Two-dimensional (2D) Dion–Jacobson (DJ) perovskites typically outperform Ruddlesden–Popper (RP) analogs in terms of photodetection (PD). However, the mechanism behind this enhanced performance remains elusive. Theoretical calculations for elucidating interlayer spacer conformation-induced multiple hydrogen bonds in 2D perovskite are presented, along with the synthesis of DPAPbBr₄ (DPB) single crystals (SCs) and their PD properties under X-ray/ultraviolet (UV) excitation. The high-quality DPB SC enhances PD with exceptional photoresponse attributes, including a high on/off ratio (4.89 × 10⁴), high responsivity (2.44 A W⁻¹), along with large dynamic linear range (154 dB) and low detection limit (7.1 nW cm⁻²), which are currently the best results among 2D perovskite SC detectors, respectively. Importantly, high-resolution images are obtained under UV illumination with weak light levels. The SC X-ray detector exhibits a high sensitivity of 663 µC Gy_air⁻¹ cm^–2 at 10 V and a detection limit of 1.44 µGy_air s⁻¹. This study explores 2D DJ perovskites for efficient and innovative optoelectronic applications.

中文翻译：

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间隔构象在二维钙钛矿中诱导多个氢键以实现高效光电器件

二维 (2D) 迪翁-雅各布森 (DJ) 钙钛矿在光电检测 (PD) 方面通常优于鲁德尔斯登-波普尔 (RP) 类似物。然而，这种增强性能背后的机制仍然难以捉摸。提出了阐明二维钙钛矿中层间间隔构象诱导的多重氢键的理论计算，以及 DPAPbBr ₄ (DPB) 单晶 (SC) 的合成及其在 X 射线/紫外线 (UV) 激发下的 PD 特性。高质量 DPB SC 增强了 PD 的卓越光响应属性，包括高开/关比 (4.89 × 10 ⁴ )、高响应度 (2.44 A W⁻ ¹ )、大动态线性范围 (154 dB) 和低检测限（7.1 nW cm⁻ ²），分别是目前二维钙钛矿 SC 探测器中最好的结果。重要的是，高分辨率图像是在弱光水平的紫外线照射下获得的。 SC X 射线探测器在 10 V 电压下表现出 663 µC Gy_空气⁻ ¹ cm ^–2的高灵敏度，检测限为 1.44 µGy_空气s⁻ ¹。这项研究探索了 2D DJ 钙钛矿在高效和创新光电应用中的应用。