Stable CsPbX3 mixed halide alloyed epitaxial films prepared by pulsed laser deposition

The pulsed laser deposition (PLD) technique has been proved to be able to grow oxide thin films with high structural quality with precisely controlled composition and thickness to achieve designed optical and electronical properties established in alloyed semiconductors and heterostructures. In this Letter, inorganic halide perovskite CsPb(IxClyBr1−x−y)3 epitaxial alloyed films on (001)-SrTiO3(STO) substrates were grown by PLD. The film crystal quality, phase stability, and the epitaxial relationship between the film and substrate were characterized with a detailed x-ray diffraction technique like high-resolution reciprocal spatial mapping and ϕ-scan. In addition, the photocarrier dynamics of the alloyed epitaxial films were investigated by photophysics spectroscopy, including steady and femtosecond transient optical absorption spectroscopy and temperature-dependent and time-resolved photoluminescence spectroscopy. The bandgap of the CsPbX3 films was tuned from 1.75 to 2.98 eV by substituting X with I/Br/Cl and their mixture of different ratios. Free exciton emissions were observed at a low temperature photoluminescence spectrum (PL, 10 K), which confirmed the high crystal and optical quality of the epitaxial perovskite alloyed films except the CsPbI3 film. The femtosecond transient absorption spectra also showed that such perovskite films are of very low concentration of exciton trap states. These results indicated that PLD is a powerful technology for growing high quality inorganic halide perovskite films with a tunable bandgap covering the full visible light range, which provided more options for CsPbX3 based panchromatic LED and other optoelectronic devices.