Unraveling Interface-Driven and Loss Mechanism-Centric Phenomena in 3D/2D Halide Perovskites: Prospects for Optoelectronic Applications.

In recent years, organic-inorganic metal halide perovskite solar cells (PSCs) have attracted considerable interest due to their remarkable and rapidly advancing efficiencies. Over the past decade, PSC efficiencies have significantly approached those of state-of-the-art silicon-based photovoltaics, making them a promising material. Currently, the scientific community widely recognizes the performance of 3D-PSCs and 2D-PSCs individually. However, when both are combined to form a heterostructure, the lattice and charge dynamics at the interface undergo a multitude of mechanisms that affect their performance. The interface between heterostructures facilitates the degradation of PSCs. The degradation pathways can be attributed to lattice distortions, inhomogeneous energy landscapes, interlayer ion migration, nonradiative recombination, and charge accumulation. This Review is dedicated to examining the phenomena that arise at the interface of 3D/2D halide perovskites and their related photophysical properties and loss mechanism processes. We mainly focus on the impact of lattice mismatch, energy level alignment, anomalous carrier dynamics, and loss mechanisms. We propose a "cause-impact-identify-rectify" approach to gain a comprehensive understanding of the ultrafast processes occurring within the material. Finally, we highlight the importance of advanced spectroscopic and imaging techniques in unraveling these intricate mechanisms. This discussion delves into the future possibilities of fabricating 3D/2D heterostructure-based optoelectronic devices, pushing the boundaries of performance across diverse fields. It envisions the creation of devices with unparalleled capabilities, exceeding the limitations of current technologies.