Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
DOI: https://doi.org/10.29363/nanoge.hopv.2023.168
Publication date: 30th March 2023
In a perovskite solar cell, the charge transport layers on either side of the light-absorbing perovskite layer provide the asymmetry necessary to extract electrons and holes through opposite sides of the device. As the fabrication of high-quality thin films of metal halide perovskite matures, the performance losses are increasingly dominated by the properties of these charge transport layers (CTLs) and their interfaces [1]. In this work, some of the most widely used CTLs were deposited on 3D lead halide perovskite layers and then studied using a range of time-resolved spectroscopies, the results of which were compared to a numerical simulation.
Using contactless optical techniques allowed the study of bilayers in which only a single interface was present. Bilayers were formed by depositing the electron transport layers (ETLs) PCBM and C60, or the hole transport layer (HTL) Spiro-OMeTAD, on top of a high performance triple cation [2] perovskite layer (FA0.79MA0.16Cs0.05)Pb(I0.83Br0.17)3. Time-resolved terahertz (THz) photoconductivity and transient absorption (TA) spectroscopies were used to track the perovskite carrier population from femtosecond to nanosecond timescales, whilst time resolved photoluminescence (TRPL) followed the population decay on nanosecond to microsecond timescales. Bilayers incorporating fullerene-based ETLs (PCBM and C60) were found to have significantly different carrier dynamics to the bilayers using the Spiro-OMeTAD HTL.
The carrier dynamics were then analysed using a numerical simulation of the spatially- and temporally-dependent carrier density, including the Poisson equation to account for charge separation across the interface, which is usually ignored. This charge separation was found to have a significant effect on the simulated carrier dynamics. To provide additional constraints for the comparison between numerical simulation and experimental data, different initial carrier distributions were generated by exciting the bilayers with different wavelengths and on alternate sides, adjacent to or away from the CTL. This comparison suggests that the PCBM and C60 layers have significant interface recombination on sub-nanosecond timescales, whereas Spiro-OMeTAD may have much slower hole extraction and interface recombination. We discuss the significant ramifications of these findings for device performance.
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