Light-matter coupling via quantum pathways for spontaneous symmetry breaking in van der Waals antiferromagnetic semiconductors

Light-matter interaction simultaneously alters both the original material and incident light. Light not only reveals material details but also activates coupling mechanisms. The coupling has been demonstrated mechanically, for instance, through the patterning of metallic antennas, resulting in the emergence of plasmonic quasiparticles and enabling wavefront engineering of light via the generalized Snell’s law. However, quantum-mechanical light-matter interaction, wherein photons coherently excite distinct quantum pathways, remains poorly understood. Here, we report on quantum interference between light-induced quantum pathways through the orbital quantum levels and spin continuum. The quantum interference immediately breaks the symmetry of the hexagonal antiferromagnetic semiconductor FePS3. Below the Néel temperature, we observe the emergence of birefringence and linear dichroism, namely, quantum anisotropy due to quantum interference, which is further enhanced by the thickness effect. We explain the direct relevance of the quantum anisotropy to a quantum phase transition by spontaneous symmetry breaking in Mexican hat potential. Our findings suggest material modulation via selective quantum pathways through quantum light-matter interaction.