Discovery of an Above-Room-Temperature Antiferroelectric in Two-Dimensional Hybrid Perovskite

Abstract

Antiferroelectric materials have been regarded as a promising candidate for electronic energy storage devices, due to their natural double polarization versus electric field (P–E) hysteresis loops. Currently, two-dimensional organic–inorganic hybrid perovskites with structural diversity and tunability, have received blooming interests, whereas above-room-temperature antiferroelectrics are still unreported in this perovskite system. Herein, for the first time, we successfully acquire a two-dimensional Ruddlesden–Popper hybrid perovskite antiferroelectric, ((CH3)2CHCH2NH3)2CsPb2Br7 (1), which shows an above-room-temperature Curie temperature at 353 K, trigging by the synergistic dynamic motion of inorganic Cs atoms and organic isobutylammonium cations. Intriguingly, the antiferroelectricity of 1 existing over a wide temperature range of 298–353 K are revealed by the distinct double P–E hysteresis loops. Besides, 1 possesses remarkable energy storage efficiency up to 69%, comparable to those of some reported inorganic antiferroelectric ceramics, promoting 1 potential application in energy storage devices. This work provides an avenue to construct novel antiferroelectric materials for high-performance electronic device applications.

Multilayered 2D Cesium‐Based Hybrid Perovskite with Strong Polarization Sensitivity: Dimensional Reduction of CsPbBr3

“…For instance, intrinsic linear dichroism of the multilayered 2D hybrid perovskite (isobutylammonium) 2 (MA)Pb 2 I 7 enables remarkable polarized‐light photoelectric detection behaviors . This design strategy was recently extended to the cesium‐based perovskites, and a few 2D Cs‐containing hybrid perovskites were fabricated by alloying organic moieties into the prototypic CsPbBr 3 such as (isobutylammonium) 2 CsPb 2 Br 7 and ( n ‐butylammonium) 2 CsPb 2 Br 7 . The results suggest that the strategy of dimensional reduction is effective to explore the new 2D materials.…”

“…[18][19][20][21][22][23][24][25][26] For instance, intrinsic linear dichroism of the multilayered 2D hybrid perovskite (isobutylammonium) 2 (MA)Pb 2 I 7 enables remarkable polarized-light photoelectric detection behaviors. [27] This design strategy was recently extended to the cesium-based perovskites, and af ew 2D Cscontaining hybrid perovskites were fabricated by alloying organic moieties into the prototypic CsPbBr 3 such as (isobutylammonium) 2 CsPb 2 Br 7 [28] and (n-butylammonium) 2 CsPb 2 Br 7 . [29] The resultss uggest that the strategy of dimensionalr eduction is effective to explore the new 2D materials.D espite great efforts, 2D analogues of this Cs-based hybrid perovskite system are quite scarce and their potential applications for polarizedlight detection remainahuge blank.I nt his context, it is urgently demandeda nd significant to reduce the dimensionality of inorganic CsPbBr 3 perovskite lattice to the highly anisotropic 2D subclasst oward polarization-sensitive photodetection.…”

Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

“…Slicing of 3D perovskite lattice along (100), (110), (111) crystallographic planes with the elimination of the octahedra lying in the slicing plane lead to common two‐dimensional (2D) perovskites with single‐octahedra or thicker slabs . Lowering the dimensionality to 2D with corner‐sharing octahedral layers and bulky organic cations separating perovskite layers gives rise to increased structural diversity and new functionalities . Besides, 2D hybrid perovskites have attracted much attention as alternative photovoltaic materials because of an improved stability arising from hydrophobic interactions, which block moisture diffusion in the material .…”

“…[8] Lowering the dimensionality to 2D with corner-sharing octahedral layers and bulky organic cations separating perovskite layers gives rise to increased structural diversity and new functionalities. [9][10][11] Besides,2 Dh ybrid perovskites have attracted much attention as alternative photovoltaic materials because of an improved stability arising from hydrophobic interactions,w hich block moisture diffusion in the material. [12][13][14] In 2D perovskites,t here is no Goldschmidtstolerance factor restriction.…”

Highly‐Anisotropic Dion–Jacobson Hybrid Perovskite by Tailoring Diamine into CsPbBr3 for Polarization‐Sensitive Photodetection

“…[ 10 ] This design strategy has been well employed to modulate the optical bandgap of 2D Ruddlesden–Popper (RP) hybrid perovskites, of which optical anisotropy and tunability allow for polarized‐light detection. [ 11 ] For instance, the wide‐bandgap 2D hybrid perovskite of ( n ‐butylammonium) 2 (methy‐lammonium)Pb 2 Br 7 was reported, showing a large dichroism ratio to polarized‐light. [ 12 ] Similarly, it is proposed that the DJ‐type 2D perovskites also enable the optical absorption anisotropy and polarization‐sensitive responses.…”