TY - JOUR A1 - Al-Sa'di, Mahmoud A1 - Jaiser, Frank A1 - Bagnich, Sergey A. A1 - Unger, Thomas A1 - Blakesley, James C. A1 - Wilke, Andreas A1 - Neher, Dieter T1 - Electrical and optical simulations of a polymer-based phosphorescent organic light-emitting diode with high efficiency JF - Journal of polymer science : B, Polymer physics N2 - A comprehensive numerical device simulation of the electrical and optical characteristics accompanied with experimental measurements of a new highly efficient system for polymer-based light-emitting diodes doped with phosphorescent dyes is presented. The system under investigation comprises an electron transporter attached to a polymer backbone blended with an electronically inert small molecule and an iridium-based green phosphorescent dye which serves as both emitter and hole transporter. The device simulation combines an electrical and an optical model. Based on the known highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels of all components as well as the measured electrical and optical characteristics of the devices, we model the emissive layer as an effective medium using the dye's HOMO as hole transport level and the polymer LUMO as electron transport level. By fine-tuning the injection barriers at the electron and hole-injecting contact, respectively, in simulated devices, unipolar device characteristics were fitted to the experimental data. Simulations using the so-obtained set of parameters yielded very good agreement to the measured currentvoltage, luminancevoltage characteristics, and the emission profile of entire bipolar light-emitting diodes, without additional fitting parameters. The simulation was used to gain insight into the physical processes and the mechanisms governing the efficiency of the organic light-emitting diode, including the position and extent of the recombination zone, carrier concentration profiles, and field distribution inside the device. The simulations show that the device is severely limited by hole injection, and that a reduction of the hole-injection barrier would improve the device efficiency by almost 50%. KW - conjugated polymers KW - high performance polymers KW - organic electronics KW - organic light-emitting diode KW - simulations KW - TCAD Y1 - 2012 U6 - https://doi.org/10.1002/polb.23158 SN - 0887-6266 VL - 50 IS - 22 SP - 1567 EP - 1576 PB - Wiley-Blackwell CY - Hoboken ER - TY - JOUR A1 - Pranav, Manasi A1 - Hultzsch, Thomas A1 - Musiienko, Artem A1 - Sun, Bowen A1 - Shukla, Atul A1 - Jaiser, Frank A1 - Shoaee, Safa A1 - Neher, Dieter T1 - Anticorrelated photoluminescence and free charge generation proves field-assisted exciton dissociation in low-offset PM6:Y5 organic solar cells JF - APL materials : high impact open access journal in functional materials science N2 - 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). Y1 - 2023 U6 - https://doi.org/10.1063/5.0151580 SN - 2166-532X VL - 11 IS - 6 PB - AIP Publishing CY - Melville ER - 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 - JOUR A1 - Brinkmann, Kai Oliver A1 - Becker, Tim A1 - Zimmermann, Florian A1 - Kreusel, Cedric A1 - Gahlmann, Tobias A1 - Theisen, Manuel A1 - Haeger, Tobias A1 - Olthof, Selina A1 - Tückmantel, Christian A1 - Günster, M. A1 - Maschwitz, Timo A1 - Göbelsmann, Fabian A1 - Koch, Christine A1 - Hertel, Dirk A1 - Caprioglio, Pietro A1 - Peña-Camargo, Francisco A1 - Perdigón-Toro, Lorena A1 - Al-Ashouri, Amran A1 - Merten, Lena A1 - Hinderhofer, Alexander A1 - Gomell, Leonie A1 - Zhang, Siyuan A1 - Schreiber, Frank A1 - Albrecht, Steve A1 - Meerholz, Klaus A1 - Neher, Dieter A1 - Stolterfoht, Martin A1 - Riedl, Thomas T1 - Perovskite-organic tandem solar cells with indium oxide interconnect JF - Nature N2 - 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). Y1 - 2022 U6 - https://doi.org/10.1038/s41586-022-04455-0 SN - 0028-0836 SN - 1476-4687 VL - 604 IS - 7905 SP - 280 EP - 286 PB - Nature Research CY - Berlin ER - TY - GEN A1 - Ye, Fangyuan A1 - Zhang, Shuo A1 - Warby, Jonathan A1 - Wu, Jiawei A1 - Gutierrez-Partida, Emilio A1 - Lang, Felix A1 - Shah, Sahil A1 - Saglamkaya, Elifnaz A1 - Sun, Bowen A1 - Zu, Fengshuo A1 - Shoaee, Safa A1 - Wang, Haifeng A1 - Stiller, Burkhard A1 - Neher, Dieter A1 - Zhu, Wei-Hong A1 - Stolterfoht, Martin A1 - Wu, Yongzhen T1 - Overcoming C₆₀-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane T2 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - Inverted perovskite solar cells still suffer from significant non-radiative recombination losses at the perovskite surface and across the perovskite/C₆₀ interface, limiting the future development of perovskite-based single- and multi-junction photovoltaics. Therefore, more effective inter- or transport layers are urgently required. To tackle these recombination losses, we introduce ortho-carborane as an interlayer material that has a spherical molecular structure and a three-dimensional aromaticity. Based on a variety of experimental techniques, we show that ortho-carborane decorated with phenylamino groups effectively passivates the perovskite surface and essentially eliminates the non-radiative recombination loss across the perovskite/C₆₀ interface with high thermal stability. We further demonstrate the potential of carborane as an electron transport material, facilitating electron extraction while blocking holes from the interface. The resulting inverted perovskite solar cells deliver a power conversion efficiency of over 23% with a low non-radiative voltage loss of 110 mV, and retain >97% of the initial efficiency after 400 h of maximum power point tracking. Overall, the designed carborane based interlayer simultaneously enables passivation, electron-transport and hole-blocking and paves the way toward more efficient and stable perovskite solar cells. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1317 Y1 - 2022 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-587705 SN - 1866-8372 IS - 1317 ER - TY - JOUR A1 - Pena-Camargo, Francisco A1 - Thiesbrummel, Jarla A1 - Hempel, Hannes A1 - Musiienko, Artem A1 - Le Corre, Vincent M. A1 - Diekmann, Jonas A1 - Warby, Jonathan A1 - Unold, Thomas A1 - Lang, Felix A1 - Neher, Dieter A1 - Stolterfoht, Martin T1 - Revealing the doping density in perovskite solar cells and its impact on device performance JF - Applied physics reviews N2 - 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. Y1 - 2022 U6 - https://doi.org/10.1063/5.0085286 SN - 1931-9401 VL - 9 IS - 2 PB - AIP Publishing CY - Melville ER - TY - JOUR 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% JF - Advanced Materials 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. KW - non-radiative interface recombination KW - perovskite solar cells KW - photoluminescence Y1 - 2020 U6 - https://doi.org/10.1002/adma.202000080 SN - 0935-9648 SN - 1521-4095 VL - 32 IS - 17 SP - 1 EP - 10 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Le Corre, Vincent M. A1 - Diekmann, Jonas A1 - Peña-Camargo, Francisco A1 - Thiesbrummel, Jarla A1 - Tokmoldin, Nurlan A1 - Gutierrez-Partida, Emilio A1 - Peters, Karol Pawel A1 - Perdigón-Toro, Lorena A1 - Futscher, Moritz H. A1 - Lang, Felix A1 - Warby, Jonathan A1 - Snaith, Henry J. A1 - Neher, Dieter A1 - Stolterfoht, Martin T1 - Quantification of efficiency losses due to mobile ions in Perovskite solar cells via fast hysteresis measurements JF - Solar RRL N2 - Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady-state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via "fast-hysteresis" measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (approximate to 1000 V s(-1)). The "ion-free" PCE is between 1% and 3% higher than the steady-state PCE, demonstrating the importance of ion-induced losses, even in cells with low levels of hysteresis at typical scan speeds (approximate to 100mv s(-1)). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the peak hysteresis position. The fast-hysteresis measurements are corroborated by transient charge extraction and capacitance measurements and numerical simulations, which confirm the experimental findings and provide important insights into the charge carrier dynamics. The proposed method to quantify PCE losses due to field screening induced by mobile ions clarifies several important experimental observations and opens up a large range of future experiments. KW - hysteresis KW - mobile ions KW - perovskite solar cells Y1 - 2021 U6 - https://doi.org/10.1002/solr.202100772 SN - 2367-198X VL - 6 IS - 4 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Grischek, Max A1 - Caprioglio, Pietro A1 - Zhang, Jiahuan A1 - Pena-Camargo, Francisco A1 - Sveinbjornsson, Kari A1 - Zu, Fengshuo A1 - Menzel, Dorothee A1 - Warby, Jonathan A1 - Li, Jinzhao A1 - Koch, Norbert A1 - Unger, Eva A1 - Korte, Lars A1 - Neher, Dieter A1 - Stolterfoht, Martin A1 - Albrecht, Steve T1 - Efficiency Potential and Voltage Loss of Inorganic CsPbI2Br Perovskite Solar Cells JF - Solar RRL N2 - 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. KW - CsPbI2Br KW - efficiency potentials KW - inorganic perovskites KW - photoluminescence KW - solar cells KW - voltage losses Y1 - 2022 U6 - https://doi.org/10.1002/solr.202200690 SN - 2367-198X VL - 6 IS - 11 PB - Wiley-VCH CY - Weinheim ER - TY - GEN A1 - Wang, Qiong A1 - Smith, Joel A. A1 - Skroblin, Dieter A1 - Steele, Julian A. A1 - Wolff, Christian Michael A1 - Caprioglio, Pietro A1 - Stolterfoht, Martin A1 - Köbler, Hans A1 - Turren-Cruz, Silver-Hamill A1 - Li, Meng A1 - Gollwitzer, Christian A1 - Neher, Dieter A1 - Abate, Antonio T1 - Managing phase purities and crystal orientation for high-performance and photostable cesium lead halide perovskite solar cells T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - 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. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1210 KW - cesium lead halides KW - crystal orientation KW - inorganic perovskites KW - ISOS-L-1I protocol KW - phase purity KW - photostability Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-525374 SN - 1866-8372 IS - 9 ER - TY - GEN 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 T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe 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. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 773 KW - charge generation KW - charge transfers KW - non-Langevin recombination KW - spin-related factors Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437512 SN - 1866-8372 IS - 773 ER - TY - JOUR A1 - Perdigón-Toro, Lorena A1 - Le Quang Phuong, A1 - Eller, Fabian A1 - Freychet, Guillaume A1 - Saglamkaya, Elifnaz A1 - Khan, Jafar A1 - Wei, Qingya A1 - Zeiske, Stefan A1 - Kroh, Daniel A1 - Wedler, Stefan A1 - Koehler, Anna A1 - Armin, Ardalan A1 - Laquai, Frederic A1 - Herzig, Eva M. A1 - Zou, Yingping A1 - Shoaee, Safa A1 - Neher, Dieter T1 - Understanding the role of order in Y-series non-fullerene solar cells to realize high open-circuit voltages JF - Advanced energy materials N2 - 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. KW - energetic disorder KW - non-fullerene acceptors KW - open-circuit voltage KW - organic solar cells Y1 - 2022 U6 - https://doi.org/10.1002/aenm.202103422 SN - 1614-6832 SN - 1614-6840 VL - 12 IS - 12 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Perdigón-Toro, Lorena A1 - Le Quang Phuong, A1 - Zeiske, Stefan A1 - Vandewal, Koen A1 - Armin, Ardalan A1 - Shoaee, Safa A1 - Neher, Dieter T1 - Excitons dominate the emission from PM6 BT - Y6 solar cells, but this does not help the open-circuit voltage of the device JF - ACS energy letters / American Chemical Society N2 - Non-fullerene acceptors (NFAs) are far more emissive than their fullerene-based counterparts. Here, we study the spectral properties of photocurrent generation and recombination of the blend of the donor polymer PM6 with the NFA Y6. We find that the radiative recombination of free charges is almost entirely due to the re-occupation and decay of Y6 singlet excitons, but that this pathway contributes less than 1% to the total recombination. As such, the open-circuit voltage of the PM6:Y6 blend is determined by the energetics and kinetics of the charge-transfer (CT) state. Moreover, we find that no information on the energetics of the CT state manifold can be gained from the low-energy tail of the photovoltaic external quantum efficiency spectrum, which is dominated by the excitation spectrum of the Y6 exciton. We, finally, estimate the charge-separated state to lie only 120 meV below the Y6 singlet exciton energy, meaning that this blend indeed represents a high-efficiency system with a low energetic offset. Y1 - 2021 U6 - https://doi.org/10.1021/acsenergylett.0c02572 SN - 2380-8195 VL - 6 IS - 2 SP - 557 EP - 564 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Scharsich, Christina A1 - Lohwasser, Ruth H. A1 - Sommer, Michael A1 - Asawapirom, Udom A1 - Scherf, Ullrich A1 - Thelakkat, Mukundan A1 - Neher, Dieter A1 - Koehler, Anna T1 - Control of aggregate formation in poly(3-hexylthiophene) by solvent, molecular weight, and synthetic method JF - Journal of polymer science : B, Polymer physics N2 - Aggregate formation in poly(3-hexylthiophene) depends on molecular weight, solvent, and synthetic method. The interplay of these parameters thus largely controls device performance. In order to obtain a quantitative understanding on how these factors control the resulting electronic properties of P3HT, we measured absorption in solution and in thin films as well as the resulting field effect mobility in transistors. By a detailed analysis of the absorption spectra, we deduce the fraction of aggregates formed, the excitonic coupling within the aggregates, and the conjugation length within the aggregates, all as a function of solvent quality for molecular weights from 5 to 19 kDa. From this, we infer in which structure the aggregated chains pack. Although the 5 kDa samples form straight chains, the 11 and 19 kDa chains are kinked or folded, with conjugation lengths that increase as the solvent quality reduces. There is a maximum fraction of aggregated chains (about 55 +/- 5%) that can be obtained, even for poor solvent quality. We show that inducing aggregation in solution leads to control of aggregate properties in thin films. As expected, the field-effect mobility correlates with the propensity to aggregation. Correspondingly, we find that a well-defined synthetic approach, tailored to give a narrow molecular weight distribution, is needed to obtain high field effect mobilities of up to 0.01 cm2/Vs for low molecular weight samples (=11 kDa), while the influence of synthetic method is negligible for samples of higher molecular weight, if low molecular weight fractions are removed by extraction. KW - conformational analysis KW - conjugated polymers KW - crystallization KW - films KW - interaction parameter KW - molecular weight distribution KW - molar mass distribution KW - nucleation KW - photophysics KW - structure KW - UV-vis spectroscopy Y1 - 2012 U6 - https://doi.org/10.1002/polb.23022 SN - 0887-6266 VL - 50 IS - 6 SP - 442 EP - 453 PB - Wiley-Blackwell CY - Hoboken ER - TY - JOUR A1 - Odziomek, Mateusz A1 - Giusto, Paolo A1 - Kossmann, Janina A1 - Tarakina, Nadezda A1 - Heske, Julian A1 - Rivadeneira, Salvador M. A1 - Keil, Waldemar A1 - Schmidt, Claudia A1 - Mazzanti, Stefano A1 - Savateev, Oleksandr A1 - Perdigon-Toro, Lorena A1 - Neher, Dieter A1 - Kühne, Thomas D. A1 - Antonietti, Markus A1 - Lopez-Salas, Nieves T1 - "Red Carbon": a rediscovered covalent crystalline semiconductor JF - Advanced materials N2 - Carbon suboxide (C3O2) is a unique molecule able to polymerize spontaneously into highly conjugated light-absorbing structures at temperatures as low as 0 degrees C. Despite obvious advantages, little is known about the nature and the functional properties of this carbonaceous material. In this work, the aim is to bring "red carbon," a forgotten polymeric semiconductor, back to the community's attention. A solution polymerization process is adapted to simplify the synthesis and control the structure. This allows one to obtain this crystalline covalent material at low temperatures. Both spectroscopic and elemental analyses support the chemical structure represented as conjugated ladder polypyrone ribbons. Density functional theory calculations suggest a crystalline structure of AB stacks of polypyrone ribbons and identify the material as a direct bandgap semiconductor with a medium bandgap that is further confirmed by optical analysis. The material shows promising photocatalytic performance using blue light. Moreover, the simple condensation-aromatization route described here allows the straightforward fabrication of conjugated ladder polymers and can be inspiring for the synthesis of carbonaceous materials at low temperatures in general. KW - carbon suboxide KW - carbonaceous materials KW - conjugated ladder polymers KW - covalent materials KW - photocatalysts Y1 - 2022 U6 - https://doi.org/10.1002/adma.202206405 SN - 0935-9648 SN - 1521-4095 VL - 34 IS - 40 PB - Wiley-VCH CY - Weinheim ER -