Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.141
Publication date: 11th July 2022
A striking difference between lead-halide perovskites and conventional semiconductors (e.g., silicon, III-V’s) is the dual ionic-covalent bond nature within the anionic inorganic framework. This weaker bond nature compared to the purely covalent bond of conventional semiconductors results in the mechanically soft and dynamically disordered perovskite lattice whose alteration affects the optoelectronic properties and the stability of these solids. Thus, metal-halide perovskites are particularly sensitive to variations in composition, fabrication and external stimuli that can induce strain in the material, interesting for developing next-generation memory devices, sensors, and energy-storage technologies. Layered Dion–Jacobson (DJ) and Ruddlesden–Popper (RP) hybrid perovskites are promising materials for optoelectronic applications due to their modular structure. To fully exploit their functionality, mechanical stimuli can be used to control their properties without changing the composition. However, the responsiveness of these systems to pressure compatible with practical applications and industrial fabrication methods (<1 GPa) remains unexploited. Hydrostatic pressure is used to investigate the structure–property relationships in representative iodide and bromide DJ and RP 2D perovskites based on 1,4-phenylenedimethylammonium (PDMA) and benzylammonium (BzA) spacers in the 0–0.35 GPa pressure range. Pressure-dependent X-ray scattering measurements reveal that lattices of these compositions monotonically shrink and density functional theory calculations provide insights into the structural changes within the organic spacer layer. These structural changes affect the optical properties; the most significant shift in the optical absorption is observed in (BzA)2PbBr4 under 0.35 GPa pressure, which is attributed to an isostructural phase transition. Surprisingly, the RP and DJ perovskites behave similarly under pressure, despite the different binding modes of the spacer molecules. This study provides important insights into how the manipulation of the crystal structure affects the optoelectronic properties of such materials, whereas the reversibility of their response expands the perspectives for future applications in e.g., sensors, actuators.
The work of L.A.M. and B.E. was part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of A.D. was supported by the EPFL-MPI Joint Research Center. B.E. and L.A.M. are grateful for the NWO Vidi grant 016.Vidi.179.005 and J.V.M. is grateful for the Swiss National Foundation PRIMA grant no. 19374 and NCCR Bio-Inspired Materials. U.R. acknowledges Swiss National Science Foundation Grant No. 200020-185092 and the NCCR-MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge Paul Scherrer Institute, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline X04SA of the SLS.
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