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


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.

SUBMITTER: DeCrescent RA 

PROVIDER: S-EPMC7007269 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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

DeCrescent Ryan A RA   Venkatesan Naveen R NR   Dahlman Clayton J CJ   Kennard Rhys M RM   Zhang Xie X   Li Wenhao W   Du Xinhong X   Chabinyc Michael L ML   Zia Rashid R   Schuller Jon A JA  

Science advances 20200207 6


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 demons  ...[more]

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