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Circularly Polarized Photoluminescence from Chiral Perovskite Thin Films at Room Temperature

Cite this: ACS Nano 2020, 14, 6, 7610–7616
Publication Date (Web):May 27, 2020
https://doi.org/10.1021/acsnano.0c03628
Copyright © 2020 American Chemical Society

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    Abstract

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    Hybrid organic–inorganic perovskites allow the synthesis of high-quality, nanostructured semiconducting films via easily accessible solution-based techniques. This has allowed tremendous development in optoelectronic applications, primarily solar cells and light-emitting diodes. Allowed by the ease of access to nanostructure, chirality has recently been introduced in semiconducting perovskites as a promising way to obtain advanced control of charge and spin and for developing circularly polarized light sources. Circular polarization of photoluminescence (CPL) is a powerful tool to probe the electronic structure of materials. However, CPL in chiral perovskites has been scarcely investigated, and a study in bulk thin films and at room temperature is still missing. In this work, we fabricate bromine-based chiral perovskites by using a bulky chiral organic cation mixed with CsBr, resulting in Ruddlesden–Popper perovskite thin films. We measure CPL on these films at room temperature and, by using unpolarized photoexcitation, we record a degree of circular polarization of photoluminescence in the order of 10–3 and provide a full spectral characterization of CPL. Our results show that chirality is imparted on the electronic structure of the semiconductor; we hypothesize that the excess in polarization of emitted light originates from the charge in the photogenerated Wannier exciton describing an orbit in a symmetry-broken environment. Furthermore, our experiments allow the direct measurement of the magnetic dipole moment of the optical transition, which we estimate to be ≥0.1 μB. Finally, we discuss the implications of our findings on the development of chiral semiconducting perovskites as sources of circularly polarized light.

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    • UV–vis absorption spectrum and SEM image of a sample based on PbBr2:CsBr:(S)-NEABr precursor mix, CD spectrum of a sample based on PbBr2:CsBr:(R)-NEABr precursor mix, PL/gPL measurements as function of time under constant photoexcitation (PDF)

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