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Phase-change behavior of hot-pressed methylammonium lead bromide hybrid perovskites

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Abstract

The investigation of hot-pressed methylammonium lead bromide (MAPbBr3) is reported. The as-prepared materials consisted of microcrystallites (30–500 μm size) with a non-centrosymmetric pseudo-cubic tetragonal crystalline structure (P4 mm space group). The thermal analysis under air showed a thermal stability of MAPbBr3 perovskite till T = 250 °C and a broad endothermic event at T = 371 °C (melting point of solid PbBr2). Under increasing pressure at room temperature, the MA–Pb–Br system retained the pseudo-cubic tetragonal structure, the optical adsorption spectra displayed a strong absorption edge between 570 and 572 nm, and the Tauc plots revealed a direct semiconducting behavior with band energy gaps around 2.20(± 0.01) eV. The steady-state emission (PL) photoluminescence spectra (excitation wavelengths λexc = 380 nm) showed an emission band at ~ 574 nm. With increase in the temperature (under constant pressure and treatment time), the MA–Pb–Br system turned into the higher cubic symmetry (space group \(Pm\, \bar{3} m\)), the absorption edges shifted to 571–575 nm, and at T = 120 °C, the absorbance profile begins to increase at higher wavelengths (> 600 nm). By increasing the pressure at constant temperature, the perovskite adopted the cubic structure and a slight decrease in the energy band gap (2.17 eV for T = 150 °C and P = 15 MPa) was recorded. With increase in the hot-pressing time at T = 150 °C and P = 20 MPa, the optical absorption edges remained at ~ 575 nm; however, the decrease in the absorbance can indicate a degradation of the materials. The changes in the emission mechanism(s) of the hot-pressed materials can be related to the observed change in the crystalline structure and morphology.

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Acknowledgements

Many thanks are owed to Mr. J.-C. Jaud for the technical assistance in XRD analysis and to Mrs. C. Fasel for the technical assistance in the thermal measurements. The author thank the Federal Ministry of Research and Development (BMBF) (Project “Perosol” Nr. 03SF0483B) for the financial support during this work.

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  1. Earth and Materials Science Department, Technische Universität Darmstadt, Otto-Berndt-Strasse 3, 64287, Darmstadt, Germany

    Lucangelo Dimesso, Carolin Wittich, Thomas Mayer & Wolfram Jaegermann

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  1. Lucangelo Dimesso
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Correspondence to Lucangelo Dimesso.

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Figure S1

Schematic representation of the hot-pressing procedure (Patm is the starting atmospheric pressure, Pn (n ≥ 1) are the intermediate pressure steps, Pfin is the setup pressure, RT is the room temperature, Tfin is the setup temperature) (TIFF 654 kb)

Figure S2

Typical XRD patterns of pressed MAPbBr3 systems at different pressures for t = 600 s at room temperature (TIFF 1259 kb)

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Dimesso, L., Wittich, C., Mayer, T. et al. Phase-change behavior of hot-pressed methylammonium lead bromide hybrid perovskites. J Mater Sci 54, 2001–2015 (2019). https://doi.org/10.1007/s10853-018-3009-6

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