Shuai Xinting, Sidhik Siraj, Xu Mingrui, Zhang Xiang, De Siena Michael, Pedesseau Laurent, Zhang Hao, Gao Guanhui, Puthirath Anand B, Li Wenbin, Agrawal Ayush, Xu Jianan, Hou Jin, Persaud Jessica H, Daum Jeremy, Mishra Anamika, Wang Yafei, Vajtai Robert, Katan Claudine, Kanatzidis Mercouri G, Even Jacky, Ajayan Pulickel M, Mohite Aditya D
Department of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United States.
Department of Chemistry and Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States.
ACS Appl Mater Interfaces. 2024 Sep 4;16(35):46560-46569. doi: 10.1021/acsami.4c05329. Epub 2024 Aug 23.
The 2D Ruddlesden-Popper (RP) perovskites CsPbICl (Pb-based, = 1) and CsSnICl (Sn-based, = 1) stand out as unique and rare instances of entirely inorganic constituents within the more expansive category of organic/inorganic 2D perovskites. These materials have recently garnered significant attention for their strong UV-light responsiveness, exceptional thermal stability, and theoretically predicted ultrahigh carrier mobility. In this study, we synthesized Pb and Sn-based = 1 2D RP perovskite films covering millimeter-scale areas for the first time, utilizing a one-step chemical vapor deposition (CVD) method under atmospheric conditions. These films feature perovskite layers oriented horizontally relative to the substrate. Multilayered CsPbICl (Pb-based, = 2) and CsSnICl (Sn-based, = 2) films were also obtained for the first time, and their crystallographic structures were refined by combining X-ray diffraction (XRD) and density functional theory (DFT) calculations. DFT calculations and experimental optical spectroscopy support band-gap energy shifts related to the perovskite layer thickness. We demonstrate bias-free photodetectors using the Sn-based, = 1 perovskite with reproducible photocurrent and a fast 84 ms response time. The present work not only demonstrates the growth of high-quality all-inorganic multilayered 2D perovskites via the CVD method but also suggests their potential as promising candidates for future optoelectronic applications.
二维Ruddlesden-Popper（RP）钙钛矿CsPbICl（铅基，n = 1）和CsSnICl（锡基，n = 1）在更广泛的有机/无机二维钙钛矿类别中是独特且罕见的完全无机成分实例。这些材料最近因其强烈的紫外光响应性、出色的热稳定性以及理论预测的超高载流子迁移率而备受关注。在本研究中，我们首次在大气条件下利用一步化学气相沉积（CVD）方法合成了覆盖毫米级区域的铅基和锡基n = 1的二维RP钙钛矿薄膜。这些薄膜的钙钛矿层相对于衬底水平取向。还首次获得了多层CsPbICl（铅基，n = 2）和CsSnICl（锡基，n = 2）薄膜，并通过结合X射线衍射（XRD）和密度泛函理论（DFT）计算对其晶体结构进行了优化。DFT计算和实验光谱学支持了与钙钛矿层厚度相关的带隙能量移动。我们展示了使用锡基n = 1钙钛矿的无偏压光电探测器，其具有可重复的光电流和84毫秒的快速响应时间。本工作不仅证明了通过CVD方法生长高质量的全无机多层二维钙钛矿，还表明了它们作为未来光电子应用有前途候选材料的潜力。
