Magnetic Field Tunable Polaritons in the Ultrastrong Coupling Regime in CrSBr

Collective excitations of bound electron-hole pairs, i.e., excitons, are ubiquitous in condensed matter systems, and it has been shown that they can strongly couple to other degrees of freedom, such as spin, orbital, and lattice. Among van der Waals materials with pronounced excitonic responses, CrSBr has attracted significant interest due to a very large energy shift of its fundamental bright exciton (at 1.36 eV) under an external magnetic field. This effect has been associated with an increased interlayer electronic hopping when the magnetic order is switched from antiferromagnetic to ferromagnetic by an external magnetic field, enabling its optical detection. In this work, we report the observation of a second bright excitonic resonance (at 1.76 eV), displaying a 5-fold enhancement of the magnetically induced energy shift to ∼100 meV, which we associate to a decreased spatial localization and increased interband nature compared to the fundamental exciton. Moreover, we show how the light-matter interaction reaches the ultrastrong regime where this exciton hybridizes with the cavity modes of photons confined to CrSBr flakes, forming polaritons with a Rabi splitting of <i>ℏ</i>Ω_R ≃ 372 meV, of the same order of magnitude as the one reported for the first exciton. These results expand the understanding of the relationship between the optical response and band structure of CrSBr and clarify the essential ingredients for optimizing magneto-electronic coupling for applications.