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Title: Tunable ferroelectricity in Ruddlesden-Popper halide perovskites
Authors: Zhang, Qiannan
Solanki, Ankur
Parida, Kaushik
Giovanni, David
Li, Mingjie
Jansen, Thomas L. C.
Pshenichnikov, Maxim S.
Sum, Tze Chien
Keywords: Science::Physics
Issue Date: 2019
Source: Zhang, Q., Solanki, A., Parida, K., Giovanni, D., Li, M., Jansen, T. L. C., . . . Sum, T. C. (2019). Tunable ferroelectricity in Ruddlesden-Popper halide perovskites. ACS Applied Materials & Interfaces, 11(14), 13523-13532. doi:10.1021/acsami.8b21579
Project: Ministry of Education AcRF Tier 1 grant RG173/16
Ministry of Education AcRF Tier 2 grant MOE2015-T2-2-015
Ministry of Education AcRF Tier 2 grant MOE2016-T2-1-034
Ministry of Education AcRF Tier 2 grant MOE2017-T2-1-110
Ministry of Education AcRF Tier 2 grant MOE2017-T2-2-002
Singapore National Research Foundation Competitive Research Program NRF-CRP14-2014-03
NRF Investigatorship Programme NRF-NRFI-2018-04
Journal: ACS Applied Materials & Interfaces
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) n̅-1Pb n̅I3 n̅+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.
ISSN: 1944-8244
DOI: 10.1021/acsami.8b21579
DOI (Related Dataset):
Schools: School of Materials Science & Engineering 
School of Physical and Mathematical Sciences 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Fulltext Permission: open
Fulltext Availability: With Fulltext
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