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Hybrid halide perovskite materials are thin-film semiconductors of interest to various applications in optoelectronics.1–3  They are soft yet crystalline solution-processable mixed ionic–electronic conductors that display excellent optoelectronic characteristics, which are highly versatile and tuneable by using different compositional elements.4–9  A hybrid organic–inorganic perovskite structure can be described by the AMX3 formula (Fig. 1A). It is based on an inorganic {MX6} octahedral corner-sharing framework, where M is a divalent metal (mostly Pb2+ or Sn2+), X is a halide anion (Cl, Br, I), and A central cation (A-cation), which can be either inorganic (e.g. Cs+) or organic (e.g. methylammonium (MA), formamidinium (FA)).9–13  Hybrid perovskites have demonstrated excellent light absorption and long-living photogenerated charges with long diffusion lengths and high defect tolerance, despite routine preparation by solution-processing.9,14,15  Their optoelectronic properties are defined by the orbital (M–X) interactions within the inorganic framework, whereas organic components indirectly contribute by affecting the structural characteristics.9,16  These properties can be tailored by using different AMX3 perovskite compositions, changing their octahedral connectivity, as well as by applying other organic species as additives or molecular modulators (Fig. 1B and C).16–18  The incorporation of larger organic moieties within the perovskite framework can lead to the formation of low-dimensional or layered (2D) perovskite structures (Fig. 1D and E).19–23  They represent a class of materials typically described by the S2An−1MnX3n+1 or S′An−1MnX3n+1 formulae, where A (MA+, FA+, Cs+) are central A-cations, M divalent metal cations, X halide anions (Cl, Br, I), and S or S′ (typically mono- or bifunctional ammonium cations, respectively) organic spacers, which often form Ruddlesden–Popper (RP) or Dion Jacobson (DJ) phases (Fig. 1D and E).24,25  Layered hybrid perovskites feature a layered structure of perovskite slabs separated by the organic spacers, where the value of n represents the number of {MX6} octahedra in the perovskite stack (n = 1, 2, etc.).22,23  The organic spacer affects the structure, orientation, as well as the morphology of the resulting material, and consequently its optoelectronic properties.23  Most commonly used organic spacers are based on hydrophobic alkyl chains terminated by ammonium groups, such as n-buthylammonium (BA) or phenylethylammonium (PEA),23  which are electronically insulating. These materials have nonetheless already shown promise in optoelectronic devices, such as solar cells,26,27  light-emitting diodes,28,29  piezoelectrics,30  transistors,30,31  and memory elements.5,8,31,32 

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