TY - GEN A1 - Stolterfoht, Martin A1 - Grischek, Max A1 - Caprioglio, Pietro A1 - Wolff, Christian Michael A1 - Gutierrez-Partida, Emilio A1 - Peña-Camargo, Francisco A1 - Rothhardt, Daniel A1 - Zhang, Shanshan A1 - Raoufi, Meysam A1 - Wolansky, Jakob A1 - Abdi-Jalebi, Mojtaba A1 - Stranks, Samuel D. A1 - Albrecht, Steve A1 - Kirchartz, Thomas A1 - Neher, Dieter T1 - How to quantify the efficiency potential of neat perovskite films BT - Perovskite semiconductors with an implied efficiency exceeding 28% T2 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - Perovskite photovoltaic (PV) cells have demonstrated power conversion efficiencies (PCE) that are close to those of monocrystalline silicon cells; however, in contrast to silicon PV, perovskites are not limited by Auger recombination under 1-sun illumination. Nevertheless, compared to GaAs and monocrystalline silicon PV, perovskite cells have significantly lower fill factors due to a combination of resistive and non-radiative recombination losses. This necessitates a deeper understanding of the underlying loss mechanisms and in particular the ideality factor of the cell. By measuring the intensity dependence of the external open-circuit voltage and the internal quasi-Fermi level splitting (QFLS), the transport resistance-free efficiency of the complete cell as well as the efficiency potential of any neat perovskite film with or without attached transport layers are quantified. Moreover, intensity-dependent QFLS measurements on different perovskite compositions allows for disentangling of the impact of the interfaces and the perovskite surface on the non-radiative fill factor and open-circuit voltage loss. It is found that potassium-passivated triple cation perovskite films stand out by their exceptionally high implied PCEs > 28%, which could be achieved with ideal transport layers. Finally, strategies are presented to reduce both the ideality factor and transport losses to push the efficiency to the thermodynamic limit. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1434 KW - non-radiative interface recombination KW - perovskite solar cells KW - photoluminescence Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-516622 SN - 1866-8372 IS - 17 ER - TY - GEN A1 - Schulze, Patricia S. C. A1 - Bett, Alexander J. A1 - Bivour, Martin A1 - Caprioglio, Pietro A1 - Gerspacher, Fabian M. A1 - Kabaklı, Özde Ş. A1 - Richter, Armin A1 - Stolterfoht, Martin A1 - Zhang, Qinxin A1 - Neher, Dieter A1 - Hermle, Martin A1 - Hillebrecht, Harald A1 - Glunz, Stefan W. A1 - Goldschmidt, Jan Christoph T1 - 25.1% high-efficiency monolithic perovskite silicon tandem solar cell with a high bandgap perovskite absorber T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - Monolithic perovskite silicon tandem solar cells can overcome the theoretical efficiency limit of silicon solar cells. This requires an optimum bandgap, high quantum efficiency, and high stability of the perovskite. Herein, a silicon heterojunction bottom cell is combined with a perovskite top cell, with an optimum bandgap of 1.68 eV in planar p-i-n tandem configuration. A methylammonium-free FA(0.75)Cs(0.25)Pb(I0.8Br0.2)(3) perovskite with high Cs content is investigated for improved stability. A 10% molarity increase to 1.1 m of the perovskite precursor solution results in approximate to 75 nm thicker absorber layers and 0.7 mA cm(-2) higher short-circuit current density. With the optimized absorber, tandem devices reach a high fill factor of 80% and up to 25.1% certified efficiency. The unencapsulated tandem device shows an efficiency improvement of 2.3% (absolute) over 5 months, showing the robustness of the absorber against degradation. Moreover, a photoluminescence quantum yield analysis reveals that with adapted charge transport materials and surface passivation, along with improved antireflection measures, the high bandgap perovskite absorber has the potential for 30% tandem efficiency in the near future. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1197 KW - heterojunction silicon solar cells KW - interfaces KW - perovskite solar cells KW - tandem solar cells KW - thin films Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-525668 SN - 1866-8372 IS - 7 ER - TY - GEN A1 - Wolff, Christian Michael A1 - Caprioglio, Pietro A1 - Stolterfoht, Martin A1 - Neher, Dieter T1 - Nonradiative recombination in perovskite solar cells BT - the role of interfaces T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - 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. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 772 KW - interfacial recombination KW - open‐circuit voltage KW - perovskite solar cells KW - photoluminescence Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437626 SN - 1866-8372 IS - 772 ER - TY - GEN A1 - Caprioglio, Pietro A1 - Stolterfoht, Martin A1 - Wolff, Christian Michael A1 - Unold, Thomas A1 - Rech, Bernd A1 - Albrecht, Steve A1 - Neher, Dieter T1 - On the relation between the open‐circuit voltage and quasi‐Fermi level splitting in efficient perovskite solar cells T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - 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. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 774 KW - electro‐optical materials KW - perovskite solar cells KW - photovoltaic devices KW - thin films Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437595 SN - 1866-8372 IS - 774 ER -