Abstract Abundant chemical diversity and structural tunability make organic–inorganic hybrid perovskites (OIHPs) a rich ore for ferroelectrics. However, compared with their inorganic counterparts such as BaTiO3, their ferroelectric key properties, including large spontaneous polarization (P s), low coercive field (E c), and strong second harmonic generation (SHG) response, have long been great challenges, which hinder their commercial applications. Here, a quasi-one-dimensional OIHP DMAGeI3 (DMA = Dimethylamine) is reported, with notable ferroelectric attributes at room temperature: a large P s of 24.14 μC/cm2 (on a par with BaTiO3), a low E c below 2.2 kV/cm, and the strongest SHG intensity in OIHP family (about 12 times of KH2PO4 (KDP)). Revealed by the first-principles calculations, its large P s originates from the synergistic effects of the stereochemically active 4s 2 lone pair of Ge2+ and the ordering of organic cations, and its low kinetic energy barrier of small DMA cations results in a low E c. Our work brings the comprehensive ferroelectric performances of OIHPs to a comparable level with commercial inorganic ferroelectric perovskites.
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