modes under symmetry-breaking magnetic fields. Moreover, we can tune the observed difference-frequency generation mode into resonance with one of the fundamental magnons, which results in parametric amplification of magnons. Our findings realize the modulation of the optical-frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide a method for optomagnonic neuromorphic computing devices.