@misc{WolffCaprioglioStolterfohtetal.2019, author = {Wolff, Christian Michael and Caprioglio, Pietro and Stolterfoht, Martin and Neher, Dieter}, title = {Nonradiative recombination in perovskite solar cells}, series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, number = {772}, issn = {1866-8372}, doi = {10.25932/publishup-43762}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-437626}, pages = {20}, year = {2019}, abstract = {Perovskite solar cells combine high carrier mobilities with long carrier lifetimes and high radiative efficiencies. Despite this, full devices suffer from significant nonradiative recombination losses, limiting their VOC to values well below the Shockley-Queisser limit. Here, recent advances in understanding nonradiative recombination in perovskite solar cells from picoseconds to steady state are presented, with an emphasis on the interfaces between the perovskite absorber and the charge transport layers. Quantification of the quasi-Fermi level splitting in perovskite films with and without attached transport layers allows to identify the origin of nonradiative recombination, and to explain the VOC of operational devices. These measurements prove that in state-of-the-art solar cells, nonradiative recombination at the interfaces between the perovskite and the transport layers is more important than processes in the bulk or at grain boundaries. Optical pump-probe techniques give complementary access to the interfacial recombination pathways and provide quantitative information on transfer rates and recombination velocities. Promising optimization strategies are also highlighted, in particular in view of the role of energy level alignment and the importance of surface passivation. Recent record perovskite solar cells with low nonradiative losses are presented where interfacial recombination is effectively overcome—paving the way to the thermodynamic efficiency limit.}, language = {en} } @misc{ShoaeeArminStolterfohtetal.2019, author = {Shoaee, Safa and Armin, Ardalan and Stolterfoht, Martin and Hosseini, Seyed Mehrdad and Kurpiers, Jona and Neher, Dieter}, title = {Decoding charge recombination through charge generation in organic solar cells}, series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, number = {773}, issn = {1866-8372}, doi = {10.25932/publishup-43751}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-437512}, pages = {8}, year = {2019}, abstract = {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.}, language = {en} } @misc{CaprioglioStolterfohtWolffetal.2019, author = {Caprioglio, Pietro and Stolterfoht, Martin and Wolff, Christian Michael and Unold, Thomas and Rech, Bernd and Albrecht, Steve and Neher, Dieter}, title = {On the relation between the open-circuit voltage and quasi-Fermi level splitting in efficient perovskite solar cells}, series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, number = {774}, issn = {1866-8372}, doi = {10.25932/publishup-43759}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-437595}, pages = {10}, year = {2019}, abstract = {Today's perovskite solar cells (PSCs) are limited mainly by their open-circuit voltage (VOC) due to nonradiative recombination. Therefore, a comprehensive understanding of the relevant recombination pathways is needed. Here, intensity-dependent measurements of the quasi-Fermi level splitting (QFLS) and of the VOC on the very same devices, including pin-type PSCs with efficiencies above 20\%, are performed. It is found that the QFLS in the perovskite lies significantly below its radiative limit for all intensities but also that the VOC is generally lower than the QFLS, violating one main assumption of the Shockley-Queisser theory. This has far-reaching implications for the applicability of some well-established techniques, which use the VOC as a measure of the carrier densities in the absorber. By performing drift-diffusion simulations, the intensity dependence of the QFLS, the QFLS-VOC offset and the ideality factor are consistently explained by trap-assisted recombination and energetic misalignment at the interfaces. Additionally, it is found that the saturation of the VOC at high intensities is caused by insufficient contact selectivity while heating effects are of minor importance. It is concluded that the analysis of the VOC does not provide reliable conclusions of the recombination pathways and that the knowledge of the QFLS-VOC relation is of great importance.}, language = {en} }