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Radiation‐Sensitive Layered Hybrid Double Perovskites Driven by a Dual‐Ion‐Woven Supramolecular Framework for X‐Ray Tomography

Xieming Xu, Hao Lu, Xiong Zhang, Lian Wang, Guiqing Feng, Luying Zheng, Xiaoming Jiang, Shaofan Wu, Shuai‐Hua Wang

2024Angewandte Chemie International Edition11 citationsDOIOpen Access PDF

Abstract

Abstract A promising candidate for X‐ray detection is layered hybrid double perovskites (LHDPs) with excellent structural stability, but their sensitivity is generally limited by unsatisfactory interlayer charge transport. Herein, employing one ethylenediamine (EDA) chain as a structural inducer, we successfully obtain unusual Dion‐Jacobson (DJ) phase LHDPs, (EDABr) 4 AgBiBr 8 and (EDABr) 4 CuBiBr 8 , featuring a Ruddlesden‐Popper‐like (RP‐like) interlayer. Thanks to the bridging of bromine anions, organic cations are linked via charge‐assisted hydrogen bonds, where two ionic spacers are orderly woven into a supramolecular framework. Consequently, the RP‐like interlayer space is regulated by the dual‐ion‐woven supramolecular framework with embedded charge‐assisted hydrogen bond networks, remarkably enriching interlayer interactions and boosting charge transport. Through theoretical calculations, structural roles of the supramolecular framework are elucidated by extra orbital contribution and large diffusion barrier of Br anions. As proof of concept, the sensitivity of RP‐like devices up to 5250 μC Gy air −1 cm −2 is a record‐high of LHDP‐based X‐ray detectors for now, while a low detection limit (91 nGy air s −1 ) and outstanding radiation‐resistant capability (50 Gy air ) are achieved. Moreover, an oriented membrane device is prepared to demonstrate high‐performance X‐ray tomography. These findings offer a brand‐new interlayer‐modulation strategy for the construction of sensitive and stable scintillation semiconductors.

Topics & Concepts

Supramolecular chemistryMaterials scienceHydrogen bondIonIonic bondingCrystallographyNanotechnologyCrystal structureChemistryMoleculeOrganic chemistryPerovskite Materials and ApplicationsAdvanced Condensed Matter PhysicsLuminescence Properties of Advanced Materials