Publication date: 17th February 2025
Organic-inorganic metal halide perovskites have emerged as attractive materials for solar cells with power-conversion efficiencies of single-junction devices now exceeding 26%. However, degradation, defective interfaces with charge extraction layers, the low hurdle for ionic migration, and the structural flexibility of the perovskite structure still pose both opportunities and challenges to their commercialization in light-harvesting applications. Combinatorial characterization approaches are vital for probing and analysing such instabilities.
We demonstrate a combined modelling and experimental approach[1] towards exploring the effects of energy-level alignment at the interface between wide-bandgap mixed-halide perovskites and charge-extraction layers, unravelling separate loss factors and highlighting avenues for improving open-circuit voltage.
We further highlight the potential of optical-pump THz-probe spectroscopy following controlled intervals of air exposure as an ideal technique to monitor air-induced degradation of optoelectronic parameters such as charge-carrier mobilities and recombination rates in low-bandgap lead-tin iodide perovskites.[2][3] We explore the best choice of A-cation in lead-tin iodide perovskites with intermediate lead-tin ratios and find that FASn0.5Pb0.5I3 emerges as the most promising contender.
In addition, we utilize a combination of ultra-low frequency Raman and infrared terahertz time-domain spectroscopies to provide a systematic examination[4,5] of the ultra-low frequency vibrational response for a wide range of metal-halide semiconductors, showing that such effects results from high anharmonicity of specific Raman-active modes.
We further probe the charge-carrier transport in layered, two-dimensional (2D) metal halide perovskites that have been found to improve the stability of metal halide perovskite thin films and devices. We demonstrate unexpectedly high densities of sustained populations of free charge carriers, surpassing the Saha equation predictions,[6] and demonstrate a high degree of transport anisotropy in highly oriented thin films.[7]
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