Merits and Challenges of Ruddlesden-Popper Soft Halide Perovskites in Electro-Optics and Optoelectronics.

Following the rejuvenation of 3D organic-inorganic hybrid perovskites, like CH3 NH3 PbI3 , (quasi)-2D Ruddlesden-Popper soft halide perovskites R2 An -1 Pbn X3 n +1 have recently become another focus in the optoelectronic and photovoltaic device community. Although quasi-2D perovskites were first introduced to stabilize optoelectronic/photovoltaic devices against moisture, more interesting properties and device applications, such as solar cells, light-emitting diodes, white-light emitters, lasers, and polaritonic emission, have followed. While delicate engineering design has pushed the performance of various devices forward remarkably, understanding of the fundamental properties, especially the charge-transfer process, electron-phonon interactions, and the growth mechanism in (quasi)-2D halide perovskites, remains limited and even controversial. Here, after reviewing the current understanding and the nexus between optoelectronic/photovoltaic properties of 2D and 3D halide perovskites, the growth mechanisms, charge-transfer processes, vibrational properties, and electron-phonon interactions of soft halide perovskites, mainly in quasi-2D systems, are discussed. It is suggested that single-crystal-based studies are needed to deepen the understanding of the aforementioned fundamental properties, and will eventually contribute to device performance.