Silicon-Inspired Analysis of Interfacial Recombination in Perovskite Photovoltaics
Sarah Gillespie a b, Jerome Gautier a, Julia van der Burgt a, John Anker b, Bart Geerligs b, Gianluca Coletti b c, Erik Garnett a d
a AMOLF Institute, Science Park 104, Amsterdam, 1098XG The Netherlands
b TNO Energy Transition, Westerduinweg 3, Petten, 1755LE Netherlands
c School of Photovoltaic and Renewable Energy Engineering, University of New South Wales, Sydney, NSW 2052 Australia
d Institute of Physics, University of Amsterdam, Science Park 904, Amsterdam, 1098XH The Netherlands
Oral, Sarah Gillespie, presentation 073
Publication date: 6th February 2024

The performance of both single junction (SJ) perovskite solar cells and perovskite-silicon tandem cells have tremendously improved in recent years; respective certified efficiencies currently stand at 26.1% and 33.7%[1]. However, a considerable fraction of the remaining photovoltaic losses is attributed to carrier recombination at the perovskite interface. To mitigate such losses, interfacial extraction layers must be reviewed to determine whether substitutions or additional (mono)layers are required to further improve the photovoltage of the device. Addressing this requirement, this work presents a facile framework elucidating how time-resolved photoluminescence spectroscopy (TRPL) measurements can be utilised to locate points of recombination in perovskite solar cells. Drawing inspiration from well-established silicon PV analytical methods, we show how TRPL analysis can be extended to determine the bulk and surface lifetimes, surface recombination velocity (SRV), the recombination parameter, J0, and the implied open-circuit voltage (iVoc) of any perovskite device configuration[2,3]. Following this framework, we experimentally compare the extent of perovskite passivation on 18 contacts that are of interest in perovskite photovoltaics, discussing differences in electron transport layer (ETL) and hole transport layer (HTL) materials, their deposition methods and position in the stack. Furthermore, the iVoc calculated from the TRPL-based framework are directly compared to the determined iVoc from photoluminescence quantum yields, noting the benefits and caveats in both techniques. Finally, the hypothetical iVoc from full cell stacks based on the summation of the contact SRVs are compared to true solar cell Voc. We emphasise that this novel and simple technique serves as a practical guide for screening and selecting multifunctional, passivating perovskite contact layers in next generation SJ and tandem solar cells. Just as with more established silicon solar cells, most of the material and interface analysis can be done without making full devices or measuring power conversion efficiency. These purely optical measurements are actually preferable when studying the quality of bulk and interfacial passivation approaches, since they remove complicating effects from poor carrier extraction. 

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