Tunable Ferroelectricity in Ruddlesden-Popper Halide Perovskites

Zhang, Q., Solanki, A., Parida, K., Giovanni, D., Li, M., Jansen, T. L. C., Pshenichnikov, M. S. & Sum, T. C., 10-Apr-2019, In : ACS Applied Materials & Interfaces. 11, 14, p. 13523-13532 10 p.

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  • Tunable Ferroelectricity in Ruddlesden–Popper Halide Perovskites

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Ruddlesden-Popper (RP) halide perovskites are the new kids on the block for high-performance perovskite photovoltaics with excellent ambient stability. The layered nature of these perovskites offers an exciting possibility of harnessing their ferroelectric property for photovoltaics. Adjacent polar domains in a ferroelectric material allow the spatial separation of electrons and holes. Presently, the structure-function properties governing the ferroelectric behavior of RP perovskites are an open question. Herein, we realize tunable ferroelectricity in 2-phenylethylammonium (PEA) and methylammonium (MA) RP perovskite (PEA)(2)(MA)((n) over bar -1)Pb(n) over barI3 (n) over bar +1. Second harmonic generation (SHG) confirms the noncentrosymmetric nature of these polycrystalline thin films, whereas piezoresponse force microscopy and polarization-electric field measurements validate the microscopic and macroscopic ferroelectric properties. Temperature-dependent SHG and dielectric constant measurements uncover a phase transition temperature at around 170 degrees C in these films. Extensive molecular dynamics simulations support the experimental results and identified the correlated reorientation of MA molecules and ion translations as the source of ferroelectricity. Current-voltage characteristics in the dark reveal the persistence of hysteresis in these devices, which has profound implications for light-harvesting and light-emitting applications. Importantly, our findings disclose a viable approach for engineering the ferroelectric properties of RP perovskites that may unlock new functionalities for perovskite optoelectronics.

Original languageEnglish
Pages (from-to)13523-13532
Number of pages10
JournalACS Applied Materials & Interfaces
Issue number14
Publication statusPublished - 10-Apr-2019


  • Ruddlesden-Popper perovskites, ferroelectricity, second harmonic generation, polarization-electric field, and molecular simulation, ORGANOMETALLIC HALIDE, CARRIER DYNAMICS, HIGH-PERFORMANCE, CH3NH3PBI3, LEAD, TEMPERATURE, ENERGY, HYSTERESIS, DOMAINS, LENGTHS

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