Magneto-optical Kerr spectroscopy of exciton Rydberg states in a magnetic van der Waals heterostructure

Abstract

Excitonic states in two-dimensional semiconductors are sensitive to time-reversal symmetry breaking, yet how interfacial exchange acts on higher-lying exciton Rydberg states remains largely unexplored. Here we show that wavelength-resolved magneto-optical Kerr spectroscopy of a proximity-coupled MoSe$_2$/Fe$_3$GaTe$_2$ van der Waals heterostructure resolves magnetic symmetry breaking across the A- and B-exciton manifolds. Combining reflection, photoluminescence, and photoluminescence excitation spectroscopy with first-principles many-body calculations including screening by the metallic Fe$_3$GaTe$_2$ layer, we assign the strongly enhanced Kerr resonances to the ground and 2s states of both manifolds. Reversing the magnetic field inverts the polarity of every resonance. A field-odd/field-even decomposition confirms a magnetic origin. The opposite Kerr polarities of the A- and B-exciton manifolds can be explained by proximity-induced exchange coupling to the opposite valence-band spins of the two exciton series. Our results establish resonant Kerr spectroscopy as a sensitive probe of magnetically induced symmetry breaking across the excitonic manifold.