Excited State Dynamics and Nonlinear Optical Properties of Two-Dimensional Hybrid Halide Perovskite Films

Chemical vapor deposition (CVD), without the use of solvents, is an efficient method for producing high-quality two-dimensional (2D) Ruddlesden-Popper-type hybrid lead-halide perovskite films such as BA₂PbI₄ and PEA₂PbI₄ [1]. Gaining insights into excited state dynamics and nonlinear optical properties of these perovskites is crucial for their use in optoelectronic applications. Employing broadband transient absorption spectroscopy and time-resolved photoluminescence, we explore excited state dynamics in these 2D perovskite systems. Our findings reveal that the carriers have fast cooling times, indicating an absence of phonon bottleneck process. The decay dynamics of the band-edge bleach show notable contributions from Auger recombination, due to the presence of free carriers alongside excitons. Furthermore, nonlinear optical studies indicate a high conversion efficiency for third-harmonic generation, underscoring the potential of these materials for frequency conversion and advanced photonic applications. This work contributes to a deeper understanding of structural and dynamic characteristics of CVD grown 2D hybrid halide perovskites.

[1] C. J. Arendse, R. Burns, D. Beckwitt, D. Babaian, S. Klue, D. Stalla, E. Karapetrova, P. F. Miceli, and S. Guha, ACS Appl. Mater. Interfaces 15 (50), 59055 (2023).