Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
Publication date: 30th March 2023
The exceptional optoelectronic properties of metal halide perovskites (MHPs) are presumed to arise, at least in part, from the peculiar interplay between the inorganic metal-halide sublattice and the atomic or molecular cations enclosed in the cage voids. The latter can exhibit a roto-translative dynamics, which is shown here to be at the origin of the structural behavior of MHPs as a function of temperature, pressure and composition. The application of high hydrostatic pressure allows for unraveling the nature of the interaction between both sublattices, characterized by the simultaneous action of hydrogen bonding and steric hindrance. In particular, we find that under the conditions of unleashed cation dynamics, the key factor that determines the structural stability of MHPs is the repulsive steric interaction rather than hydrogen bonding. Taking as example the results from pressure and temperature-dependent photoluminescence and Raman experiments on MAPbBr3 but also considering the pertinent MHP literature, we provide a general picture about the relationship between the crystal structure and the presence or absence of cationic dynamic disorder. The reason for the structural sequences observed in MHPs with increasing temperature, pressure, A-site cation size or decreasing halide ionic radius is found principally in the strengthening of the dynamic steric interaction with the increase of the dynamic disorder. In this way, we have deepened our fundamental understanding of MHPs; knowledge that could be coined to improve performance in future optoelectronic devices based on this promising class of semiconductors.
The Spanish Ministerio de Ciencia e Innovación (MICINN) is gratefully acknowledged for its support through grant CEX2019-000917-S (FUNFUTURE) in the framework of the Spanish Severo Ochoa Centre of Excellence program and the AEI/FEDER(UE) grants PGC2018-095411-B-100 (RAINBOW) and PID2021-128924OB-I00 (ISOSCELLES). The authors also thank the Catalan agency AGAUR for grant 2017-SGR-00488 and the National Network "Red Perovskitas" (MICINN funded). K.X. acknowledges a fellowship (CSC201806950006) from China Scholarship Council and the PhD programme in Materials Science from Universitat Autònoma de Barcelona in which he was enrolled. B.C. thanks the EPSRC for PhD studentship funding via the University of Bath, CSCT CDT (EP/G03768X/1).
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