@article{BrinkmannBeckerZimmermannetal.2022, author = {Brinkmann, Kai Oliver and Becker, Tim and Zimmermann, Florian and Kreusel, Cedric and Gahlmann, Tobias and Theisen, Manuel and Haeger, Tobias and Olthof, Selina and T{\"u}ckmantel, Christian and G{\"u}nster, M. and Maschwitz, Timo and G{\"o}belsmann, Fabian and Koch, Christine and Hertel, Dirk and Caprioglio, Pietro and Pe{\~n}a-Camargo, Francisco and Perdig{\´o}n-Toro, Lorena and Al-Ashouri, Amran and Merten, Lena and Hinderhofer, Alexander and Gomell, Leonie and Zhang, Siyuan and Schreiber, Frank and Albrecht, Steve and Meerholz, Klaus and Neher, Dieter and Stolterfoht, Martin and Riedl, Thomas}, title = {Perovskite-organic tandem solar cells with indium oxide interconnect}, series = {Nature}, volume = {604}, journal = {Nature}, number = {7905}, publisher = {Nature Research}, address = {Berlin}, issn = {0028-0836}, doi = {10.1038/s41586-022-04455-0}, pages = {280 -- 286}, year = {2022}, abstract = {Multijunction solar cells can overcome the fundamental efficiency limits of single-junction devices. The bandgap tunability of metal halide perovskite solar cells renders them attractive for multijunction architectures(1). Combinations with silicon and copper indium gallium selenide (CIGS), as well as all-perovskite tandem cells, have been reported(2-5). Meanwhile, narrow-gap non-fullerene acceptors have unlocked skyrocketing efficiencies for organic solar cells(6,7). Organic and perovskite semiconductors are an attractive combination, sharing similar processing technologies. Currently, perovskite-organic tandems show subpar efficiencies and are limited by the low open-circuit voltage (V-oc) of wide-gap perovskite cells(8) and losses introduced by the interconnect between the subcells(9,10). Here we demonstrate perovskite-organic tandem cells with an efficiency of 24.0 per cent (certified 23.1 per cent) and a high V-oc of 2.15 volts. Optimized charge extraction layers afford perovskite subcells with an outstanding combination of high V-oc and fill factor. The organic subcells provide a high external quantum efficiency in the near-infrared and, in contrast to paradigmatic concerns about limited photostability of non-fullerene cells(11), show an outstanding operational stability if excitons are predominantly generated on the non-fullerene acceptor, which is the case in our tandems. The subcells are connected by an ultrathin (approximately 1.5 nanometres) metal-like indium oxide layer with unprecedented low optical/electrical losses. This work sets a milestone for perovskite-organic tandems, which outperform the best p-i-n perovskite single junctions(12) and are on a par with perovskite-CIGS and all-perovskite multijunctions(13).}, language = {en} } @article{PranavHultzschMusiienkoetal.2023, author = {Pranav, Manasi and Hultzsch, Thomas and Musiienko, Artem and Sun, Bowen and Shukla, Atul and Jaiser, Frank and Shoaee, Safa and Neher, Dieter}, title = {Anticorrelated photoluminescence and free charge generation proves field-assisted exciton dissociation in low-offset PM6:Y5 organic solar cells}, series = {APL materials : high impact open access journal in functional materials science}, volume = {11}, journal = {APL materials : high impact open access journal in functional materials science}, number = {6}, publisher = {AIP Publishing}, address = {Melville}, issn = {2166-532X}, doi = {10.1063/5.0151580}, pages = {8}, year = {2023}, abstract = {Understanding the origin of inefficient photocurrent generation in organic solar cells with low energy offset remains key to realizing high-performance donor-acceptor systems. Here, we probe the origin of field-dependent free-charge generation and photoluminescence in wnon-fullereneacceptor (NFA)-based organic solar cells using the polymer PM6 and the NFA Y5-a non-halogenated sibling to Y6, with a smaller energetic offset to PM6. By performing time-delayed collection field (TDCF) measurements on a variety of samples with different electron transport layers and active layer thickness, we show that the fill factor and photocurrent are limited by field-dependent free charge generation in the bulk of the blend. We also introduce a new method of TDCF called m-TDCF to prove the absence of artifacts from non-geminate recombination of photogenerated and dark charge carriers near the electrodes. We then correlate free charge generation with steady-state photoluminescence intensity and find perfect anticorrelation between these two properties. Through this, we conclude that photocurrent generation in this low-offset system is entirely controlled by the field-dependent dissociation of local excitons into charge-transfer states. (c) 2023 Author(s).}, language = {en} } @article{PerdigonToroLeQuangPhuongElleretal.2022, author = {Perdig{\´o}n-Toro, Lorena and Le Quang Phuong, and Eller, Fabian and Freychet, Guillaume and Saglamkaya, Elifnaz and Khan, Jafar and Wei, Qingya and Zeiske, Stefan and Kroh, Daniel and Wedler, Stefan and Koehler, Anna and Armin, Ardalan and Laquai, Frederic and Herzig, Eva M. and Zou, Yingping and Shoaee, Safa and Neher, Dieter}, title = {Understanding the role of order in Y-series non-fullerene solar cells to realize high open-circuit voltages}, series = {Advanced energy materials}, volume = {12}, journal = {Advanced energy materials}, number = {12}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.202103422}, pages = {13}, year = {2022}, abstract = {Non-fullerene acceptors (NFAs) as used in state-of-the-art organic solar cells feature highly crystalline layers that go along with low energetic disorder. Here, the crucial role of energetic disorder in blends of the donor polymer PM6 with two Y-series NFAs, Y6, and N4 is studied. By performing temperature-dependent charge transport and recombination studies, a consistent picture of the shape of the density of state distributions for free charges in the two blends is developed, allowing an analytical description of the dependence of the open-circuit voltage V-OC on temperature and illumination intensity. Disorder is found to influence the value of the V-OC at room temperature, but also its progression with temperature. Here, the PM6:Y6 blend benefits substantially from its narrower state distributions. The analysis also shows that the energy of the equilibrated free charge population is well below the energy of the NFA singlet excitons for both blends and possibly below the energy of the populated charge transfer manifold, indicating a down-hill driving force for free charge formation. It is concluded that energetic disorder of charge-separated states has to be considered in the analysis of the photovoltaic properties, even for the more ordered PM6:Y6 blend.}, language = {en} } @article{LangKoehnenWarbyetal.2021, author = {Lang, Felix and K{\"o}hnen, Eike and Warby, Jonathan and Xu, Ke and Grischek, Max and Wagner, Philipp and Neher, Dieter and Korte, Lars and Albrecht, Steve and Stolterfoht, Martin}, title = {Revealing fundamental efficiency limits of monolithic perovskite/silicon tandem photovoltaics through subcell characterization}, series = {ACS Energy Letters}, volume = {6}, journal = {ACS Energy Letters}, number = {11}, publisher = {American Chemical Society}, address = {Washington}, issn = {2380-8195}, doi = {10.1021/acsenergylett.1c01783}, pages = {3982 -- 3991}, year = {2021}, abstract = {Perovskite/silicon tandem photovoltaics (PVs) promise to accelerate the decarbonization of our energy systems. Here, we present a thorough subcell diagnosis methodology to reveal deep insights into the practical efficiency limitations of state-of-the-art perovskite/silicon tandem PVs. Our subcell selective intensity-dependent photoluminescence (PL) and injection-dependent electroluminescence (EL) measurements allow independent assessment of pseudo-V-OC and power conversion efficiencies (PCEs) for both subcells. We reveal identical metrics from PL and EL, which implies well-aligned energy levels throughout the entire cell. Relatively large ideality factors and insufficient charge extraction, however, cause each a fill factor penalty of about 6\% (absolute). Using partial device stacks, we then identify significant losses in standard perovskite subcells due to bulk and interfacial recombination. Lastly, we present strategies to minimize these losses using triple halide (CsFAPb(IBrCI)(3)) based perovskites. Our results give helpful feedback for device development and lay the foundation toward advanced perovskite/silicon tandem PVs capable of exceeding 33\% PCE.}, language = {en} } @article{YuanZhangQiuetal.2022, author = {Yuan, Jun and Zhang, Chujun and Qiu, Beibei and Liu, Wei and So, Shu Kong and Mainville, Mathieu and Leclerc, Mario and Shoaee, Safa and Neher, Dieter and Zou, Yingping}, title = {Effects of energetic disorder in bulk heterojunction organic solar cells}, series = {Energy \& environmental science}, volume = {15}, journal = {Energy \& environmental science}, number = {7}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1754-5692}, doi = {10.1039/d2ee00271j}, pages = {2806 -- 2818}, year = {2022}, abstract = {Organic solar cells (OSCs) have progressed rapidly in recent years through the development of novel organic photoactive materials, especially non-fullerene acceptors (NFAs). Consequently, OSCs based on state-of-the-art NFAs have reached significant milestones, such as similar to 19\% power conversion efficiencies (PCEs) and small energy losses (less than 0.5 eV). Despite these significant advances, understanding of the interplay between molecular structure and optoelectronic properties lags significantly behind. For example, despite the theoretical framework for describing the energetic disorder being well developed for the case of inorganic semiconductors, the question of the applicability of classical semiconductor theories in analyzing organic semiconductors is still under debate. A general observation in the inorganic field is that inorganic photovoltaic materials possessing a polycrystalline microstructure exhibit suppressed disorder properties and better charge carrier transport compared to their amorphous analogs. Accordingly, this principle extends to the organic semiconductor field as many organic photovoltaic materials are synthesized to pursue polycrystalline-like features. Yet, there appears to be sporadic examples that exhibit an opposite trend. However, full studies decoupling energetic disorder from aggregation effects have largely been left out. Hence, the potential role of the energetic disorder in OSCs has received little attention. Interestingly, recently reported state-of-the-art NFA-based devices could achieve a small energetic disorder and high PCE at the same time; and interest in this investigation related to the disorder properties in OSCs was revived. In this contribution, progress in terms of the correlation between molecular design and energetic disorder is reviewed together with their effects on the optoelectronic mechanism and photovoltaic performance. Finally, the specific challenges and possible solutions in reducing the energetic disorder of OSCs from the viewpoint of materials and devices are proposed.}, language = {en} } @article{KrohEllerSchoetzetal.2022, author = {Kroh, Daniel and Eller, Fabian and Sch{\"o}tz, Konstantin and Wedler, Stefan and Perdig{\´o}n-Toro, Lorena and Freychet, Guillaume and Wei, Qingya and D{\"o}rr, Maximilian and Jones, David and Zou, Yingping and Herzig, Eva M. and Neher, Dieter and K{\"o}hler, Anna}, title = {Identifying the signatures of intermolecular interactions in blends of PM6 with Y6 and N4 using absorption spectroscopy}, series = {Advanced functional materials}, volume = {32}, journal = {Advanced functional materials}, number = {44}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1616-301X}, doi = {10.1002/adfm.202205711}, pages = {14}, year = {2022}, abstract = {In organic solar cells, the resulting device efficiency depends strongly on the local morphology and intermolecular interactions of the blend film. Optical spectroscopy was used to identify the spectral signatures of interacting chromophores in blend films of the donor polymer PM6 with two state-of-the-art nonfullerene acceptors, Y6 and N4, which differ merely in the branching point of the side chain. From temperature-dependent absorption and luminescence spectroscopy in solution, it is inferred that both acceptor materials form two types of aggregates that differ in their interaction energy. Y6 forms an aggregate with a predominant J-type character in solution, while for N4 molecules the interaction is predominantly in a H-like manner in solution and freshly spin-cast film, yet the molecules reorient with respect to each other with time or thermal annealing to adopt a more J-type interaction. The different aggregation behavior of the acceptor materials is also reflected in the blend films and accounts for the different solar cell efficiencies reported with the two blends.}, language = {en} } @article{FritschKurpiersRolandetal.2022, author = {Fritsch, Tobias and Kurpiers, Jona and Roland, Steffen and Tokmoldin, Nurlan and Shoaee, Safa and Ferron, Thomas and Collins, Brian A. and Janietz, Silvia and Vandewal, Koen and Neher, Dieter}, title = {On the interplay between CT and singlet exciton emission in organic solar cells with small driving force and its impact on voltage loss}, series = {Advanced energy materials}, volume = {12}, journal = {Advanced energy materials}, number = {31}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.202200641}, pages = {11}, year = {2022}, abstract = {The interplay between free charge carriers, charge transfer (CT) states and singlet excitons (S-1) determines the recombination pathway and the resulting open circuit voltage (V-OC) of organic solar cells. By combining a well-aggregated low bandgap polymer with different blend ratios of the fullerenes PCBM and ICBA, the energy of the CT state (E-CT) is varied by 130 meV while leaving the S-1 energy of the polymer (ES1\[{E_{{{\rm{S}}_1}}}\]) unaffected. It is found that the polymer exciton dominates the radiative properties of the blend when ECT\[{E_{{\rm{CT}}}}\] approaches ES1\[{E_{{{\rm{S}}_1}}}\], while the V-OC remains limited by the non-radiative decay of the CT state. It is concluded that an increasing strength of the exciton in the optical spectra of organic solar cells will generally decrease the non-radiative voltage loss because it lowers the radiative V-OC limit (V-OC,V-rad), but not because it is more emissive. The analysis further suggests that electronic coupling between the CT state and the S-1 will not improve the V-OC, but rather reduce the V-OC,V-rad. It is anticipated that only at very low CT state absorption combined with a fairly high CT radiative efficiency the solar cell benefit from the radiative properties of the singlet excitons.}, language = {en} } @article{GrischekCaprioglioZhangetal.2022, author = {Grischek, Max and Caprioglio, Pietro and Zhang, Jiahuan and Pena-Camargo, Francisco and Sveinbjornsson, Kari and Zu, Fengshuo and Menzel, Dorothee and Warby, Jonathan H. and Li, Jinzhao and Koch, Norbert and Unger, Eva and Korte, Lars and Neher, Dieter and Stolterfoht, Martin and Albrecht, Steve}, title = {Efficiency Potential and Voltage Loss of Inorganic CsPbI2Br Perovskite Solar Cells}, series = {Solar RRL}, volume = {6}, journal = {Solar RRL}, number = {11}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202200690}, pages = {12}, year = {2022}, abstract = {Inorganic perovskite solar cells show excellent thermal stability, but the reported power conversion efficiencies are still lower than for organic-inorganic perovskites. This is mainly caused by lower open-circuit voltages (V(OC)s). Herein, the reasons for the low V-OC in inorganic CsPbI2Br perovskite solar cells are investigated. Intensity-dependent photoluminescence measurements for different layer stacks reveal that n-i-p and p-i-n CsPbI2Br solar cells exhibit a strong mismatch between quasi-Fermi level splitting (QFLS) and V-OC. Specifically, the CsPbI2Br p-i-n perovskite solar cell has a QFLS-e center dot V-OC mismatch of 179 meV, compared with 11 meV for a reference cell with an organic-inorganic perovskite of similar bandgap. On the other hand, this study shows that the CsPbI2Br films with a bandgap of 1.9 eV have a very low defect density, resulting in an efficiency potential of 20.3\% with a MeO-2PACz hole-transporting layer and 20.8\% on compact TiO2. Using ultraviolet photoelectron spectroscopy measurements, energy level misalignment is identified as a possible reason for the QFLS-e center dot V-OC mismatch and strategies for overcoming this V-OC limitation are discussed. This work highlights the need to control the interfacial energetics in inorganic perovskite solar cells, but also gives promise for high efficiencies once this issue is resolved.}, language = {en} } @article{PenaCamargoThiesbrummelHempeletal.2022, author = {Pena-Camargo, Francisco and Thiesbrummel, Jarla and Hempel, Hannes and Musiienko, Artem and Le Corre, Vincent M. and Diekmann, Jonas and Warby, Jonathan and Unold, Thomas and Lang, Felix and Neher, Dieter and Stolterfoht, Martin}, title = {Revealing the doping density in perovskite solar cells and its impact on device performance}, series = {Applied physics reviews}, volume = {9}, journal = {Applied physics reviews}, number = {2}, publisher = {AIP Publishing}, address = {Melville}, issn = {1931-9401}, doi = {10.1063/5.0085286}, pages = {11}, year = {2022}, abstract = {Traditional inorganic semiconductors can be electronically doped with high precision. Conversely, there is still conjecture regarding the assessment of the electronic doping density in metal-halide perovskites, not to mention of a control thereof. This paper presents a multifaceted approach to determine the electronic doping density for a range of different lead-halide perovskite systems. Optical and electrical characterization techniques, comprising intensity-dependent and transient photoluminescence, AC Hall effect, transfer-length-methods, and charge extraction measurements were instrumental in quantifying an upper limit for the doping density. The obtained values are subsequently compared to the electrode charge per cell volume under short-circuit conditions ( CUbi/eV), which amounts to roughly 10(16) cm(-3). This figure of merit represents the critical limit below which doping-induced charges do not influence the device performance. The experimental results consistently demonstrate that the doping density is below this critical threshold 10(12) cm(-3), which means << CUbi / e V) for all common lead-based metal-halide perovskites. Nevertheless, although the density of doping-induced charges is too low to redistribute the built-in voltage in the perovskite active layer, mobile ions are present in sufficient quantities to create space-charge-regions in the active layer, reminiscent of doped pn-junctions. These results are well supported by drift-diffusion simulations, which confirm that the device performance is not affected by such low doping densities.}, language = {en} } @article{RaoufiHoermannLigorioetal.2020, author = {Raoufi, Meysam and H{\"o}rmann, Ulrich and Ligorio, Giovanni and Hildebrandt, Jana and P{\"a}tzel, Michael and Schultz, Thorsten and Perdig{\´o}n-Toro, Lorena and Koch, Norbert and List-Kratochvil, Emil and Hecht, Stefan and Neher, Dieter}, title = {Simultaneous effect of ultraviolet radiation and surface modification on the work function and hole injection properties of ZnO thin films}, series = {Physica Status Solidi. A , Applications and materials science}, volume = {217}, journal = {Physica Status Solidi. A , Applications and materials science}, number = {5}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1862-6300}, doi = {10.1002/pssa.201900876}, pages = {1 -- 6}, year = {2020}, abstract = {The combined effect of ultraviolet (UV) light soaking and self-assembled monolayer deposition on the work function (WF) of thin ZnO layers and on the efficiency of hole injection into the prototypical conjugated polymer poly(3-hexylthiophen-2,5-diyl) (P3HT) is systematically investigated. It is shown that the WF and injection efficiency depend strongly on the history of UV light exposure. Proper treatment of the ZnO layer enables ohmic hole injection into P3HT, demonstrating ZnO as a potential anode material for organic optoelectronic devices. The results also suggest that valid conclusions on the energy-level alignment at the ZnO/organic interfaces may only be drawn if the illumination history is precisely known and controlled. This is inherently problematic when comparing electronic data from ultraviolet photoelectron spectroscopy (UPS) measurements carried out under different or ill-defined illumination conditions.}, language = {en} }