Large-Area Nanocrystalline Caesium Lead Chloride Thin Films: A Focus on the Exciton Recombination Dynamics

Caesium lead halide perovskites were recently demonstrated to be a relevant class of semiconductors for photonics and optoelectronics. Unlike CsPbBr₃ and CsPbI₃, the realization of high-quality thin films of CsPbCl₃, particularly interesting for highly efficient white LEDs when coupled to converting phosphors, is still a very demanding task. In this work we report the first successful deposition of nanocrystalline CsPbCl₃ thin films (70-150 nm) by radio frequency magnetron sputtering on large-area substrates. We present a detailed investigation of the optical properties by high resolution photoluminescence (PL) spectroscopy, resolved in time and space in the range 10-300 K, providing quantitative information concerning carriers and excitons recombination dynamics. The PL is characterized by a limited inhomogeneous broadening (~15 meV at 10 K) and its origin is discussed from detailed analysis with investigations at the micro-scale. The samples, obtained without any post-growth treatment, show a homogeneous PL emission in spectrum and intensity on large sample areas (several cm²). Temperature dependent and time-resolved PL spectra elucidate the role of carrier trapping in determining the PL quenching up to room temperature. Our results open the route for the realization of large-area inorganic halide perovskite films for photonic and optoelectronic devices.