Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.016
Publication date: 23rd September 2021
Given the vast chemical space of layered hybrid perovskites, the systematic analysis of structure-property relationship in this type of materials is of high importance. Understanding the differences between Dion-Jacobson and Ruddlesden-Popper (RP) hybrid halide perovskites is limited. Thus, in this study we analyze compositions based on iodide or bromide for the halide and on phenylenedimethanammonium (PDMA) and benzylammonium (BN) as the spacers, which are structurally comparable. We use hydrostatic pressure as a tool to investigate the structure-property relationship. We probe optical, structural properties in the range of 0-0.35 GPa, which effects might be comparable to the processes occurring in the optoelectronic devices (polaron induced strain, lattice mismatch, chemical strain). At this pressure levels we observe optical bandgap reduction in all the compositions. The most significant shift (-54.9 meV) is recorded in (BN)2PbBr4 composition under 0.35 GPa pressure. Structural analysis reveals that lattice of all compositions monotonically shrinks but (BN)2PbBr4 experience an abrupt change in the lattice parameters lenght at 0.14 GPa. In addition, though the compression along all axes is comparable, there is consistent trend in all the systems showing slightly larger compression along the c axis with a more pronounced trend in the (BN)2PbBr4. Bulk modulus calculations reveal a much softer perovskite lattice in the latter composition, in agreement with the much larger shift of the excitonic peak observed as a function of pressure. Similarly, the other three compositions show a comparable bulk modulus as expected from the trend of the excitonic peak under pressure. Molecular dynamics provide additional insights into structure-property relationship. With this work we extend the knowledge about the layered hybrid perovskites based on aromatic spacers providing important insights into the mechanochromic properties of layered hybrid perovskites. Finally, the unique reversibility of their mechanochromic response in this mild pressure range opens new perspective towards the utility of layered hybrid perovskites as platforms for amphidynamic materials and mechanophores, which expands the perspectives for their future applications.
The work of L.A.M. is 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. is 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.
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