@article{NeherKniepertElimelechetal.2016, author = {Neher, Dieter and Kniepert, Juliane and Elimelech, Arik and Koster, L. Jan Anton}, title = {A New Figure of Merit for Organic Solar Cells with Transport-limited Photocurrents}, series = {Scientific reports}, volume = {6}, journal = {Scientific reports}, publisher = {Nature Publishing Group}, address = {London}, issn = {2045-2322}, doi = {10.1038/srep24861}, pages = {9}, year = {2016}, abstract = {Compared to their inorganic counterparts, organic semiconductors suffer from relatively low charge carrier mobilities. Therefore, expressions derived for inorganic solar cells to correlate characteristic performance parameters to material properties are prone to fail when applied to organic devices. This is especially true for the classical Shockley-equation commonly used to describe current-voltage (JV)-curves, as it assumes a high electrical conductivity of the charge transporting material. Here, an analytical expression for the JV-curves of organic solar cells is derived based on a previously published analytical model. This expression, bearing a similar functional dependence as the Shockley-equation, delivers a new figure of merit α to express the balance between free charge recombination and extraction in low mobility photoactive materials. This figure of merit is shown to determine critical device parameters such as the apparent series resistance and the fill factor.}, language = {en} } @misc{NeherKniepertElimelechetal.2016, author = {Neher, Dieter and Kniepert, Juliane and Elimelech, Arik and Koster, L. Jan Anton}, title = {A New Figure of Merit for Organic Solar Cells with Transport-limited Photocurrents}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-91414}, pages = {9}, year = {2016}, abstract = {Compared to their inorganic counterparts, organic semiconductors suffer from relatively low charge carrier mobilities. Therefore, expressions derived for inorganic solar cells to correlate characteristic performance parameters to material properties are prone to fail when applied to organic devices. This is especially true for the classical Shockley-equation commonly used to describe current-voltage (JV)-curves, as it assumes a high electrical conductivity of the charge transporting material. Here, an analytical expression for the JV-curves of organic solar cells is derived based on a previously published analytical model. This expression, bearing a similar functional dependence as the Shockley-equation, delivers a new figure of merit α to express the balance between free charge recombination and extraction in low mobility photoactive materials. This figure of merit is shown to determine critical device parameters such as the apparent series resistance and the fill factor.}, language = {en} } @article{FoertigKniepertGlueckeretal.2014, author = {Foertig, Alexander and Kniepert, Juliane and Gluecker, Markus and Brenner, Thomas J. K. and Dyakonov, Vladimir and Neher, Dieter and Deibel, Carsten}, title = {Nongeminate and geminate recombination in PTB7: PCBM solar cells}, series = {Advanced functional materials}, volume = {24}, journal = {Advanced functional materials}, number = {9}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1616-301X}, doi = {10.1002/adfm.201302134}, pages = {1306 -- 1311}, year = {2014}, language = {en} } @article{KniepertPaulkePerdigonToroetal.2019, author = {Kniepert, Juliane and Paulke, Andreas and Perdigon-Toro, Lorena and Kurpiers, Jona and Zhang, Huotian and Gao, Feng and Yuan, Jun and Zou, Yingping and Le Corre, Vincent M. and Koster, Lambert Jan Anton and Neher, Dieter}, title = {Reliability of charge carrier recombination data determined with charge extraction methods}, series = {Journal of applied physics}, volume = {126}, journal = {Journal of applied physics}, number = {20}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0021-8979}, doi = {10.1063/1.5129037}, pages = {15}, year = {2019}, abstract = {Charge extraction methods are popular for measuring the charge carrier density in thin film organic solar cells and to draw conclusions about the order and coefficient of nongeminate charge recombination. However, results from such studies may be falsified by inhomogeneous steady state carrier profiles or surface recombination. Here, we present a detailed drift-diffusion study of two charge extraction methods, bias-assisted charge extraction (BACE) and time-delayed collection field (TDCF). Simulations are performed over a wide range of the relevant parameters. Our simulations reveal that both charge extraction methods provide reliable information about the recombination order and coefficient if the measurements are performed under appropriate conditions. However, results from BACE measurements may be easily affected by surface recombination, in particular for small active layer thicknesses and low illumination densities. TDCF, on the other hand, is more robust against surface recombination due to its transient nature but also because it allows for a homogeneous high carrier density to be inserted into the active layer. Therefore, TDCF is capable to provide meaningful information on the order and coefficient of recombination even if the model conditions are not exactly fulfilled. We demonstrate this for an only 100 nm thick layer of a highly efficient nonfullerene acceptor (NFA) blend, comprising the donor polymer PM6 and the NFA Y6. TDCF measurements were performed as a function of delay time for different laser fluences and bias conditions. The full set of data could be consistently fitted by a strict second order recombination process, with a bias- and fluence-independent bimolecular recombination coefficient k(2) = 1.7 x 10(-17)m(3) s(-1). BACE measurements performed on the very same layer yielded the identical result, despite the very different excitation conditions. This proves that recombination in this blend is mostly through processes in the bulk and that surface recombination is of minor importance despite the small active layer thickness. Published under license by AIP Publishing.}, language = {en} } @article{PaulkeStranksKniepertetal.2016, author = {Paulke, Andreas and Stranks, Samuel D. and Kniepert, Juliane and Kurpiers, Jona and Wolff, Christian Michael and Sch{\"o}n, Natalie and Snaith, Henry J. and Brenner, Thomas J. K. and Neher, Dieter}, title = {Charge carrier recombination dynamics in perovskite and polymer solar cells}, series = {Applied physics letters}, volume = {108}, journal = {Applied physics letters}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.4944044}, pages = {252 -- 262}, year = {2016}, abstract = {Time-delayed collection field experiments are applied to planar organometal halide perovskite (CH3NH3PbI3) based solar cells to investigate charge carrier recombination in a fully working solar cell at the nanosecond to microsecond time scale. Recombination of mobile (extractable) charges is shown to follow second-order recombination dynamics for all fluences and time scales tested. Most importantly, the bimolecular recombination coefficient is found to be time-dependent, with an initial value of ca. 10(-9) cm(3)/s and a progressive reduction within the first tens of nanoseconds. Comparison to the prototypical organic bulk heterojunction device PTB7:PC71BM yields important differences with regard to the mechanism and time scale of free carrier recombination. (C) 2016 AIP Publishing LLC.}, language = {en} } @article{AlbrechtJanietzSchindleretal.2012, author = {Albrecht, Steve and Janietz, Silvia and Schindler, Wolfram and Frisch, Johannes and Kurpiers, Jona and Kniepert, Juliane and Inal, Sahika and Pingel, Patrick and Fostiropoulos, Konstantinos and Koch, Norbert and Neher, Dieter}, title = {Fluorinated Copolymer PCPDTBT with enhanced open-circuit voltage and reduced recombination for highly efficient polymer solar cells}, series = {Journal of the American Chemical Society}, volume = {134}, journal = {Journal of the American Chemical Society}, number = {36}, publisher = {American Chemical Society}, address = {Washington}, issn = {0002-7863}, doi = {10.1021/ja305039j}, pages = {14932 -- 14944}, year = {2012}, abstract = {A novel fluorinated copolymer (F-PCPDTBT) is introduced and shown to exhibit significantly higher power conversion efficiency in bulk heterojunction solar cells with PC70BM compared to the well-known low-band-gap polymer PCPDTBT. Fluorination lowers the polymer HOMO level, resulting in high open-circuit voltages well exceeding 0.7 V. Optical spectroscopy and morphological studies with energy-resolved transmission electron microscopy reveal that the fluorinated polymer aggregates more strongly in pristine and blended layers, with a smaller amount of additives needed to achieve optimum device performance. Time-delayed collection field and charge extraction by linearly increasing voltage are used to gain insight into the effect of fluorination on the field dependence of free charge-carrier generation and recombination. F-PCPDTBT is shown to exhibit a significantly weaker field dependence of free charge-carrier generation combined with an overall larger amount of free charges, meaning that geminate recombination is greatly reduced. Additionally, a 3-fold reduction in non-geminate recombination is measured compared to optimized PCPDTBT blends. As a consequence of reduced non-geminate recombination, the performance of optimized blends of fluorinated PCPDTBT with PC70BM is largely determined by the field dependence of free-carrier generation, and this field dependence is considerably weaker compared to that of blends comprising the non-fluorinated polymer. For these optimized blends, a short-circuit current of 14 mA/cm(2), an open-circuit voltage of 0.74 V, and a fill factor of 58\% are achieved, giving a highest energy conversion efficiency of 6.16\%. The superior device performance and the low band-gap render this new polymer highly promising for the construction of efficient polymer-based tandem solar cells.}, language = {en} } @article{KniepertLangeHeidbrinketal.2015, author = {Kniepert, Juliane and Lange, Ilja and Heidbrink, Jan and Kurpiers, Jona and Brenner, Thomas J. K. and Koster, L. Jan Anton and Neher, Dieter}, title = {Effect of Solvent Additive on Generation, Recombination, and Extraction in PTB7:PCBM Solar Cells: A Conclusive Experimental and Numerical Simulation Study}, series = {The journal of physical chemistry : C, Nanomaterials and interfaces}, volume = {119}, journal = {The journal of physical chemistry : C, Nanomaterials and interfaces}, number = {15}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/jp512721e}, pages = {8310 -- 8320}, year = {2015}, abstract = {Time-delayed collection field (TDCF), bias-assisted charge extraction (BACE), and space charge-limited current (SCLC) measurements are combined with complete numerical device simulations to unveil the effect of the solvent additive 1,8-diiodooctane (DIO) on the performance of PTB7:PCBM bulk heterojunction solar cells. DIO is shown to increase the charge generation rate, reduce geminate and bimolecular recombination, and increase the electron mobility. In total, the reduction of loss currents by processing with the additive raises the power conversion efficiency of the PTB7:PCBM blend by a factor of almost three. The lower generation rates and higher geminate recombination losses in devices without DIO are consistent with a blend morphology comprising large fullerene clusters embedded within a PTB7-rich matrix, while the low electron mobility suggests that these fullerene clusters are themselves composed of smaller pure fullerene aggregates separated by disordered areas. Our device simulations show unambiguously that the effect of the additive on the shape of the currentvoltage curve (J-V) cannot be ascribed to the variation of only the mobility, the recombination, or the field dependence of generation. It is only when the changes of all three parameters are taken into account that the simulation matches the experimental J-V characteristics under all illumination conditions and for a wide range of voltages.}, language = {en} } @article{BartesaghiPerezKniepertetal.2015, author = {Bartesaghi, Davide and Perez, Irene del Carmen and Kniepert, Juliane and Roland, Steffen and Turbiez, Mathieu and Neher, Dieter and Koster, L. Jan Anton}, title = {Competition between recombination and extraction of free charges determines the fill factor of organic solar cells}, series = {Nature Communications}, volume = {6}, journal = {Nature Communications}, publisher = {Nature Publ. Group}, address = {London}, issn = {2041-1723}, doi = {10.1038/ncomms8083}, pages = {10}, year = {2015}, abstract = {Among the parameters that characterize a solar cell and define its power-conversion efficiency, the fill factor is the least well understood, making targeted improvements difficult. Here we quantify the competition between charge extraction and recombination by using a single parameter theta, and we demonstrate that this parameter is directly related to the fill factor of many different bulk-heterojunction solar cells. Our finding is supported by experimental measurements on 15 different donor: acceptor combinations, as well as by drift-diffusion simulations of organic solar cells in which charge-carrier mobilities, recombination rate, light intensity, energy levels and active-layer thickness are all varied over wide ranges to reproduce typical experimental conditions. The results unify the fill factors of several very different donor: acceptor combinations and give insight into why fill factors change so much with thickness, light intensity and materials properties. To achieve fill factors larger than 0.8 requires further improvements in charge transport while reducing recombination.}, language = {en} } @article{KniepertSchubertBlakesleyetal.2011, author = {Kniepert, Juliane and Schubert, Marcel and Blakesley, James C. and Neher, Dieter}, title = {Photogeneration and recombination in P3HT/PCBM solar cells probed by time-delayed collection field experiments}, series = {The journal of physical chemistry letters}, volume = {2}, journal = {The journal of physical chemistry letters}, number = {7}, publisher = {American Chemical Society}, address = {Washington}, issn = {1948-7185}, doi = {10.1021/jz200155b}, pages = {700 -- 705}, year = {2011}, abstract = {Time-delayed collection field (TDCF) experiments are performed on bulk heterojunction solar cells comprised of a blend of poly(3-hexylthiophene) and [6,6]-phenyl C-71 butyric acid methyl ester. TDCF is analogous to a pump-probe experiment using optical excitation and an electrical probe with a resolution of < 100 ns. The number of free charge carriers extracted after a short delay is found to be independent of the electric field during illumination. Also, experiments performed with a variable delay between the optical excitation and the electrical probe do not reveal any evidence for the generation of charge via field-assisted dissociation of bound long-lived polaron pairs. Photocurrent transients are well fitted by computational drift diffusion simulations with only direct generation of free charge carriers. With increasing delay times between pump and probe, two loss mechanisms are identified; first, charge-carriers are swept out of the device by the internal electric field, and second, bimolecular recombination of the remaining carriers takes place with a reduced recombination coefficient.}, language = {en} } @article{KniepertLangevanderKaapetal.2014, author = {Kniepert, Juliane and Lange, Ilja and van der Kaap, Niels J. and Koster, L. Jan Anton and Neher, Dieter}, title = {A conclusive view on charge generation, recombination, and extraction in As-prepared and annealed P3HT:PCBM blends: combined experimental and simulation work}, series = {dvanced energy materials}, volume = {4}, journal = {dvanced energy materials}, number = {7}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.201301401}, pages = {11}, year = {2014}, abstract = {Time-delayed collection field (TDCF) and bias-amplified charge extraction (BACE) are applied to as-prepared and annealed poly(3-hexylthiophene):[6,6]-phenyl C-71 butyric acid methyl ester (P3HT:PCBM) blends coated from chloroform. Despite large differences in fill factor, short-circuit current, and power conversion efficiency, both blends exhibit a negligible dependence of photogeneration on the electric field and strictly bimolecular recombination (BMR) with a weak dependence of the BMR coefficient on charge density. Drift-diffusion simulations are performed using the measured coefficients and mobilities, taking into account bimolecular recombination and the possible effects of surface recombination. The excellent agreement between the simulation and the experimental data for an intensity range covering two orders of magnitude indicates that a field-independent generation rate and a density-independent recombination coefficient describe the current-voltage characteristics of the annealed P3HT: PCBM devices, while the performance of the as-prepared blend is shown to be limited by space charge effects due to a low hole mobility. Finally, even though the bimolecular recombination coefficient is small, surface recombination is found to be a negligible loss mechanism in these solar cells.}, language = {en} }