Single Crystal Ruddlesden-Popper and Dion-Jacobson Metal Halide Perovskites for Visible Light Photodetectors: Present Status and Future Perspectives.

2D metal halide perovskites (MHPs), mainly the studied Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) phases, have gained enormous popularity as optoelectronic materials owing to their self-assembled multiple quantum well structures, tunable semiconducting properties, and improved structural stability compared to their bulk 3D counterparts. The performance of polycrystalline thin film devices is limited due to the formation of defects and trap states. However, as studied so far, single crystal-based devices can provide a better platform to improve device performance and investigate their fundamental properties more reliably. This Review provides the first comprehensive report on the emerging field of RP and DJ perovskite single crystals and their use in visible light photodetectors of varied device configurations. This Review structurally summarizes the 2D MHP single crystal growth methods and the parameters that control the crystal growth process. In addition, the characterization techniques used to investigate their crystal properties are discussed. The review further provides detailed insights into the working mechanisms as well as the operational performance of 2D MHP single crystal photodetector devices. In the end, to outline the present status and future directions, this Review provides a forward-looking perspective concerning the technical challenges and bottlenecks associated with the developing field of RP and DJ perovskite single crystals. Therefore, this timely review will provide a detailed overview of the fast-growing field of 2D MHP single crystal-based photodetectors as well as ignite new concepts for a wide range of applications including solar cells, photocatalysts, solar H production, neuromorphic bioelectronics, memory devices, etc.