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Bright magnetic dipole radiation from two-dimensional lead-halide perovskites.

  • Author(s): DeCrescent, Ryan A
  • Venkatesan, Naveen R
  • Dahlman, Clayton J
  • Kennard, Rhys M
  • Zhang, Xie
  • Li, Wenhao
  • Du, Xinhong
  • Chabinyc, Michael L
  • Zia, Rashid
  • Schuller, Jon A
  • et al.
Abstract

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.

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