Tunable Ferroelectricity in Ruddlesden-Popper Halide Perovskites

Qiannan Zhang, Ankur Solanki, Kaushik Parida, David Giovanni, Mingjie Li, Thomas L. C. Jansen, Maxim S. Pshenichnikov, Tze Chien Sum

Research output: Contribution to journalArticleAcademicpeer-review

18 Citations (Scopus)

Abstract

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
Volume11
Issue number14
DOIs
Publication statusPublished - 10-Apr-2019

Keywords

  • 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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