Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV16)
Publication date: 28th March 2016
Layered (2D) hybrid perovskites are attracting great attention as solution processable and low-cost white light emissive materials [1,2]. Although ultra-broadband photoluminescence is highly attractive for solid-state lightning and displays, it appears to be intrinsically different from the sharp emission typical of excitonic states, and the nature of its emission mechanism remains elusive. In this work, we investigate the photoluminescence properties of broadband emitting 2D perovskites (EDBE)PbCl4 and (EDBE)PbBr4. Combining steady state and time resolved spectroscopy with ab-initio calculations, we show that their unusually large Stokes shift and broadband photoluminescence derive from carriers self-trapped within their own lattice distortion field, in form of localized polarons. Polaron formation is fostered by the quantum confinement induced by the layered structure, which strongly enhances charge-phonon correlations. We identify the nature of the intra-band emissive states as polaronic excitons deriving from charge self-localization within the inorganic lattice, with the consequent formation of self-trapped electrons (STEL) Pb23+ and self-trapped holes (STH) Pb3+, X2- (X=Cl, Br). This model could apply to other 2D white light emitting perovskites or 3D perovskites characterized by strong electron-phonon correlations, which may aid the design of new perovskite materials with improved emissive properties.
[1] Dohner, E. R., Jaffe, A., Bradshaw, L. R. & Karunadasa, H. I. Intrinsic White-Light Emission from Layered Hybrid Perovskites. Journal of the American Chemical Society. 136, 13154-13157 (2014).
[2] Yangui, A. et al. Optical Investigation of Broadband White-Light Emission in Self-Assembled Organic–Inorganic Perovskite (C6H11NH3)2PbBr4. The Journal of Physical Chemistry C. 119, 23638-23647 (2015).
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