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 H. 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 - 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 - Zu, Fengshuo A1 - Warby, Jonathan A1 - Stolterfoht, Martin A1 - Li, Jinzhao A1 - Shin, Dongguen A1 - Unger, Eva A1 - Koch, Norbert T1 - Photoinduced energy-level realignment at interfaces between organic semiconductors and metal-halide perovskites JF - Physical review letters N2 - In contrast to the common conception that the interfacial energy-level alignment is affixed once the interface is formed, we demonstrate that heterojunctions between organic semiconductors and metal-halide perovskites exhibit huge energy-level realignment during photoexcitation. Importantly, the photoinduced level shifts occur in the organic component, including the first molecular layer in direct contact with the perovskite. This is caused by charge-carrier accumulation within the organic semiconductor under illumination and the weak electronic coupling between the junction components. Y1 - 2021 U6 - https://doi.org/10.1103/PhysRevLett.127.246401 SN - 0031-9007 SN - 1079-7114 VL - 127 IS - 24 PB - American Physical Society CY - College Park ER - TY - GEN A1 - Kirchartz, Thomas A1 - Márquez, José A. A1 - Stolterfoht, Martin A1 - Unold, Thomas T1 - Photoluminescence-based characterization of halide perovskites for photovoltaics T2 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non-radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1419 KW - metal halide perovskites KW - numerical simulations KW - photoluminescence KW - photon recycling Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-519702 SN - 1866-8372 IS - 26 ER - TY - JOUR A1 - Kirchartz, Thomas A1 - Márquez, José A. A1 - Stolterfoht, Martin A1 - Unold, Thomas T1 - Photoluminescence-based characterization of halide perovskites for photovoltaics JF - Advanced Energy Materials N2 - Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non-radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials. KW - metal halide perovskites KW - numerical simulations KW - photoluminescence KW - photon recycling Y1 - 2020 U6 - https://doi.org/10.1002/aenm.201904134 SN - 1614-6832 SN - 1614-6840 VL - 10 IS - 26 SP - 1 EP - 21 PB - Wiley CY - Weinheim 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 - 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 - Samson, Stephanie A1 - Rech, Jeromy A1 - Perdigon-Toro, Lorena A1 - Peng, Zhengxing A1 - Shoaee, Safa A1 - Ade, Harald A1 - Neher, Dieter A1 - Stolterfoht, Martin A1 - You, Wei T1 - Organic solar cells with large insensitivity to donor polymer molar mass across all acceptor classes JF - ACS applied polymer materials N2 - 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. KW - polymer solar cells KW - conjugated polymers KW - fullerenes KW - fluorination KW - molecular weight KW - non-fullerene acceptors KW - power conversion efficiency Y1 - 2020 U6 - https://doi.org/10.1021/acsapm.0c01041 SN - 2637-6105 VL - 2 IS - 11 SP - 5300 EP - 5308 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Lai, Huagui A1 - Luo, Jincheng A1 - Zwirner, Yannick A1 - Olthof, Selina A1 - Wieczorek, Alexander A1 - Ye, Fangyuan A1 - Jeangros, Quentin A1 - Yin, Xinxing A1 - Akhundova, Fatima A1 - Ma, Tianshu A1 - He, Rui A1 - Kothandaraman, Radha K. A1 - Chin, Xinyu A1 - Gilshtein, Evgeniia A1 - Muller, Andre A1 - Wang, Changlei A1 - Thiesbrummel, Jarla A1 - Siol, Sebastian A1 - Prieto, Jose Marquez A1 - Unold, Thomas A1 - Stolterfoht, Martin A1 - Chen, Cong A1 - Tiwari, Ayodhya N. A1 - Zhao, Dewei A1 - Fu, Fan T1 - High-performance flexible all-Perovskite tandem solar cells with reduced V-OC-deficit in wide-bandgap subcell JF - Advanced energy materials N2 - Among various types of perovskite-based tandem solar cells (TSCs), all-perovskite TSCs are of particular attractiveness for building- and vehicle-integrated photovoltaics, or space energy areas as they can be fabricated on flexible and lightweight substrates with a very high power-to-weight ratio. However, the efficiency of flexible all-perovskite tandems is lagging far behind their rigid counterparts primarily due to the challenges in developing efficient wide-bandgap (WBG) perovskite solar cells on the flexible substrates as well as their low open-circuit voltage (V-OC). Here, it is reported that the use of self-assembled monolayers as hole-selective contact effectively suppresses the interfacial recombination and allows the subsequent uniform growth of a 1.77 eV WBG perovskite with superior optoelectronic quality. In addition, a postdeposition treatment with 2-thiopheneethylammonium chloride is employed to further suppress the bulk and interfacial recombination, boosting the V-OC of the WBG top cell to 1.29 V. Based on this, the first proof-of-concept four-terminal all-perovskite flexible TSC with a power conversion efficiency of 22.6% is presented. When integrating into two-terminal flexible tandems, 23.8% flexible all-perovskite TSCs with a superior V-OC of 2.1 V is achieved, which is on par with the V-OC reported on the 28% all-perovskite tandems grown on the rigid substrate. KW - all-perovskite tandems KW - flexible tandem solar cells KW - perovskite KW - V OC-deficit KW - wide-bandgap Y1 - 2022 U6 - https://doi.org/10.1002/aenm.202202438 SN - 1614-6832 SN - 1614-6840 VL - 12 IS - 45 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Zeiske, Stefan A1 - Sandberg, Oskar J. A1 - Zarrabi, Nasim A1 - Wolff, Christian Michael A1 - Raoufi, Meysam A1 - Peña-Camargo, Francisco A1 - Gutierrez-Partida, Emilio A1 - Meredith, Paul A1 - Stolterfoht, Martin A1 - Armin, Ardalan T1 - Static disorder in lead halide perovskites JF - The journal of physical chemistry letters N2 - In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 +/- 1.0, 13.2 +/- 1.0, and 13.5 +/- 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ?+/- 0.5, 4.7 +/- 0.3, and 3.3 +/- 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices. KW - Cations KW - External quantum efficiency KW - Perovskites KW - Solar cells KW - Solar energy Y1 - 2022 U6 - https://doi.org/10.1021/acs.jpclett.2c01652 SN - 1948-7185 VL - 13 IS - 31 SP - 7280 EP - 7285 PB - American Chemical Society CY - Washington 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 - Tockhorn, Philipp A1 - Sutter, Johannes A1 - Cruz Bournazou, Alexandros A1 - Wagner, Philipp A1 - Jäger, Klaus A1 - Yoo, Danbi A1 - Lang, Felix A1 - Grischek, Max A1 - Li, Bor A1 - Li, Jinzhao A1 - Shargaieva, Oleksandra A1 - Unger, Eva A1 - Al-Ashouri, Amran A1 - Köhnen, Eike A1 - Stolterfoht, Martin A1 - Neher, Dieter A1 - Schlatmann, Rutger A1 - Rech, Bernd A1 - Stannowski, Bernd A1 - Albrecht, Steve A1 - Becker, Christiane T1 - Nano-optical designs for high-efficiency monolithic perovskite-silicon tandem solar cells JF - Nature nanotechnology N2 - Designing gentle sinusoidal nanotextures enables the realization of high-efficiency perovskite-silicon solar cells
Perovskite-silicon tandem solar cells offer the possibility of overcoming the power conversion efficiency limit of conventional silicon solar cells. Various textured tandem devices have been presented aiming at improved optical performance, but optimizing film growth on surface-textured wafers remains challenging. Here we present perovskite-silicon tandem solar cells with periodic nanotextures that offer various advantages without compromising the material quality of solution-processed perovskite layers. We show a reduction in reflection losses in comparison to planar tandems, with the new devices being less sensitive to deviations from optimum layer thicknesses. The nanotextures also enable a greatly increased fabrication yield from 50% to 95%. Moreover, the open-circuit voltage is improved by 15 mV due to the enhanced optoelectronic properties of the perovskite top cell. Our optically advanced rear reflector with a dielectric buffer layer results in reduced parasitic absorption at near-infrared wavelengths. As a result, we demonstrate a certified power conversion efficiency of 29.80%. Y1 - 2022 U6 - https://doi.org/10.1038/s41565-022-01228-8 SN - 1748-3387 SN - 1748-3395 VL - 17 IS - 11 SP - 1214 EP - 1221 PB - Nature Publishing Group CY - London [u.a.] ER - TY - JOUR A1 - Perdigon-Toro, Lorena A1 - Zhang, Huotian A1 - Markina, Anastaa si A1 - Yuan, Jun A1 - Hosseini, Seyed Mehrdad A1 - Wolff, Christian Michael A1 - Zuo, Guangzheng A1 - Stolterfoht, Martin A1 - Zou, Yingping A1 - Gao, Feng A1 - Andrienko, Denis A1 - Shoaee, Safa A1 - Neher, Dieter T1 - Barrierless free charge generation in the high-performance PM6:Y6 bulk heterojunction non-fullerene solar cell JF - Advanced materials N2 - 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. KW - driving force KW - non-fullerene acceptors KW - organic solar cells KW - photocurrent generation Y1 - 2020 U6 - https://doi.org/10.1002/adma.201906763 SN - 0935-9648 SN - 1521-4095 VL - 32 IS - 9 PB - Wiley-VCH CY - Weinheim ER - TY - GEN A1 - Wolff, Christian Michael A1 - Canil, Laura A1 - Rehermann, Carolin A1 - Nguyen, Ngoc Linh A1 - Zu, Fengshuo A1 - Ralaiarisoa, Maryline A1 - Caprioglio, Pietro A1 - Fiedler, Lukas A1 - Stolterfoht, Martin A1 - Kogikoski, Junior, Sergio A1 - Bald, Ilko A1 - Koch, Norbert A1 - Unger, Eva L. A1 - Dittrich, Thomas A1 - Abate, Antonio A1 - Neher, Dieter T1 - Correction to 'Perfluorinated self-assembled monolayers enhance the stability and efficiency of inverted perovskite solar cells' (2020, 14 (2), 1445−1456) T2 - ACS nano Y1 - 2020 U6 - https://doi.org/10.1021/acsnano.0c08081 SN - 1936-0851 SN - 1936-086X VL - 14 IS - 11 SP - 16156 EP - 16156 PB - American Chemical Society CY - Washington, DC ER - TY - JOUR 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 C-60-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane JF - Nature Communications N2 - Inverted perovskite solar cells still suffer from significant non-radiative recombination losses at the perovskite surface and across the perovskite/C-60 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/C-60 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 110mV, and retain >97% of the initial efficiency after 400h 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. Effective transport layers are essential to suppress non-radiative recombination losses. Here, the authors introduce phenylamino-functionalized ortho-carborane as an interfacial layer, and realise inverted perovskite solar cells with efficiency of over 23% and operational stability of T97=400h. Y1 - 2022 U6 - https://doi.org/10.1038/s41467-022-34203-x SN - 2041-1723 VL - 13 IS - 1 PB - Nature Publishing Group CY - London ER - TY - JOUR A1 - Jiang, Wei A1 - Stolterfoht, Martin A1 - Jin, Hui A1 - Burn, Paul L. T1 - Hole-transporting poly(dendrimer)s as electron donors for low donor organic solar cells with efficient charge transport JF - Macromolecules : a publication of the American Chemical Society N2 - Recent work on bulk-heterojunction organic solar cells has shown that photoexcitation of the electron acceptor followed by photoinduced hole transfer can play a significant role in photocurrent generation. To establish a clear understanding of the role of the donor in the photoinduced hole transfer process, we have synthesized a series of triphenylamine-based hole-transporting poly(dendrimer)s with mechanically flexible nonconjugated backbones via ring-opening metathesis polymerization and used them in low donor content solar cells. The poly(dendrimer)s were found to retain the hole transporting properties of the parent dendrimer, with hole mobilities of similar to 10(-3) cm(2)/(V s) for solution processed neat films. However, when blended with [6,6]-phenyl-C-70-butyric acid methyl ester (PC70BM), the best performing poly(dendrimer) was found to form films that had balanced and relatively high hole/electron mobilities of similar to 5 x 10(-4) cm(2) /(V s). In contrast, at the same concentration the parent dendrimer:PC70BM blend was found to have a hole mobility of 4 orders of magnitude less than the electron mobility. The balanced hole and electron mobilities for the 6 wt % poly(dendrimer):PC70BM blend led to an absence of second-order bimolecular recombination losses at the maximum power point and resulted in a fill factor of 0.65 and a PCE 2.1% for the devices, which was almost three times higher than the cells composed of the parent dendrimer:PC70BM blends. Y1 - 2020 U6 - https://doi.org/10.1021/acs.macromol.0c00520 SN - 0024-9297 SN - 1520-5835 VL - 53 IS - 8 SP - 2902 EP - 2911 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Jiang, Wei A1 - Tao, Chen A1 - Stolterfoht, Martin A1 - Jin, Hui A1 - Stephen, Meera A1 - Lin, Qianqian A1 - Nagiri, Ravi C. R. A1 - Burn, Paul L. A1 - Gentle, Ian R. T1 - Hole-transporting materials for low donor content organic solar cells BT - charge transport and device performance JF - Organic electronics : physics, materials and applications N2 - Low donor content solar cells are an intriguing class of photovoltaic device about which there is still considerable discussion with respect to their mode of operation. We have synthesized a series of triphenylamine-based materials for use in low donor content devices with the electron accepting [6,6]-phenyl-C71-butyric acid methyl ester (PC(7)0BM). The triphenylamine-based materials absorb light in the near UV enabling the PC(7)0BM to be be the main light absorbing organic semiconducting material in the solar cell. It was found that the devices did not operate as classical Schottky junctions but rather photocurrent was generated by hole transfer from the photo-excited PC(7)0BM to the triphenylamine-based donors. We found that replacing the methoxy surface groups with methyl groups on the donor material led to a decrease in hole mobility for the neat films, which was due to the methyl substituted materials having the propensity to aggregate. The thermodynamic drive to aggregate was advantageous for the performance of the low donor content (6 wt%) films. It was found that the 6 wt% donor devices generally gave higher performance than devices containing 50 wt% of the donor. KW - photoexcited hole transfer KW - photocurrent generation KW - synthesis KW - hole KW - mobility KW - low donor content KW - Schottky junction Y1 - 2020 U6 - https://doi.org/10.1016/j.orgel.2019.105480 SN - 1566-1199 SN - 1878-5530 VL - 76 PB - Elsevier CY - Amsterdam 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 - 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 - Shoai, 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 JF - Nature Communications 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. Y1 - 2022 U6 - https://doi.org/10.1038/s41467-022-34203-x SN - 2041-1723 VL - 13 PB - Springer Nature CY - London ER - TY - JOUR A1 - Sandberg, Oskar J. A1 - Kurpiers, Jona A1 - Stolterfoht, Martin A1 - Neher, Dieter A1 - Meredith, Paul A1 - Shoaee, Safa A1 - Armin, Ardalan T1 - On the question of the need for a built-in potential in Perovskite solar cells JF - Advanced materials interfaces N2 - 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. KW - built-in potential KW - charge collection KW - charge transport layers KW - perovskite solar cells Y1 - 2020 U6 - https://doi.org/10.1002/admi.202000041 SN - 2196-7350 VL - 7 IS - 10 PB - Wiley CY - Hoboken ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Lang, Felix T1 - All-perovskite tandems get flexible JF - Nature energy N2 - Flexible all-perovskite tandem photovoltaics open up new opportunities for application compared to rigid devices, yet their performance lags behind. Now, researchers show that molecule-bridged interfaces mitigate charge recombination and crack formation, improving the efficiency and mechanical reliability of flexible devices. Y1 - 2022 U6 - https://doi.org/10.1038/s41560-022-01087-6 SN - 2058-7546 VL - 7 IS - 8 SP - 688 EP - 689 PB - Nature Publishing Group CY - London ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Wolff, Christian Michael A1 - Amir, Yohai A1 - Paulke, Andreas A1 - Perdigon-Toro, Lorena A1 - Caprioglio, Pietro A1 - Neher, Dieter T1 - Approaching the fill factor Shockley-Queisser limit in stable, dopant-free triple cation perovskite solar cells JF - Energy & Environmental Science N2 - Perovskite solar cells now compete with their inorganic counterparts in terms of power conversion efficiency, not least because of their small open-circuit voltage (V-OC) losses. A key to surpass traditional thin-film solar cells is the fill factor (FF). Therefore, more insights into the physical mechanisms that define the bias dependence of the photocurrent are urgently required. In this work, we studied charge extraction and recombination in efficient triple cation perovskite solar cells with undoped organic electron/hole transport layers (ETL/HTL). Using integral time of flight we identify the transit time through the HTL as the key figure of merit for maximizing the fill factor (FF) and efficiency. Complementarily, intensity dependent photocurrent and V-OC measurements elucidate the role of the HTL on the bias dependence of non-radiative and transport-related loss channels. We show that charge transport losses can be completely avoided under certain conditions, yielding devices with FFs of up to 84%. Optimized cells exhibit power conversion efficiencies of above 20% for 6 mm(2) sized pixels and 18.9% for a device area of 1 cm(2). These are record efficiencies for hybrid perovskite devices with dopant-free transport layers, highlighting the potential of this device technology to avoid charge-transport limitations and to approach the Shockley-Queisser limit. Y1 - 2017 U6 - https://doi.org/10.1039/c7ee00899f SN - 1754-5692 SN - 1754-5706 VL - 10 SP - 1530 EP - 1539 PB - Royal Society of Chemistry CY - Cambridge ER - TY - GEN A1 - Saliba, Michael A1 - Stolterfoht, Martin A1 - Wolff, Christian Michael A1 - Neher, Dieter A1 - Abate, Antonio T1 - Measuring aging stability of perovskite solar cells T2 - Joule Y1 - 2018 U6 - https://doi.org/10.1016/j.joule.2018.05.005 SN - 2542-4351 VL - 2 IS - 6 SP - 1019 EP - 1024 PB - Cell Press CY - Cambridge ER - TY - JOUR A1 - Yazmaciyan, Aren A1 - Stolterfoht, Martin A1 - Burn, Paul L. A1 - Lin, Qianqian A1 - Meredith, Paul A1 - Armin, Ardalan T1 - Recombination losses above and below the transport percolation threshold in bulk heterojunction organic solar cells JF - Advanced energy materials N2 - Achieving the highest power conversion efficiencies in bulk heterojunction organic solar cells requires a morphology that delivers electron and hole percolation pathways for optimized transport, plus sufficient donor:acceptor contact area for near unity charge transfer state formation. This is a significant structural challenge, particularly in semiconducting polymer:fullerene systems. This balancing act in the model high efficiency PTB7:PC70BM blend is studied by tuning the donor:acceptor ratio, with a view to understanding the recombination loss mechanisms above and below the fullerene transport percolation threshold. The internal quantum efficiency is found to be strongly correlated to the slower carrier mobility in agreement with other recent studies. Furthermore, second-order recombination losses dominate the shape of the current density-voltage curve in efficient blend combinations, where the fullerene phase is percolated. However, below the charge transport percolation threshold, there is an electric-field dependence of first-order losses, which includes electric-field-dependent photogeneration. In the intermediate regime, the fill factor appears to be limited by both first- and second-order losses. These findings provide additional basic understanding of the interplay between the bulk heterojunction morphology and the order of recombination in organic solar cells. They also shed light on the limitations of widely used transport models below the percolation threshold. KW - bulk heterojunctions KW - charge transport KW - organic solar cells KW - percolation threshold KW - recombination losses Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201703339 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 18 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 - JOUR 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 JF - Solar RRL 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. KW - cesium lead halides KW - crystal orientation KW - inorganic perovskites KW - ISOS-L-1I protocol KW - phase purity KW - photostability Y1 - 2020 VL - 4 IS - 9 PB - WILEY-VCH CY - Weinheim ER - TY - JOUR A1 - Zhang, Shanshan A1 - Stolterfoht, Martin A1 - Armin, Ardalan A1 - Lin, Qianqian A1 - Zu, Fengshuo A1 - Sobus, Jan A1 - Jin, Hui A1 - Koch, Norbert A1 - Meredith, Paul A1 - Burn, Paul L. A1 - Neher, Dieter T1 - Interface Engineering of Solution-Processed Hybrid Organohalide Perovskite Solar Cells JF - ACS applied materials & interfaces N2 - Engineering the interface between the perovskite absorber and the charge-transporting layers has become an important method for improving the charge extraction and open-circuit voltage (V-OC) of hybrid perovskite solar cells. Conjugated polymers are particularly suited to form the hole-transporting layer, but their hydrophobicity renders it difficult to solution-process the perovskite absorber on top. Herein, oxygen plasma treatment is introduced as a simple means to change the surface energy and work function of hydrophobic polymer interlayers for use as p-contacts in perovskite solar cells. We find that upon oxygen plasma treatment, the hydrophobic surfaces of different prototypical p-type polymers became sufficiently hydrophilic to enable subsequent perovskite junction processing. In addition, the oxygen plasma treatment also increased the ionization potential of the polymer such that it became closer to the valance band energy of the perovskite. It was also found that the oxygen plasma treatment could increase the electrical conductivity of the p-type polymers, facilitating more efficient charge extraction. On the basis of this concept, inverted MAPbI(3) perovskite devices with different oxygen plasma-treated polymers such as P3HT, P3OT, polyTPD, or PTAA were fabricated with power conversion efficiencies of up to 19%. KW - organohalide lead perovskites KW - solar cells KW - surface wetting KW - work function KW - oxygen plasma KW - transport layer Y1 - 2018 U6 - https://doi.org/10.1021/acsami.8b02503 SN - 1944-8244 VL - 10 IS - 25 SP - 21681 EP - 21687 PB - American Chemical Society CY - Washington ER - TY - JOUR 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 JF - Solar RRL 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. KW - heterojunction silicon solar cells KW - interfaces KW - perovskite solar cells KW - tandem solar cells KW - thin films Y1 - 2020 VL - 4 IS - 7 PB - John Wiley & Sons, Inc. CY - New Jersey 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 - Krückemeier, Lisa A1 - Rau, Uwe A1 - Stolterfoht, Martin A1 - Kirchartz, Thomas T1 - How to report record open-circuit voltages in lead-halide perovskite solar cells T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - Open-circuit voltages of lead-halide perovskite solar cells are improving rapidly and are approaching the thermodynamic limit. Since many different perovskite compositions with different bandgap energies are actively being investigated, it is not straightforward to compare the open-circuit voltages between these devices as long as a consistent method of referencing is missing. For the purpose of comparing open-circuit voltages and identifying outstanding values, it is imperative to use a unique, generally accepted way of calculating the thermodynamic limit, which is currently not the case. Here a meta-analysis of methods to determine the bandgap and a radiative limit for open-circuit voltage is presented. The differences between the methods are analyzed and an easily applicable approach based on the solar cell quantum efficiency as a general reference is proposed. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1194 KW - Shockley-Queisser model KW - bandgap KW - fill factor losses KW - nonradiative voltage losses KW - photovoltaics KW - radiative limit KW - recombination Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-525289 SN - 1866-8372 IS - 1 ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Wolff, Christian Michael A1 - Marquez, Jose A. A1 - Zhang, Shanshan A1 - Hages, Charles J. A1 - Rothhardt, Daniel A1 - Albrecht, Steve A1 - Burn, Paul L. A1 - Meredith, Paul A1 - Unold, Thomas A1 - Neher, Dieter T1 - Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells JF - Nature Energy N2 - The performance of perovskite solar cells is predominantly limited by non-radiative recombination, either through trap-assisted recombination in the absorber layer or via minority carrier recombination at the perovskite/transport layer interfaces. Here, we use transient and absolute photoluminescence imaging to visualize all non-radiative recombination pathways in planar pintype perovskite solar cells with undoped organic charge transport layers. We find significant quasi-Fermi-level splitting losses (135 meV) in the perovskite bulk, whereas interfacial recombination results in an additional free energy loss of 80 meV at each individual interface, which limits the open-circuit voltage (V-oc) of the complete cell to similar to 1.12 V. Inserting ultrathin interlayers between the perovskite and transport layers leads to a substantial reduction of these interfacial losses at both the p and n contacts. Using this knowledge and approach, we demonstrate reproducible dopant-free 1 cm(2) perovskite solar cells surpassing 20% efficiency (19.83% certified) with stabilized power output, a high V-oc (1.17 V) and record fill factor (>81%). KW - Energy science and technology KW - Solar cells Y1 - 2018 U6 - https://doi.org/10.1038/s41560-018-0219-8 SN - 2058-7546 VL - 3 IS - 10 SP - 847 EP - 854 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Shoaee, Safa A1 - Stolterfoht, Martin A1 - Neher, Dieter T1 - The Role of Mobility on Charge Generation, Recombination, and Extraction in Polymer-Based Solar Cells JF - dvanced energy materials N2 - Organic semiconductors are of great interest for a broad range of optoelectronic applications due to their solution processability, chemical tunability, highly scalable fabrication, and mechanical flexibility. In contrast to traditional inorganic semiconductors, organic semiconductors are intrinsically disordered systems and therefore exhibit much lower charge carrier mobilities-the Achilles heel of organic photovoltaic cells. In this progress review, the authors discuss recent important developments on the impact of charge carrier mobility on the charge transfer state dissociation, and the interplay of free charge extraction and recombination. By comparing the mobilities on different timescales obtained by different techniques, the authors highlight the dispersive nature of these materials and how this reflects on the key processes defining the efficiency of organic photovoltaics. KW - charge generation KW - charge recombination KW - extraction KW - mobility KW - organic solar cells KW - polymer:fullerene bulk heterojunction Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201703355 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 28 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Krückemeier, Lisa A1 - Rau, Uwe A1 - Stolterfoht, Martin A1 - Kirchartz, Thomas T1 - How to report record open-circuit voltages in lead-halide perovskite solar cells JF - Advanced energy materials N2 - Open-circuit voltages of lead-halide perovskite solar cells are improving rapidly and are approaching the thermodynamic limit. Since many different perovskite compositions with different bandgap energies are actively being investigated, it is not straightforward to compare the open-circuit voltages between these devices as long as a consistent method of referencing is missing. For the purpose of comparing open-circuit voltages and identifying outstanding values, it is imperative to use a unique, generally accepted way of calculating the thermodynamic limit, which is currently not the case. Here a meta-analysis of methods to determine the bandgap and a radiative limit for open-circuit voltage is presented. The differences between the methods are analyzed and an easily applicable approach based on the solar cell quantum efficiency as a general reference is proposed. KW - bandgap KW - fill factor losses KW - nonradiative voltage losses KW - photovoltaics KW - radiative limit KW - recombination KW - Shockley-Queisser model Y1 - 2019 U6 - https://doi.org/10.1002/aenm.201902573 SN - 1614-6832 SN - 1614-6840 VL - 10 IS - 1 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Caprioglio, Pietro A1 - Zu, Fengshuo A1 - Wolff, Christian Michael A1 - Prieto, Jose A. Marquez A1 - Stolterfoht, Martin A1 - Becker, Pascal A1 - Koch, Norbert A1 - Unold, Thomas A1 - Rech, Bernd A1 - Albrecht, Steve A1 - Neher, Dieter T1 - High open circuit voltages in pin-type perovskite solar cells through strontium addition JF - Sustainable Energy & Fuels N2 - The incorporation of even small amounts of strontium (Sr) into lead-base hybrid quadruple cation perovskite solar cells results in a systematic increase of the open circuit voltage (V-oc) in pin-type perovskite solar cells. We demonstrate via absolute and transient photoluminescence (PL) experiments how the incorporation of Sr significantly reduces the non-radiative recombination losses in the neat perovskite layer. We show that Sr segregates at the perovskite surface, where it induces important changes of morphology and energetics. Notably, the Sr-enriched surface exhibits a wider band gap and a more n-type character, accompanied with significantly stronger surface band bending. As a result, we observe a significant increase of the quasi-Fermi level splitting in the neat perovskite by reduced surface recombination and more importantly, a strong reduction of losses attributed to non-radiative recombination at the interface to the C-60 electron-transporting layer. The resulting solar cells exhibited a V-oc of 1.18 V, which could be further improved to nearly 1.23 V through addition of a thin polymer interlayer, reducing the non-radiative voltage loss to only 110 meV. Our work shows that simply adding a small amount of Sr to the precursor solutions induces a beneficial surface modification in the perovskite, without requiring any post treatment, resulting in high efficiency solar cells with power conversion efficiency (PCE) up to 20.3%. Our results demonstrate very high V-oc values and efficiencies in Sr-containing quadruple cation perovskite pin-type solar cells and highlight the imperative importance of addressing and minimizing the recombination losses at the interface between perovskite and charge transporting layer. Y1 - 2019 U6 - https://doi.org/10.1039/c8se00509e SN - 2398-4902 VL - 3 IS - 2 SP - 550 EP - 563 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR 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 JF - advanced energy materials 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. KW - electro-optical materials KW - perovskite solar cells KW - photovoltaic devices KW - thin films Y1 - 2019 U6 - https://doi.org/10.1002/aenm.201901631 SN - 1614-6832 SN - 1614-6840 VL - 9 IS - 33 PB - Wiley-VCH CY - Weinheim ER - TY - GEN A1 - Pisoni, Stefano A1 - Stolterfoht, Martin A1 - Lockinger, Johannes A1 - Moser, Thierry A1 - Jiang, Yan A1 - Caprioglio, Pietro A1 - Neher, Dieter A1 - Buecheler, Stephan A1 - Tiwari, Ayodhya N. T1 - On the origin of open-circuit voltage losses in flexible n-i-p perovskite solar cells T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] . T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1110 KW - Perovskite solar cell KW - flexible KW - interface engineering KW - non-radiative recombination KW - quasi-Fermi level splitting Y1 - 2021 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-459617 SN - 1866-8372 IS - 1110 ER - TY - JOUR A1 - Würfel, Uli A1 - Perdigon-Toro, Lorena A1 - Kurpiers, Jona A1 - Wolff, Christian Michael A1 - Caprioglio, Pietro A1 - Rech, Jeromy James A1 - Zhu, Jingshuai A1 - Zhan, Xiaowei A1 - You, Wei A1 - Shoaee, Safa A1 - Neher, Dieter A1 - Stolterfoht, Martin T1 - Recombination between Photogenerated and Electrode-Induced Charges Dominates the Fill Factor Losses in Optimized Organic Solar Cells JF - The journal of physical chemistry letters N2 - Charge extraction in organic solar cells (OSCs) is commonly believed to be limited by bimolecular recombination of photogenerated charges. However, the fill factor of OSCs is usually almost entirely governed by recombination processes that scale with the first order of the light intensity. This linear loss was often interpreted to be a consequence of geminate or trap-assisted recombination. Numerical simulations show that this linear dependence is a direct consequence of the large amount of excess dark charge near the contact. The first-order losses increase with decreasing mobility of minority carriers, and we discuss the impact of several material and device parameters on this loss mechanism. This work highlights that OSCs are especially vulnerable to injected charges as a result of their poor charge transport properties. This implies that dark charges need to be better accounted for when interpreting electro-optical measurements and charge collection based on simple figures of merit. Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpclett.9b01175 SN - 1948-7185 VL - 10 IS - 12 SP - 3473 EP - 3480 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Zhang, Shanshan A1 - Hosseini, Seyed Mehrdad A1 - Gunder, Rene A1 - Petsiuk, Andrei A1 - Caprioglio, Pietro A1 - Wolff, Christian Michael A1 - Shoaee, Safa A1 - Meredith, Paul A1 - Schorr, Susan A1 - Unold, Thomas A1 - Burn, Paul L. A1 - Neher, Dieter A1 - Stolterfoht, Martin T1 - The Role of Bulk and Interface Recombination in High-Efficiency Low-Dimensional Perovskite Solar Cells JF - Advanced materials N2 - 2D Ruddlesden-Popper perovskite (RPP) solar cells have excellent environmental stability. However, the power conversion efficiency (PCE) of RPP cells remains inferior to 3D perovskite-based cells. Herein, 2D (CH3(CH2)(3)NH3)(2)(CH3NH3)(n-1)PbnI3n+1 perovskite cells with different numbers of [PbI6](4-) sheets (n = 2-4) are analyzed. Photoluminescence quantum yield (PLQY) measurements show that nonradiative open-circuit voltage (V-OC) losses outweigh radiative losses in materials with n > 2. The n = 3 and n = 4 films exhibit a higher PLQY than the standard 3D methylammonium lead iodide perovskite although this is accompanied by increased interfacial recombination at the top perovskite/C-60 interface. This tradeoff results in a similar PLQY in all devices, including the n = 2 system where the perovskite bulk dominates the recombination properties of the cell. In most cases the quasi-Fermi level splitting matches the device V-OC within 20 meV, which indicates minimal recombination losses at the metal contacts. The results show that poor charge transport rather than exciton dissociation is the primary reason for the reduction in fill factor of the RPP devices. Optimized n = 4 RPP solar cells had PCEs of 13% with significant potential for further improvements. KW - 2D perovskites KW - interface recombination KW - perovskite solar cells KW - photoluminescence KW - V-OC loss Y1 - 2019 U6 - https://doi.org/10.1002/adma.201901090 SN - 0935-9648 SN - 1521-4095 VL - 31 IS - 30 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Caprioglio, Pietro A1 - Wolff, Christian Michael A1 - Marquez, Jose A. A1 - Nordmann, Joleik A1 - Zhang, Shanshan A1 - Rothhardt, Daniel A1 - Hörmann, Ulrich A1 - Amir, Yohai A1 - Redinger, Alex A1 - Kegelmann, Lukas A1 - Zu, Fengshuo A1 - Albrecht, Steve A1 - Koch, Norbert A1 - Kirchartz, Thomas A1 - Saliba, Michael A1 - Unold, Thomas A1 - Neher, Dieter T1 - The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells JF - Energy & environmental science N2 - Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces. Y1 - 2019 U6 - https://doi.org/10.1039/c9ee02020a SN - 1754-5692 SN - 1754-5706 VL - 12 IS - 9 SP - 2778 EP - 2788 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Le Corre, Vincent M. A1 - Stolterfoht, Martin A1 - Perdigón-Toro, Lorena A1 - Feuerstein, Markus A1 - Wolff, Christian Michael A1 - Gil-Escrig, Lidon A1 - Bolink, Henk J. A1 - Neher, Dieter A1 - Koster, L. Jan Anton T1 - Charge Transport Layers Limiting the Efficiency of Perovskite Solar Cells: How To Optimize Conductivity, Doping, and Thickness JF - ACS Applied Energy Materials N2 - Perovskite solar cells (PSCs) are one of the main research topics of the photovoltaic community; with efficiencies now reaching up to 24%, PSCs are on the way to catching up with classical inorganic solar cells. However, PSCs have not yet reached their full potential. In fact, their efficiency is still limited by nonradiative recombination, mainly via trap-states and by losses due to the poor transport properties of the commonly used transport layers (TLs). Indeed, state-of-the-art TLs (especially if organic) suffer from rather low mobilities, typically within 10(-5) and 10(-2) cm(-2) V-1 s(-1), when compared to the high mobilities, 1-10 cm(-2) V-1 s(-1), measured for perovskites. This work presents a comprehensive analysis of the effect of the mobility, thickness, and doping density of the transport layers based on combined experimental and modeling results of two sets of devices made of a solution-processed high-performing triple-cation (PCE approximate to 20%). The results are also cross-checked on vacuum-processed MAPbI(3) devices. From this analysis, general guidelines on how to optimize a TL are introduced and especially a new and simple formula to easily calculate the amount of doping necessary to counterbalance the low mobility of the TLs. KW - perovskite solar cells KW - transport layers KW - conductivity KW - doping KW - charge transport Y1 - 2019 U6 - https://doi.org/10.1021/acsaem.9b00856 SN - 2574-0962 VL - 2 IS - 9 SP - 6280 EP - 6287 PB - American Chemical Society CY - Washington ER - TY - JOUR 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 JF - Solar RRL 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. KW - charge generation KW - charge transfers KW - non-Langevin recombination KW - spin-related factors Y1 - 2019 U6 - https://doi.org/10.1002/solr.201900184 SN - 2367-198X VL - 3 IS - 11 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Le Corre, Vincent M. A1 - Feuerstein, Markus A1 - Caprioglio, Pietro A1 - Koster, Lambert Jan Anton A1 - Neher, Dieter T1 - Voltage-Dependent Photoluminescence and How It Correlates with the Fill Factor and Open-Circuit Voltage in Perovskite Solar Cells JF - Acs energy letters N2 - Optimizing the photoluminescence (PL) yield of a solar cell has long been recognized as a key principle to maximize the power conversion efficiency. While PL measurements are routinely applied to perovskite films and solar cells under open circuit conditions (V-OC), it remains unclear how the emission depends on the applied voltage. Here, we performed PL(V) measurements on perovskite cells with different hole transport layer thicknesses and doping concentrations, resulting in remarkably different fill factors (FFs). The results reveal that PL(V) mirrors the current-voltage (JV) characteristics in the power-generating regime, which highlights an interesting correlation between radiative and nonradiative recombination losses. In particular, high FF devices show a rapid quenching of PL(V) from open-circuit to the maximum power point. We conclude that, while the PL has to be maximized at V-OC at lower biases < V-OC the PL must be rapidly quenched as charges need to be extracted prior to recombination. Y1 - 2019 U6 - https://doi.org/10.1021/acsenergylett.9b02262 SN - 2380-8195 VL - 4 IS - 12 SP - 2887 EP - 2892 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Pisoni, Stefano A1 - Stolterfoht, Martin A1 - Lockinger, Johannes A1 - Moser, Thierry A1 - Jiang, Yan A1 - Caprioglio, Pietro A1 - Neher, Dieter A1 - Buecheler, Stephan A1 - Tiwari, Ayodhya N. T1 - On the origin of open-circuit voltage losses in flexible n-i-p perovskite solar cells JF - Science and technology of advanced materials : STAM N2 - The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] . KW - Perovskite solar cell KW - flexible KW - interface engineering KW - non-radiative recombination KW - quasi-Fermi level splitting Y1 - 2019 U6 - https://doi.org/10.1080/14686996.2019.1633952 SN - 1468-6996 SN - 1878-5514 VL - 20 SP - 786 EP - 795 PB - Taylor & Francis CY - Abingdon ER - TY - JOUR A1 - Stolterfoht, Martin A1 - Armin, Ardalan A1 - Philippa, Bronson A1 - Neher, Dieter T1 - The Role of Space Charge Effects on the Competition between Recombination and Extraction in Solar Cells with Low-Mobility Photoactive Layers JF - The journal of physical chemistry letters N2 - The competition between charge extraction and nongeminate recombination critically determines the current-voltage characteristics of organic solar cells (OSCs) and their fill factor. As a measure of this competition, several figures of merit (FOMs) have been put forward; however, the impact of space charge effects has been either neglected, or not specifically addressed. Here we revisit recently reported FOMs and discuss the role of space charge effects on the interplay between recombination and extraction. We find that space charge effects are the primary cause for the onset of recombination in so-called non-Langevin systems, which also depends on the slower carrier mobility and recombination coefficient. The conclusions are supported with numerical calculations and experimental results of 25 different donor/acceptor OSCs with different charge transport parameters, active layer thicknesses or composition ratios. The findings represent a conclusive understanding of bimolecular recombination for drift dominated photocurrents and allow one to minimize these losses for given device parameters. Y1 - 2016 U6 - https://doi.org/10.1021/acs.jpclett.6b02106 SN - 1948-7185 VL - 7 SP - 4716 EP - 4721 PB - American Chemical Society CY - Washington ER -