UC Santa Barbara

Light-matter interactions in semiconductors are uniformly treated within the electric dipole approximation; multipolar interactions are considered "forbidden." We experimentally demonstrate that this approximation inadequately describes light emission in two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs), solution processable semiconductors with promising optoelectronic properties. By exploiting the highly oriented crystal structure, we use energy-momentum spectroscopies to demonstrate that an exciton-like sideband in 2D HOIPs exhibits a multipolar radiation pattern with highly directed emission. Electromagnetic and quantum-mechanical analyses indicate that this emission originates from an out-of-plane magnetic dipole transition arising from the 2D character of electronic states. Symmetry arguments and temperature-dependent measurements suggest a dynamic symmetry-breaking mechanism that is active over a broad temperature range. These results challenge the paradigm of electric dipole-dominated light-matter interactions in optoelectronic materials, provide new perspectives on the origins of unexpected sideband emission in HOIPs, and tease the possibility of metamaterial-like scattering phenomena at the quantum-mechanical level.