@article{ZuSchultzWolffetal.2020, author = {Zu, Fengshuo and Schultz, Thorsten and Wolff, Christian Michael and Shin, Dongguen and Frohloff, Lennart and Neher, Dieter and Amsalem, Patrick and Koch, Norbert}, title = {Position-locking of volatile reaction products by atmosphere and capping layers slows down photodecomposition of methylammonium lead triiodide perovskite}, series = {RSC Advances}, volume = {10}, journal = {RSC Advances}, number = {30}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2046-2069}, doi = {10.1039/d0ra03572f}, pages = {17534 -- 17542}, year = {2020}, abstract = {The remarkable progress of metal halide perovskites in photovoltaics has led to the power conversion efficiency approaching 26\%. However, practical applications of perovskite-based solar cells are challenged by the stability issues, of which the most critical one is photo-induced degradation. Bare CH3NH3PbI3 perovskite films are known to decompose rapidly, with methylammonium and iodine as volatile species and residual solid PbI2 and metallic Pb, under vacuum under white light illumination, on the timescale of minutes. We find, in agreement with previous work, that the degradation is non-uniform and proceeds predominantly from the surface, and that illumination under N-2 and ambient air (relative humidity 20\%) does not induce substantial degradation even after several hours. Yet, in all cases the release of iodine from the perovskite surface is directly identified by X-ray photoelectron spectroscopy. This goes in hand with a loss of organic cations and the formation of metallic Pb. When CH3NH3PbI3 films are covered with a few nm thick organic capping layer, either charge selective or non-selective, the rapid photodecomposition process under ultrahigh vacuum is reduced by more than one order of magnitude, and becomes similar in timescale to that under N-2 or air. We conclude that the light-induced decomposition reaction of CH3NH3PbI3, leading to volatile methylammonium and iodine, is largely reversible as long as these products are restrained from leaving the surface. This is readily achieved by ambient atmospheric pressure, as well as a thin organic capping layer even under ultrahigh vacuum. In addition to explaining the impact of gas pressure on the stability of this perovskite, our results indicate that covalently "locking" the position of perovskite components at the surface or an interface should enhance the overall photostability.}, language = {en} } @article{WangSmithSkroblinetal.2020, author = {Wang, Qiong and Smith, Joel A. and Skroblin, Dieter and Steele, Julian A. and Wolff, Christian Michael and Caprioglio, Pietro and Stolterfoht, Martin and K{\"o}bler, Hans and Turren-Cruz, Silver-Hamill and Li, Meng and Gollwitzer, Christian and Neher, Dieter and Abate, Antonio}, title = {Managing phase purities and crystal orientation for high-performance and photostable cesium lead halide perovskite solar cells}, series = {Solar RRL}, volume = {4}, journal = {Solar RRL}, number = {9}, publisher = {WILEY-VCH}, address = {Weinheim}, pages = {9}, year = {2020}, abstract = {Inorganic perovskites with cesium (Cs+) as the cation have great potential as photovoltaic materials if their phase purity and stability can be addressed. Herein, a series of inorganic perovskites is studied, and it is found that the power conversion efficiency of solar cells with compositions CsPbI1.8Br1.2, CsPbI2.0Br1.0, and CsPbI2.2Br0.8 exhibits a high dependence on the initial annealing step that is found to significantly affect the crystallization and texture behavior of the final perovskite film. At its optimized annealing temperature, CsPbI1.8Br1.2 exhibits a pure orthorhombic phase and only one crystal orientation of the (110) plane. Consequently, this allows for the best efficiency of up to 14.6\% and the longest operational lifetime, T-S80, of approximate to 300 h, averaged of over six solar cells, during the maximum power point tracking measurement under continuous light illumination and nitrogen atmosphere. This work provides essential progress on the enhancement of photovoltaic performance and stability of CsPbI3 - xBrx perovskite solar cells.}, language = {en} } @article{TokmoldinHosseiniRaoufietal.2020, author = {Tokmoldin, Nurlan and Hosseini, Seyed Mehrdad and Raoufi, Meysam and Phuong, Le Quang and Sandberg, Oskar J. and Guan, Huilan and Zou, Yingping and Neher, Dieter and Shoaee, Safa}, title = {Extraordinarily long diffusion length in PM6:Y6 organic solar cells}, series = {Journal of materials chemistry : A, materials for energy and sustainability}, volume = {8}, journal = {Journal of materials chemistry : A, materials for energy and sustainability}, number = {16}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2050-7488}, doi = {10.1039/d0ta03016c}, pages = {7854 -- 7860}, year = {2020}, abstract = {The PM6:Y6 bulk-heterojunction (BHJ) blend system achieves high short-circuit current (J(SC)) values in thick photovoltaic junctions. Here we analyse these solar cells to understand the observed independence of the short-circuit current upon photoactive layer thickness. We employ a range of optoelectronic measurements and analyses, including Mott-Schottky analysis, CELIV, photoinduced absorption spectroscopy, mobility measurements and simulations, to conclude that, the invariant photocurrent for the devices with different active layer thicknesses is associated with the Y6's diffusion length exceeding 300 nm in case of a 300 nm thick cell. This is despite unintentional doping that occurs in PM6 and the associated space-charge effect, which is expected to be even more profound upon photogeneration. This extraordinarily long diffusion length - which is an order of magnitude larger than typical values for organics - dominates transport in the flat-band region of thick junctions. Our work suggests that the performance of the doped PM6:Y6 organic solar cells resembles that of inorganic devices with diffusion transport playing a pivotal role. Ultimately, this is expected to be a key requirement for the fabrication of efficient, high-photocurrent, thick organic solar cells.}, language = {en} } @article{StolterfohtGrischekCaprioglioetal.2020, author = {Stolterfoht, Martin and Grischek, Max and Caprioglio, Pietro and Wolff, Christian Michael and Gutierrez-Partida, Emilio and Pe{\~n}a-Camargo, Francisco and Rothhardt, Daniel and Zhang, Shanshan and Raoufi, Meysam and Wolansky, Jakob and Abdi-Jalebi, Mojtaba and Stranks, Samuel D. and Albrecht, Steve and Kirchartz, Thomas and Neher, Dieter}, title = {How to quantify the efficiency potential of neat perovskite films}, series = {Advanced Materials}, volume = {32}, journal = {Advanced Materials}, number = {17}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {0935-9648}, doi = {10.1002/adma.202000080}, pages = {1 -- 10}, year = {2020}, abstract = {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.}, language = {en} } @article{SchulzeBettBivouretal.2020, author = {Schulze, Patricia S. C. and Bett, Alexander J. and Bivour, Martin and Caprioglio, Pietro and Gerspacher, Fabian M. and Kabakl{\i}, {\"O}zde Ş. and Richter, Armin and Stolterfoht, Martin and Zhang, Qinxin and Neher, Dieter and Hermle, Martin and Hillebrecht, Harald and Glunz, Stefan W. and Goldschmidt, Jan Christoph}, title = {25.1\% high-efficiency monolithic perovskite silicon tandem solar cell with a high bandgap perovskite absorber}, series = {Solar RRL}, volume = {4}, journal = {Solar RRL}, number = {7}, publisher = {John Wiley \& Sons, Inc.}, address = {New Jersey}, pages = {10}, year = {2020}, abstract = {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.}, language = {en} } @article{SandbergKurpiersStolterfohtetal.2020, author = {Sandberg, Oskar J. and Kurpiers, Jona and Stolterfoht, Martin and Neher, Dieter and Meredith, Paul and Shoaee, Safa and Armin, Ardalan}, title = {On the question of the need for a built-in potential in Perovskite solar cells}, series = {Advanced materials interfaces}, volume = {7}, journal = {Advanced materials interfaces}, number = {10}, publisher = {Wiley}, address = {Hoboken}, issn = {2196-7350}, doi = {10.1002/admi.202000041}, pages = {8}, year = {2020}, abstract = {Perovskite semiconductors as the active materials in efficient solar cells exhibit free carrier diffusion lengths on the order of microns at low illumination fluxes and many hundreds of nanometers under 1 sun conditions. These lengthscales are significantly larger than typical junction thicknesses, and thus the carrier transport and charge collection should be expected to be diffusion controlled. A consensus along these lines is emerging in the field. However, the question as to whether the built-in potential plays any role is still of matter of some conjecture. This important question using phase-sensitive photocurrent measurements and theoretical device simulations based upon the drift-diffusion framework is addressed. In particular, the role of the built-in electric field and charge-selective transport layers in state-of-the-art p-i-n perovskite solar cells comparing experimental findings and simulation predictions is probed. It is found that while charge collection in the junction does not require a drift field per se, a built-in potential is still needed to avoid the formation of reverse electric fields inside the active layer, and to ensure efficient extraction through the charge transport layers.}, language = {en} } @article{SamsonRechPerdigonToroetal.2020, author = {Samson, Stephanie and Rech, Jeromy and Perdigon-Toro, Lorena and Peng, Zhengxing and Shoaee, Safa and Ade, Harald and Neher, Dieter and Stolterfoht, Martin and You, Wei}, title = {Organic solar cells with large insensitivity to donor polymer molar mass across all acceptor classes}, series = {ACS applied polymer materials}, volume = {2}, journal = {ACS applied polymer materials}, number = {11}, publisher = {American Chemical Society}, address = {Washington}, issn = {2637-6105}, doi = {10.1021/acsapm.0c01041}, pages = {5300 -- 5308}, year = {2020}, abstract = {Donor polymer number-average molar mass (M-n) has long been known to influence organic photovoltaic (OPV) performance via changes in both the polymer properties and the resulting bulk heterojunction morphology. The exact nature of these M-n effects varies from system to system, although there is generally some intermediate M-n that results in optimal performance. Interestingly, our earlier work with the difluorobenzotriazole (FTAZ)-based donor polymer, paired with either N2200 (polymer acceptor) or PC61BM (fullerene acceptor), PcBm demonstrated <10\% variation in power conversion efficiency and a consistent morphology over a large span of M-n (30 kg/mol to over 100 kg/mol). Would such insensitivity to polymer M-n still hold true when prevailing small molecular acceptors were used with FTAZ? To answer this question, we explored the impact of FTAZ on OPVs with ITIC, a high-performance small-molecule fused-ring electron acceptor (FREA). By probing the photovoltaic characteristics of the resulting OPVs, we show that a similar FTAZ mn insensitivity is also found in the FTAZ:ITIC system. This study highlights a single-donor polymer which, when paired with an archetypal fullerene, polymer, and FREA, results in systems that are largely insensitive to donor M. Our results may have implications in polymer batch-to-batch reproducibility, in particular, relaxing the need for tight M-n control during synthesis.}, 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 Perdigon-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} } @article{PhuongHosseiniSandbergetal.2020, author = {Phuong, Le Quang and Hosseini, Seyed Mehrdad and Sandberg, Oskar J. and Zou, Yingping and Woo, Han Young and Neher, Dieter and Shoaee, Safa}, title = {Quantifying quasi-fermi level splitting and open-circuit voltage losses in highly efficient nonfullerene organic solar cells}, series = {Solar RRL}, volume = {5}, journal = {Solar RRL}, number = {1}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202000649}, pages = {6}, year = {2020}, abstract = {The power conversion efficiency (PCE) of state-of-the-art organic solar cells is still limited by significant open-circuit voltage (V-OC) losses, partly due to the excitonic nature of organic materials and partly due to ill-designed architectures. Thus, quantifying different contributions of the V-OC losses is of importance to enable further improvements in the performance of organic solar cells. Herein, the spectroscopic and semiconductor device physics approaches are combined to identify and quantify losses from surface recombination and bulk recombination. Several state-of-the-art systems that demonstrate different V-OC losses in their performance are presented. By evaluating the quasi-Fermi level splitting (QFLS) and the V-OC as a function of the excitation fluence in nonfullerene-based PM6:Y6, PM6:Y11, and fullerene-based PPDT2FBT:PCBM devices with different architectures, the voltage losses due to different recombination processes occurring in the active layers, the transport layers, and at the interfaces are assessed. It is found that surface recombination at interfaces in the studied solar cells is negligible, and thus, suppressing the non-radiative recombination in the active layers is the key factor to enhance the PCE of these devices. This study provides a universal tool to explain and further improve the performance of recently demonstrated high-open-circuit-voltage organic solar cells.}, language = {en} } @article{PerdigonToroZhangMarkinaetal.2020, author = {Perdigon-Toro, Lorena and Zhang, Huotian and Markina, Anastaa si and Yuan, Jun and Hosseini, Seyed Mehrdad and Wolff, Christian Michael and Zuo, Guangzheng and Stolterfoht, Martin and Zou, Yingping and Gao, Feng and Andrienko, Denis and Shoaee, Safa and Neher, Dieter}, title = {Barrierless free charge generation in the high-performance PM6:Y6 bulk heterojunction non-fullerene solar cell}, series = {Advanced materials}, volume = {32}, journal = {Advanced materials}, number = {9}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {0935-9648}, doi = {10.1002/adma.201906763}, pages = {9}, year = {2020}, abstract = {Organic solar cells are currently experiencing a second golden age thanks to the development of novel non-fullerene acceptors (NFAs). Surprisingly, some of these blends exhibit high efficiencies despite a low energy offset at the heterojunction. Herein, free charge generation in the high-performance blend of the donor polymer PM6 with the NFA Y6 is thoroughly investigated as a function of internal field, temperature and excitation energy. Results show that photocurrent generation is essentially barrierless with near-unity efficiency, regardless of excitation energy. Efficient charge separation is maintained over a wide temperature range, down to 100 K, despite the small driving force for charge generation. Studies on a blend with a low concentration of the NFA, measurements of the energetic disorder, and theoretical modeling suggest that CT state dissociation is assisted by the electrostatic interfacial field which for Y6 is large enough to compensate the Coulomb dissociation barrier.}, language = {en} }