4.8 Article

Circular dichroism in non-chiral metal halide perovskites

Journal

NANOSCALE
Volume 12, Issue 35, Pages 18067-18078

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d0nr05232a

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Funding

  1. Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE) an Energy Frontier Research Center - Office of Basic Energy Sciences, Office of Science within the US Department of Energy [DE-AC3608G028308]
  2. US Office of Naval Research
  3. Laboratory-University Collaboration Initiative (LUCI) program of the DoD Basic Research Office

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We demonstrate theoretically that non-chiral perovskite layers can exhibit circular dichroism (CD) in the absence of a magnetic field and without chiral activation by chiral molecules. The effect is shown to be due to splitting ofhelicalexcitonic states which can form in structures of orthorhombic or lower symmetry that exhibit Rashba spin effects. The selective coupling of these helical exciton states to helical light is shown to give rise to circular dichroism. Polarization dependent absorption is shown to occur due to the combined effect of Rashba splitting, in-plane symmetry breaking, and the effect of the exciton momentum on its fine structure, which takes the form of Zeeman splitting in an effective magnetic field. This phenomenon, which can be considered as a manifestation of extrinsic chirality, results in significant CD with an anisotropy factor of up to 30% in orthorhombic perovskite layers under off-normal, top illumination conditions, raising the possibility of its observation in non-chiral perovskite structures.

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