Tunable Ferroelectricity in Ruddlesden-Popper Halide Perovskites.
ACS Appl Mater Interfaces
; 11(14): 13523-13532, 2019 Apr 10.
Article
em En
| MEDLINE
| ID: mdl-30854841
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) nÌ
-1Pb nÌ
I3 nÌ
+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 °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.
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2019
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Article