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

Abstract

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.

Dual Modifications of TiO2/1D g-C3N4 Nanocomposites and Metal–Organic Framework-Derived Porous CuO/Carbon for High-Performance Perovskite Solar Cells

“…This material will also reduce lead leakages and improve the device’s stability. However, inorganic HTL deposition on top of the perovskite layer is a more complex process requiring specialized device construction . To overcome these issues, the researchers focus on low-temperature solution-processed carbon paste to improve the performance of PSCs.…”

Advances and challenges in molecular engineering of 2D/3D perovskite heterostructures

“…This type of cation exchange and structural conversion mechanism has also been demonstrated in perovskite nanocrystals. 19 Based on this method, different strategies, including solvent engineering, 20–24 annealing engineering, 25,26 and processing engineering 27–29 have been developed to precisely manipulate the microstructures. Among them, for any given 2D perovskites, the ligand configuration is one of the most critical parameters that determines the structures and subsequently the optoelectronic properties and long-term stability of the desired materials.…”