Vapor Growth of All-Inorganic 2D Ruddlesden–Popper Lead- and Tin-Based Perovskites

• Published in: ACS applied materials & interfaces 2024-09, Vol.16 (35), p.46560-46569
• Main Authors: 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.
• Format: Article
• Language: English
• Subjects: Chemical Sciences; Functional Nanostructured Materials (including low-D carbon); Material chemistry
• ISSN: 1944-8244; 1944-8252; 1944-8252
• DOI: 10.1021/acsami.4c05329

The 2D Ruddlesden–Popper (RP) perovskites Cs2PbI2Cl2 (Pb-based, n = 1) and Cs2SnI2Cl2 (Sn-based, n = 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 n = 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 Cs3Pb2I3Cl4 (Pb-based, n = 2) and Cs3Sn2I3Cl4 (Sn-based, n = 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, n = 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.