Resolving the Ultrafast Charge Carrier Dynamics of 2D and 3D Domains within a Mixed 2D/3D Lead‐Tin Perovskite

Mixed 2D/3D perovskite materials are of particular interest to the photovoltaics and light‐ emitting diode (LED) communities due to their impressive opto‐electronic properties alongside improved moisture stability compared to conventional 3D perovskite absorbers. Here, a mixed lead‐tin perovskite containing distinct, self‐assembled domains of either 3D structures or highly phase‐pure Ruddlesden–Popper 2D structures is studied. The complex energy landscape of the material is revealed with ultrafast optical transient absorption measurements. It is shown that charge transfer between these microscale domains only occurs on nanosecond timescales, consistent with the large size of the domains. Using optical pump‐terahertz probe spectroscopy, the effective charge‐carrier mobility is shown to be an intermediary between analogous pure 2D and 3D perovskites. Furthermore, detailed analysis of the free carrier recombination dynamics is presented. By combining results from a range of excitation wavelengths within a full dynamic model of the photoexcited carrier population, it is shown that the 2D domains in the film exhibit remarkably similar carrier dynamics to the 3D domains, suggesting that long‐range charge‐transport should not be impeded by the heterogeneous structure of the material. Using a series of laser pulses to probe charge carriers on picosecond timescales; a metal halide perovskite semiconductor, with promising potential applications in next‐generation solar cells and light‐ emitting diodes, which consists of a mix of 2D‐like and 3D‐like domains is studied. Surprisingly, the dimensionality is found to have only a minor effect on the dynamics of the charges.