Near-unity Charge Generation Yield towards high performance thick-junction Organic Solar Cells
Wei Li a, Stefan Zeiske a, Oskar Sandberg a, Drew Riley a, Paul Meredith a, Ardalan Armin a
a Sustainable Advanced Materials Program (Sêr SAM), Department of Physics, Singleton Park, Swansea, United Kingdom
International Conference on Hybrid and Organic Photovoltaics
Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Online, Spain, 2021 May 24th - 28th
Organizers: Marina Freitag, Feng Gao and Sam Stranks
Oral, Wei Li, presentation 015
Publication date: 11th May 2021

Organic solar cells (OSCs) have experienced an explosive development in the last 5 years with the emergence of the so-called fused-ring-based non-fullerene acceptors (NFAs), leading to power conversion efficiencies (PCEs) surpassing 18% recently and with 20% firmly on the radar.  Such performance metrics are now challenging the traditional inorganic semiconductor photovoltaics and have aroused increased interest in manufacturing. In this regard, realizing high-efficiency OSCs with thick-junction active layer while understanding the charge generation/recombination mechanisms is an acknowledged prerequisite for high-throughput deposition processing such as roll-to-roll. In this contribution, we advance a new approach for accurate measurement of charge generation yield (CGY) in a series of polymer: non-fullerene OSCs. We show that the state-of-art PM6:Y6 system possess a near unity yield of 98.4%, and this value can be further improved to 99.3% in a Y6 derivative based PM6:BTP-eC9 system. Importantly, we find this apparently modest improvement of 0.9% in CGY can translate to a dramatic impact on photo-generated carrier recombination, leading to a reduced factor of 2.5 relative to the Langevin limit and delivering an unprecedented PCE of >16% (fill factor exceeding 70%) in a 300nm PM6:BTP-eC9 device, which we also probe and understand using drift diffusion simulations. Our work not only reveals the interplay between charge generation, recombination, and device efficiency, but also provides a correlation between basic device physics and practical solar cell engineering. 

This work was supported by the Sêr Cymru II Program through the European Regional Development Fund, Welsh European Funding Office, and Swansea University strategic initiative in Sustainable Advanced Materials. A.A. is a Sêr Cymru II Rising Star Fellow and P.M.is a Sêr Cymru II National Research Chair. S.Z. is the recipient of EPSRC Doctoral Training Partnership studentships. D.B.R. acknowledges the support of the Natural Sciences and Engineering Research Council of Canada (NSERC), [PGSD3-545694-2020]. This work was also funded by UKRI through the EPSRC Program Grant EP/T028511/1 Application Targeted Integrated Photovoltaics (ATIP).

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