High-quality CsPbBr₃ single-crystal films prepared by facile TIF-CVD and their multiscenario optoelectronic...

All-inorganic CsPbBr₃ perovskites feature exceptional optoelectronic properties and distinct nonlinear optical characteristics, making them highly promising for advanced photonic applications. However, state-of-the-art two-photon absorption photodetectors typically rely on intricate heterojunction configurations, which pose substantial bottlenecks to their large-scale integration and practical deployment. This study employed the "tube-in-furnace" chemical vapor deposition (TIF-CVD) method to prepare centimeter-scale high-quality CsPbBr₃ single-crystal films and systematically investigated their optoelectronic properties. The films demonstrated low-threshold amplified spontaneous emission ~24.7 μJ/cm² under 266 nm one-photon excitation (OPE) and stable lasing emission under 1064 nm two-photon excitation (TPE). Two-photon fluorescence imaging showed higher spatial resolution and contrast than single-photon imaging. Photodetectors with a simple electrode structure achieved high responsivity ~0.82 A/W under OPE and ~9.78 μA/W under TPE. This work provides a high-quality material platform for multifunctional optoelectronic integration and an economically feasible foundation for large-scale applications.