Structurally Tunable Two-Dimensional Layered Perovskites: From Confinement and Enhanced Charge Transport to Prolonged Hot Carrier Cooling Dynamics

[Image: see text] Two-dimensional (2D) layered metal halide perovskites are potential alternatives to three-dimensional perovskites in optoelectronic applications owing to their improved photostabilities and chemical stabilities. Recent investigations of 2D metal halide perovskites have demonstrated interesting optical and electronic properties of various structures that are controlled by their elemental composition and organic spacers. However, photovoltaic devices that utilize 2D perovskites suffer from poor device efficiency due to inefficient charge carrier separation and extraction. In this Perspective, we shed light on confinement control and structural variation strategies that provide better parameters for the efficient collection of charges. The influence of these strategies on the exciton binding energies, charge-carrier mobilities, hot-carrier dynamics, and electron–phonon coupling in 2D perovskites is thoroughly discussed; these parameters highlight unique opportunities for further system optimization. Beyond the tunability of these fundamental parameters, we conclude this Perspective with the most notable strategies for attaining 2D perovskites with reduced bandgaps to better suit photovoltaic applications.