TY - JOUR A1 - Zeiske, Stefan A1 - Sandberg, Oskar J. A1 - Kurpiers, Jona A1 - Shoaee, Safa A1 - Meredith, Paul A1 - Armin, Ardalan T1 - Probing charge generation efficiency in thin-film solar cells by integral-mode transient charge extraction JF - ACS photonics N2 - The photogeneration of free charges in light-harvesting devices is a multistep process, which can be challenging to probe due to the complexity of contributing energetic states and the competitive character of different driving mechanisms. In this contribution, we advance a technique, integral-mode transient charge extraction (ITCE), to probe these processes in thin-film solar cells. ITCE combines capacitance measurements with the integral-mode time-of-flight method in the low intensity regime of sandwich-type thin-film devices and allows for the sensitive determination of photogenerated charge-carrier densities. We verify the theoretical framework of our method by drift-diffusion simulations and demonstrate the applicability of ITCE to organic and perovskite semiconductor-based thin-film solar cells. Furthermore, we examine the field dependence of charge generation efficiency and find our ITCE results to be in excellent agreement with those obtained via time-delayed collection field measurements conducted on the same devices. KW - charge generation KW - thin-film solar cells KW - organic semiconductors; KW - perovskite semiconductors KW - external generation efficiency Y1 - 2022 U6 - https://doi.org/10.1021/acsphotonics.1c01532 SN - 2330-4022 VL - 9 IS - 4 SP - 1188 EP - 1195 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Shoaee, Safa A1 - Armin, Ardalan A1 - Stolterfoht, Martin A1 - Hosseini, Seyed Mehrdad A1 - Kurpiers, Jona A1 - Neher, Dieter T1 - Decoding Charge Recombination through Charge Generation in Organic Solar Cells JF - Solar RRL N2 - The in-depth understanding of charge carrier photogeneration and recombination mechanisms in organic solar cells is still an ongoing effort. In donor:acceptor (bulk) heterojunction organic solar cells, charge photogeneration and recombination are inter-related via the kinetics of charge transfer states-being singlet or triplet states. Although high-charge-photogeneration quantum yields are achieved in many donor:acceptor systems, only very few systems show significantly reduced bimolecular recombination relative to the rate of free carrier encounters, in low-mobility systems. This is a serious limitation for the industrialization of organic solar cells, in particular when aiming at thick active layers. Herein, a meta-analysis of the device performance of numerous bulk heterojunction organic solar cells is presented for which field-dependent photogeneration, charge carrier mobility, and fill factor are determined. Herein, a "spin-related factor" that is dependent on the ratio of back electron transfer of the triplet charge transfer (CT) states to the decay rate of the singlet CT states is introduced. It is shown that this factor links the recombination reduction factor to charge-generation efficiency. As a consequence, it is only in the systems with very efficient charge generation and very fast CT dissociation that free carrier recombination is strongly suppressed, regardless of the spin-related factor. KW - charge generation KW - charge transfers KW - non-Langevin recombination KW - spin-related factors Y1 - 2019 U6 - https://doi.org/10.1002/solr.201900184 SN - 2367-198X VL - 3 IS - 11 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Albrecht, Steve A1 - Vandewal, Koen A1 - Tumbleston, John R. A1 - Fischer, Florian S. U. A1 - Douglas, Jessica D. A1 - Frechet, Jean M. J. A1 - Ludwigs, Sabine A1 - Ade, Harald W. A1 - Salleo, Alberto A1 - Neher, Dieter T1 - On the efficiency of charge transfer state splitting in polymer: Fullerene solar cells JF - Advanced materials KW - organic solar cells KW - charge generation KW - geminate recombination KW - charge transfer states KW - driving force KW - excess energy KW - morphology KW - spectroelectrochemistry Y1 - 2014 U6 - https://doi.org/10.1002/adma.201305283 SN - 0935-9648 SN - 1521-4095 VL - 26 IS - 16 SP - 2533 EP - 2539 PB - Wiley-VCH CY - Weinheim ER -