Publication date: 22nd July 2026
Lead halide perovskites have received great interest in recent years due to their excellent photovoltaic, optical (linear and nonlinear) and electrical properties. An efficient way to increase structural diversity and tune functional properties of hybrid lead halides is mixing of organic cations. The most famous subclasses of mixed-cation hybrid halide perovskites are multilayered Ruddlesden–Popper (RP, A’2An-1PbnX3n+1) and Dion–Jacobson (DJ, A”An-1PbnX3n+1) phases, where the parameter n defines the thickness of corner-sharing PbX₆ octahedral slabs, A’ and A” are large interlayer cations, and A denote small cations located in the perovskite cages [1]. These compounds exhibit improved environmental stability relative to their 3D counterparts and increasing n progressively reduces confinement effects, narrows the band gap, and enhances charge-carrier transport, thereby improving photovoltaic-relevant performance. It is worth noting that these compounds often crystallize in polar structures [2], which is prerequisite for piezo-, pyro- and ferroelectric properties and second-order nonlinear optical properties (e.g. second-harmonic generation, SHG). However, majority of these compounds exhibit in-plane polarization and only a handful of compounds with out-of-plane polarization are known. Mixing of organic cations may also lead to other type of structures, for instance, 3D perovskitoids such as (c-C3A)3(MA)3Pb5I16 (c-C3A= cyclopropylammonium, MA= methylammonium) or MPDA2FAPb4Br13 (MPDA = N-methylpropanediammonium, FA = formamidinium) [3,4].
In hybrid lead halides, structural distortions of the inorganic framework play a decisive role in governing emission characteristics, excitonic absorption energies, and the emergence of ferroelectricity or SHG activity upon symmetry breaking [5]. Therefore, a comprehensive understanding of the interplay between inorganic layer distortions and organic cation dynamics is essential for rational materials design of these compounds. In this contribution, we report temperature-dependent studies of selected mixed-cation lead halides comprising large mono and diammonium cations as well as small cage cations to elucidate mechanisms of the observed structural phase transitions and relation between structural changes and optoelectronic properties of these compounds.
This research was supported by the National Science Center (Narodowe Centrum Nauki) in Poland under project No. 2023/49/B/ST5/00119.
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