@article{AlbrechtSchaeferLangeetal.2012, author = {Albrecht, Steve and Schaefer, Sebastian and Lange, Ilja and Yilmaz, Seyfullah and Dumsch, Ines and Allard, Sybille and Scherf, Ullrich and Hertwig, Andreas and Neher, Dieter}, title = {Light management in PCPDTBT:PC70BM solar cells: A comparison of standard and inverted device structures}, series = {Organic electronics : physics, materials and applications}, volume = {13}, journal = {Organic electronics : physics, materials and applications}, number = {4}, publisher = {Elsevier}, address = {Amsterdam}, issn = {1566-1199}, doi = {10.1016/j.orgel.2011.12.019}, pages = {615 -- 622}, year = {2012}, abstract = {We compare standard and inverted bulk heterojunction solar cells composed of PCPDTBT:PC70BM blends. Inverted devices comprising 100 nm thick active layers exhibited short circuit currents of 15 mA/cm(2), 10\% larger than in corresponding standard devices. Modeling of the optical field distribution in the different device stacks proved that this enhancement originates from an increased absorption of incident light in the active layer. Internal quantum efficiencies (IQEs) were obtained from the direct comparison of experimentally derived and modeled currents for different layer thicknesses, yielding IQEs of similar to 70\% for a layer thickness of 100 nm. Simulations predict a significant increase of the light harvesting efficiency upon increasing the layer thickness to 270 nm. However, a continuous deterioration of the photovoltaic properties with layer thickness was measured for both device architectures, attributed to incomplete charge extraction. On the other hand, our optical modeling suggests that inverted devices based on PCPDTBT should be able to deliver high power conversion efficiencies (PCEs) of more than 7\% provided that recombination losses can be reduced.}, language = {en} } @article{AlbrechtSchindlerKurpiersetal.2012, author = {Albrecht, Steve and Schindler, Wolfram and Kurpiers, Jona and Kniepert, Juliane and Blakesley, James C. and Dumsch, Ines and Allard, Sybille and Fostiropoulos, Konstantinos and Scherf, Ullrich and Neher, Dieter}, title = {On the field dependence of free charge carrier generation and recombination in blends of PCPDTBT/PC70BM influence of solvent additives}, series = {The journal of physical chemistry letters}, volume = {3}, journal = {The journal of physical chemistry letters}, number = {5}, publisher = {American Chemical Society}, address = {Washington}, issn = {1948-7185}, doi = {10.1021/jz3000849}, pages = {640 -- 645}, year = {2012}, abstract = {We have applied time-delayed collection field (TDCF) and charge extraction by linearly increasing voltage (CELIV) to investigate the photogeneration, transport, and recombination of charge carriers in blends composed of PCPDTBT/PC70BM processed with and without the solvent additive diiodooctane. The results suggest that the solvent additive has severe impacts on the elementary processes involved in the photon to collected electron conversion in these blends. First, a pronounced field dependence of the free carrier generation is found for both blends, where the field dependence is stronger without the additive. Second, the fate of charge carriers in both blends can be described with a rather high bimolecular recombination coefficients, which increase with decreasing internal field. Third, the mobility is three to four times higher with the additive. Both blends show a negative field dependence of mobility, which we suggest to cause bias-dependent recombination coefficients.}, 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{SchattauerReinholdAlbrechtetal.2012, author = {Schattauer, Sylvia and Reinhold, Beate and Albrecht, Steve and Fahrenson, Christoph and Schubert, Marcel and Janietz, Silvia and Neher, Dieter}, title = {Influence of sintering on the structural and electronic properties of TiO2 nanoporous layers prepared via a non-sol-gel approach}, series = {Colloid and polymer science : official journal of the Kolloid-Gesellschaft}, volume = {290}, journal = {Colloid and polymer science : official journal of the Kolloid-Gesellschaft}, number = {18}, publisher = {Springer}, address = {New York}, issn = {0303-402X}, doi = {10.1007/s00396-012-2708-9}, pages = {1843 -- 1854}, year = {2012}, abstract = {In this work, a nonaqueous method is used to fabricate thin TiO2 layers. In contrast to the common aqueous sol-gel approach, our method yields layers of anatase nanocrystallites already at low temperature. Raman spectroscopy, electron microscopy and charge extraction by linearly increasing voltage are employed to study the effect of sintering temperature on the structural and electronic properties of the nanocrystalline TiO2 layer. Raising the sintering temperature from 120 to 600 A degrees C is found to alter the chemical composition, the layer's porosity and its surface but not the crystal phase. The room temperature mobility increases from 2 x 10(-6) to 3 x 10(-5) cm(2)/Vs when the sinter temperature is increased from 400 to 600 A degrees C, which is explained by a better interparticle connectivity. Solar cells comprising such nanoporous TiO2 layers and a soluble derivative of cyclohexylamino-poly(p-phenylene vinylene) were fabricated and studied with regard to their structural and photovoltaic properties. We found only weak polymer infiltration into the oxide layer for sintering temperatures up to 550 A degrees C, while the polymer penetrated deeply into titania layers that were sintered at 600 A degrees C. Best photovoltaic performance was reached with a nanoporous TiO2 film sintered at 550 A degrees C, which yielded a power conversion efficiency of 0.5 \%. Noticeably, samples with the TiO2 layer dried at 120 A degrees C displayed short-circuit currents and open circuit voltages only about 15-20 \% lower than for the most efficient devices, meaning that our nonaqueous route yields titania layers with reasonable transport properties even at low sintering temperatures.}, language = {en} } @article{AlbrechtGrootoonkNeubertetal.2014, author = {Albrecht, Steve and Grootoonk, Bjorn and Neubert, Sebastian and Roland, Steffen and Wordenweber, Jan and Meier, Matthias and Schlatmann, Rutger and Gordijn, Aad and Neher, Dieter}, title = {Efficient hybrid inorganic/organic tandem solar cells with tailored recombination contacts}, series = {Solar energy materials \& solar cells : an international journal devoted to photovoltaic, photothermal, and photochemical solar energy conversion}, volume = {127}, journal = {Solar energy materials \& solar cells : an international journal devoted to photovoltaic, photothermal, and photochemical solar energy conversion}, publisher = {Elsevier}, address = {Amsterdam}, issn = {0927-0248}, doi = {10.1016/j.solmat.2014.04.020}, pages = {157 -- 162}, year = {2014}, abstract = {In this work, the authors present a 7.5\% efficient hybrid tandem solar cell with the bottom cell made of amorphous silicon and a Si-PCPDTBT:PC70BM bulk heterojunction top cell. Loss-free recombination contacts were realized by combing Al-doped ZnO with either the conducting polymer composite PEDOT:PSS or with a bilayer of ultrathin Al and MoO3. Optimization of these contacts results in tandem cells with high fill factors of 70\% and an open circuit voltage close to the sum of those of the sub-cells. This is the best efficiency reported for this type of hybrid tandem cell so far. Optical and electrical device modeling suggests that the efficiency can be increased to similar to 12\% on combining a donor polymer with suitable absorption onset with PCBM. We also describe proof-of-principle studies employing light trapping in hybrid tandem solar cells, suggesting that this device architecture has the potential to achieve efficiencies well above 12\%. (C) 2014 Elsevier B.V. All rights reserved.}, language = {en} } @article{AlbrechtVandewalTumblestonetal.2014, author = {Albrecht, Steve and Vandewal, Koen and Tumbleston, John R. and Fischer, Florian S. U. and Douglas, Jessica D. and Frechet, Jean M. J. and Ludwigs, Sabine and Ade, Harald W. and Salleo, Alberto and Neher, Dieter}, title = {On the efficiency of charge transfer state splitting in polymer: Fullerene solar cells}, series = {Advanced materials}, volume = {26}, journal = {Advanced materials}, number = {16}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {0935-9648}, doi = {10.1002/adma.201305283}, pages = {2533 -- 2539}, year = {2014}, language = {en} } @article{AlbrechtTumblestonJanietzetal.2014, author = {Albrecht, Steve and Tumbleston, John R. and Janietz, Silvia and Dumsch, Ines and Allard, Sybille and Scherf, Ullrich and Ade, Harald W. and Neher, Dieter}, title = {Quantifying charge extraction in organic solar cells: The case of fluorinated PCPDTBT}, series = {The journal of physical chemistry letters}, volume = {5}, journal = {The journal of physical chemistry letters}, number = {7}, publisher = {American Chemical Society}, address = {Washington}, issn = {1948-7185}, doi = {10.1021/jz500457b}, pages = {1131 -- 1138}, year = {2014}, abstract = {We introduce a new and simple method to quantify the effective extraction mobility in organic solar cells at low electric fields and charge carrier densities comparable to operation conditions under one sun illumination. By comparing steady-state carrier densities at constant illumination intensity and under open-circuit conditions, the gradient of the quasi-Fermi potential driving the current is estimated as a function of external bias and charge density. These properties are then related to the respective steady-state current to determine the effective extraction mobility. The new technique is applied to different derivatives of the well-known low-band-gap polymer PCPDTBT blended with PC70BM. We show that the slower average extraction due to lower mobility accounts for the moderate fill factor when solar cells are fabricated with mono- or difluorinated PCPDTBT. This lower extraction competes with improved generation and reduced nongeminate recombination, rendering the monofluorinated derivative the most efficient donor polymer.}, language = {en} } @article{PradhanAlbrechtStilleretal.2014, author = {Pradhan, Basudev and Albrecht, Steve and Stiller, Burkhard and Neher, Dieter}, title = {Inverted organic solar cells comprising low-temperature-processed ZnO films}, series = {Applied physics : A, Materials science \& processing}, volume = {115}, journal = {Applied physics : A, Materials science \& processing}, number = {2}, publisher = {Springer}, address = {New York}, issn = {0947-8396}, doi = {10.1007/s00339-014-8373-8}, pages = {365 -- 369}, year = {2014}, abstract = {Inverted organic solar cells are fabricated using low-temperature-annealed ZnO film as an electron transport layer. Uniform ZnO films were prepared by spin coating a diethylzinc (DEZ) precursor solution in air, followed by annealing at 100 A degrees C. Organic solar cells prepared on these ZnO films with a 1:1 P3HT:PCBM blend as the active layer show a high power conversion efficiency of 4.03 \%, which is more than 10 \% higher than the PCE of solar cells comprising ZnO prepared via a high-temperature sol-gel route.}, language = {en} } @article{VandewalAlbrechtHokeetal.2014, author = {Vandewal, Koen and Albrecht, Steve and Hoke, Eric T. and Graham, Kenneth R. and Widmer, Johannes and Douglas, Jessica D. and Schubert, Marcel and Mateker, William R. and Bloking, Jason T. and Burkhard, George F. and Sellinger, Alan and Frechet, Jean M. J. and Amassian, Aram and Riede, Moritz K. and McGehee, Michael D. and Neher, Dieter and Salleo, Alberto}, title = {Efficient charge generation by relaxed charge-transfer states at organic interfaces}, series = {Nature materials}, volume = {13}, journal = {Nature materials}, number = {1}, publisher = {Nature Publ. Group}, address = {London}, issn = {1476-1122}, doi = {10.1038/NMAT3807}, pages = {63 -- 68}, year = {2014}, abstract = {carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold viaweakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer: fullerene, small-molecule:C-60 and polymer: polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90\% without the need for excess electronic or vibrational energy.}, language = {en} } @phdthesis{Albrecht2014, author = {Albrecht, Steve}, title = {Generation, recombination and extraction of charges in polymer}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-72285}, school = {Universit{\"a}t Potsdam}, pages = {144}, year = {2014}, abstract = {A dramatic efficiency improvement of bulk heterojunction solar cells based on electron-donating conjugated polymers in combination with soluble fullerene derivatives has been achieved over the past years. Certified and reported power conversion efficiencies now reach over 9\% for single junctions and exceed the 10\% benchmark for tandem solar cells. This trend brightens the vision of organic photovoltaics becoming competitive with inorganic solar cells including the realization of low-cost and large-area organic photovoltaics. For the best performing organic materials systems, the yield of charge generation can be very efficient. However, a detailed understanding of the free charge carrier generation mechanisms at the donor acceptor interface and the energy loss associated with it needs to be established. Moreover, organic solar cells are limited by the competition between charge extraction and free charge recombination, accounting for further efficiency losses. A conclusive picture and the development of precise methodologies for investigating the fundamental processes in organic solar cells are crucial for future material design, efficiency optimization, and the implementation of organic solar cells into commercial products. In order to advance the development of organic photovoltaics, my thesis focuses on the comprehensive understanding of charge generation, recombination and extraction in organic bulk heterojunction solar cells summarized in 6 chapters on the cumulative basis of 7 individual publications. The general motivation guiding this work was the realization of an efficient hybrid inorganic/organic tandem solar cell with sub-cells made from amorphous hydrogenated silicon and organic bulk heterojunctions. To realize this project aim, the focus was directed to the low band-gap copolymer PCPDTBT and its derivatives, resulting in the examination of the charge carrier dynamics in PCPDTBT:PC70BM blends in relation to by the blend morphology. The phase separation in this blend can be controlled by the processing additive diiodooctane, enhancing domain purity and size. The quantitative investigation of the free charge formation was realized by utilizing and improving the time delayed collection field technique. Interestingly, a pronounced field dependence of the free carrier generation for all blends is found, with the field dependence being stronger without the additive. Also, the bimolecular recombination coefficient for both blends is rather high and increases with decreasing internal field which we suggest to be caused by a negative field dependence of mobility. The additive speeds up charge extraction which is rationalized by the threefold increase in mobility. By fluorine attachment within the electron deficient subunit of PCPDTBT, a new polymer F-PCPDTBT is designed. This new material is characterized by a stronger tendency to aggregate as compared to non-fluorinated PCPDTBT. Our measurements show that for F-PCPDTBT:PCBM blends the charge carrier generation becomes more efficient and the field-dependence of free charge carrier generation is weakened. The stronger tendency to aggregate induced by the fluorination also leads to increased polymer rich domains, accompanied in a threefold reduction in the non-geminate recombination coefficient at conditions of open circuit. The size of the polymer domains is nicely correlated to the field-dependence of charge generation and the Langevin reduction factor, which highlights the importance of the domain size and domain purity for efficient charge carrier generation. In total, fluorination of PCPDTBT causes the PCE to increase from 3.6 to 6.1\% due to enhanced fill factor, short circuit current and open circuit voltage. Further optimization of the blend ratio, active layer thickness, and polymer molecular weight resulted in 6.6\% efficiency for F-PCPDTBT:PC70BM solar cells. Interestingly, the double fluorinated version 2F-PCPDTBT exhibited poorer FF despite a further reduction of geminate and non-geminate recombination losses. To further analyze this finding, a new technique is developed that measures the effective extraction mobility under charge carrier densities and electrical fields comparable to solar cell operation conditions. This method involves the bias enhanced charge extraction technique. With the knowledge of the carrier density under different electrical field and illumination conditions, a conclusive picture of the changes in charge carrier dynamics leading to differences in the fill factor upon fluorination of PCPDTBT is attained. The more efficient charge generation and reduced recombination with fluorination is counterbalanced by a decreased extraction mobility. Thus, the highest fill factor of 60\% and efficiency of 6.6\% is reached for F-PCPDTBT blends, while 2F-PCPDTBT blends have only moderate fill factors of 54\% caused by the lower effective extraction mobility, limiting the efficiency to 6.5\%. To understand the details of the charge generation mechanism and the related losses, we evaluated the yield and field-dependence of free charge generation using time delayed collection field in combination with sensitive measurements of the external quantum efficiency and absorption coefficients for a variety of blends. Importantly, both the yield and field-dependence of free charge generation is found to be unaffected by excitation energy, including direct charge transfer excitation below the optical band gap. To access the non-detectable absorption at energies of the relaxed charge transfer emission, the absorption was reconstructed from the CT emission, induced via the recombination of thermalized charges in electroluminescence. For a variety of blends, the quantum yield at energies of charge transfer emission was identical to excitations with energies well above the optical band-gap. Thus, the generation proceeds via the split-up of the thermalized charge transfer states in working solar cells. Further measurements were conducted on blends with fine-tuned energy levels and similar blend morphologies by using different fullerene derivatives. A direct correlation between the efficiency of free carrier generation and the energy difference of the relaxed charge transfer state relative to the energy of the charge separated state is found. These findings open up new guidelines for future material design as new high efficiency materials require a minimum energetic offset between charge transfer and the charge separated state while keeping the HOMO level (and LUMO level) difference between donor and acceptor as small as possible.}, language = {en} }