Two-Dimensional Layered Simple Aliphatic Monoammonium Tin Perovskite Thin Films and Potential Applications in Field-Effect Transistors

Abstract

Two-dimensional (2D) layered organic-inorganic perovskites have great potential for fabricating field-effect transistors due to their unique structure that enables the horizontal transport of charge carriers in metal-halide octahedra, resembling the transport behavior in semiconducting channels. Their electronic band structures are mainly dominated by the metal-halide octahedra, which eventually determine the optical and electrical characteristics, whereas organic cations have no direct contributions but would impact the electronic structures via distorting the octahedra. So far, high performance has been achieved in 2D Sn perovskites compared to their Pb counterparts because the intrinsic differences of Sn promote transport properties. The champion hole mobility has been obtained in single-ring aromatic phenylethylammonium tin iodide perovskite [(PEA)₂SnI₄]. However, simple aliphatic monoammonium tin perovskites and their device applications have rarely been reported. Herein, 2D layered n-butylammonium tin iodide perovskite [(BA)₂SnI₄] thin films have been synthesized by a spin-coating approach. A structural phase transition occurs at about 225 K in the films, accompanied by the changes in the photoluminescence peak and exciton binding energy. Longitudinal optical (LO) phonons are found to govern the scattering of charge carriers and excitons via the Fröhlich interactions in the temperature range 77-300 K. The first-principles calculations predict that the perovskite has excellent transport characteristics comparable to those of molybdenum disulfide (MoS₂) and methylammonium lead iodide perovskite (MAPbI₃). The (BA)₂SnI₄ thin film field-effect transistors constructed on polymer dielectrics with a maximum hole mobility of 0.03 cm² V^-1 s^-1 in ambient conditions have been successfully demonstrated for the first time. Our findings not only offer a deep insight into the physical properties of 2D layered aliphatic monoammonium tin perovskite thin films but also provide important experimental and theoretical guidance for their potential applications in lateral-type flexible optoelectronic devices.

Keywords: 2D layered n-butylammonium tin iodide perovskite thin films; crystallization dynamics; field-effect transistors; first-principles calculations; physical properties.