Olasupo Oluwadara J, Adewolu Abiodun M, Khizr Mohammad, Manny Tarannuma F, Liu He, Shonde Tunde B, Islam Md S, Moslemi Sahel, Kim Ethan, Winfred J S Raaj V, Gamaralalage Thilina N D D, Hu Yan-Yan, Das Ranjan, Ma Biwu
Department of Chemistry and Biochemistry, Florida State University, Tallahassee, Florida, 32306, USA.
Department of Chemistry, University of West Florida, Pensacola, Florida, 32514, USA.
Angew Chem Int Ed Engl. 2025 Aug 25;64(35):e202509589. doi: 10.1002/anie.202509589. Epub 2025 Jul 9.
Zero-dimensional (0D) organic metal halide hybrids (OMHHs) are emerging materials with significant potential for optoelectronic applications, including direct X-ray detectors. While 0D OMHH single crystals exhibit excellent X-ray detection properties, their scalability remains a significant challenge due to the time-intensive growth process and difficulty in producing large single crystals exceeding a few centimeters. This limitation hinders their practicality for large-area detector applications. Here, we report for the first time the development of amorphous 0D OMHH films via solution processing for efficient direct X-ray detection. By reacting a non-crystalline organic halide, triphenyl(9-phenyl-9H-carbazol-3-yl)phosphonium bromide (TPPCarzBr), with zinc bromide (ZnBr), we have successfully produced amorphous 0D (TPPCarz)ZnBr films with controlled thickness via facile solution processing. The organic cations (TPPCarz⁺) feature a lower bandgap than the ZnBr anions, enabling efficient molecular sensitization, where ZnBr anions serve as X-ray absorbers and TPPCarz⁺ cations as charge transporters. Direct X-ray detectors based on 0D (TPPCarz)ZnBr films demonstrate outstanding performance, achieving a stable X-ray detection sensitivity of 2,165 µC Gy⁻cm⁻ at 20 Vmm⁻¹ and a detection limit of 6.01 nGy s⁻¹. The amorphous nature of these films enhances their processability, allowing for fabrication in various sizes and shapes, and making them highly adaptable for scalable detector applications.
零维（0D）有机金属卤化物杂化物（OMHHs）是一类新兴材料，在光电子应用领域具有巨大潜力，包括直接X射线探测器。尽管0D OMHH单晶展现出优异的X射线探测性能，但由于其生长过程耗时且难以制备出超过几厘米的大尺寸单晶，其可扩展性仍是一个重大挑战。这一限制阻碍了它们在大面积探测器应用中的实用性。在此，我们首次报道了通过溶液处理制备非晶态0D OMHH薄膜用于高效直接X射线探测。通过使非晶态有机卤化物三苯基（9-苯基-9H-咔唑-3-基）溴化鏻（TPPCarzBr）与溴化锌（ZnBr）反应，我们通过简便的溶液处理成功制备出了厚度可控的非晶态0D（TPPCarz）ZnBr薄膜。有机阳离子（TPPCarz⁺）的带隙低于ZnBr阴离子，从而实现了高效的分子敏化，其中ZnBr阴离子作为X射线吸收剂，TPPCarz⁺阳离子作为电荷传输体。基于0D（TPPCarz）ZnBr薄膜的直接X射线探测器表现出卓越性能，在20 Vmm⁻¹时实现了2,165 µC Gy⁻cm⁻的稳定X射线探测灵敏度以及6.01 nGy s⁻¹的探测限。这些薄膜的非晶态特性增强了其可加工性，允许制备各种尺寸和形状的探测器，使其非常适合可扩展探测器应用。
