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Circular dichroism in non-chiral metal halide perovskites

Sercel, Peter C. and Vardeny, Zeev Valy and Efros, Alexander L. (2020) Circular dichroism in non-chiral metal halide perovskites. Nanoscale, 12 (35). pp. 18067-18078. ISSN 2040-3364. doi:10.1039/d0nr05232a.

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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 of helical excitonic 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.

Item Type:Article
Related URLs:
URLURL TypeDescription Information Paper
Sercel, Peter C.0000-0002-1734-3793
Vardeny, Zeev Valy0000-0002-2298-398X
Efros, Alexander L.0000-0003-1938-553X
Additional Information:© 2020 The Royal Society of Chemistry. Submitted 13 Jul 2020; Accepted 17 Aug 2020; First published 17 Aug 2020. Note added after first publication: This article replaces the version published on 17th August 2020, which contained an error in Equation 13 that incorrectly omitted the identity matrix symbol, and incorrect references to two equations in the main body of text. The first of these references was in the sentence beginning “Although the off-diagonal terms in Hamiltonian described by eqn (17)....” and has been changed to read “Although the off-diagonal terms in the Hamiltonian described by eqn (13)....” The second reference was in the sentence beginning “Fig. 3 shows the exciton energies calculated along the Ky direction using eqn (18)...” and has been changed to read “Fig. 3 shows the exciton energies calculated along the Ky direction using eqn (14)...” P. C. S. and Z. V. V. acknowledge support from the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE) an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the US Department of Energy through contract number DE-AC36-08G028308. Al. L. E. acknowledges support from the US Office of Naval Research and the Laboratory-University Collaboration Initiative (LUCI) program of the DoD Basic Research Office. The authors acknowledge Dr Haoliang Liu for useful discussions, Aditi Chandrashekar for assistance with manuscript preparation and Prof. D. J. Norris for a critical reading of the manuscript and valuable comments. The authors declare no competing financial interests.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC36-08G028308
Office of Naval Research (ONR)UNSPECIFIED
Subject Keywords:chirality, circular dichroism, lead halide perovskite, hybrid organic inorganic perovskite, Rashba effect, exciton fine structure, nanoplatelet
Issue or Number:35
Record Number:CaltechAUTHORS:20200803-084556906
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Official Citation:Circular dichroism in non-chiral metal halide perovskites. Nanoscale, 2020, 12, 18067-18078; doi: 10.1039/d0nr05232a
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104695
Deposited By: Tony Diaz
Deposited On:03 Aug 2020 15:59
Last Modified:16 Nov 2021 18:34

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