@article{SchubertDolfenFrischetal.2012,
  author    = {Schubert, Marcel and Dolfen, Daniel and Frisch, Johannes and Roland, Steffen and Steyrleuthner, Robert and Stiller, Burkhard and Chen, Zhihua and Scherf, Ullrich and Koch, Norbert and Facchetti, Antonio and Neher, Dieter},
  title     = {Influence of aggregation on the performance of All-Polymer Solar Cells containing Low-Bandgap Naphthalenediimide Copolymers},
  series = {dvanced energy materials},
  volume    = {2},
  journal   = {dvanced energy materials},
  number    = {3},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {1614-6832},
  doi       = {10.1002/aenm.201100601},
  pages     = {369 -- 380},
  year      = {2012},
  abstract  = {The authors present efficient all-polymer solar cells comprising two different low-bandgap naphthalenediimide (NDI)-based copolymers as acceptors and regioregular P3HT as the donor. It is shown that these naphthalene copolymers have a strong tendency to preaggregate in specific organic solvents, and that preaggregation can be completely suppressed when using suitable solvents with large and highly polarizable aromatic cores. Organic solar cells prepared from such nonaggregated polymer solutions show dramatically increased power conversion efficiencies of up to 1.4\%, which is mainly due to a large increase of the short circuit current. In addition, optimized solar cells show remarkable high fill factors of up to 70\%. The analysis of the blend absorbance spectra reveals a surprising anticorrelation between the degree of polymer aggregation in the solid P3HT:NDI copolymer blends and their photovoltaic performance. Scanning near-field optical microscopy (SNOM) and atomic force microscopy (AFM) measurements reveal important information on the blend morphology. It is shown that films with high degree of aggregation and low photocurrents exhibit large-scale phase-separation into rather pure donor and acceptor domains. It is proposed that, by suppressing the aggregation of NDI copolymers at the early stage of film formation, the intermixing of the donor and acceptor component is improved, thereby allowing efficient harvesting of photogenerated excitons at the donoracceptor heterojunction.},
  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{SchubertCollinsMangoldetal.2014,
  author    = {Schubert, Marcel and Collins, Brian A. and Mangold, Hannah and Howard, Ian A. and Schindler, Wolfram and Vandewal, Koen and Roland, Steffen and Behrends, Jan and Kraffert, Felix and Steyrleuthner, Robert and Chen, Zhihua and Fostiropoulos, Konstantinos and Bittl, Robert and Salleo, Alberto and Facchetti, Antonio and Laquai, Frederic and Ade, Harald W. and Neher, Dieter},
  title     = {Correlated donor/acceptor crystal orientation controls photocurrent generation in all-polymer solar cells},
  series = {Advanced functional materials},
  volume    = {24},
  journal   = {Advanced functional materials},
  number    = {26},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {1616-301X},
  doi       = {10.1002/adfm.201304216},
  pages     = {4068 -- 4081},
  year      = {2014},
  abstract  = {New polymers with high electron mobilities have spurred research in organic solar cells using polymeric rather than fullerene acceptors due to their potential of increased diversity, stability, and scalability. However, all-polymer solar cells have struggled to keep up with the steadily increasing power conversion efficiency of polymer: fullerene cells. The lack of knowledge about the dominant recombination process as well as the missing concluding picture on the role of the semi-crystalline microstructure of conjugated polymers in the free charge carrier generation process impede a systematic optimization of all-polymer solar cells. These issues are examined by combining structural and photo-physical characterization on a series of poly(3-hexylthiophene) (donor) and P(NDI2OD-T2) (acceptor) blend devices. These experiments reveal that geminate recombination is the major loss channel for photo-excited charge carriers. Advanced X-ray and electron-based studies reveal the effect of chloronaphthalene co-solvent in reducing domain size, altering domain purity, and reorienting the acceptor polymer crystals to be coincident with those of the donor. This reorientation correlates well with the increased photocurrent from these devices. Thus, effi cient split-up of geminate pairs at polymer/polymer interfaces may necessitate correlated donor/acceptor crystal orientation, which represents an additional requirement compared to the isotropic fullerene acceptors.},
  language  = {en}
}
@article{LiAbrechtYangetal.2014,
  author    = {Li, Wentao and Abrecht, Steve and Yang, Liqiang and Roland, Steffen and Tumbleston, John R. and McAfee, Terry and Yan, Liang and Kelly, Mary Allison and Ade, Harald W. and Neher, Dieter and You, Wei},
  title     = {Mobility-controlled performance of thick solar cells based on fluorinated copolymers},
  series = {Journal of the American Chemical Society},
  volume    = {136},
  journal   = {Journal of the American Chemical Society},
  number    = {44},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {0002-7863},
  doi       = {10.1021/ja5067724},
  pages     = {15566 -- 15576},
  year      = {2014},
  abstract  = {Developing novel materials and device architectures to further enhance the efficiency of polymer solar cells requires a fundamental understanding of the impact of chemical structures on photovoltaic properties. Given that device characteristics depend on many parameters, deriving structureproperty relationships has been very challenging. Here we report that a single parameter, hole mobility, determines the fill factor of several hundred nanometer thick bulk heterojunction photovoltaic devices based on a series of copolymers with varying amount of fluorine substitution. We attribute the steady increase of hole mobility with fluorine content to changes in polymer molecular ordering. Importantly, all other parameters, including the efficiency of free charge generation and the coefficient of nongeminate recombination, are nearly identical. Our work emphasizes the need to achieve high mobility in combination with strongly suppressed charge recombination for the thick devices required by mass production technologies.},
  language  = {en}
}
@article{GehrigRolandHowardetal.2014,
  author    = {Gehrig, Dominik W. and Roland, Steffen and Howard, Ian A. and Kamm, Valentin and Mangold, Hannah and Neher, Dieter and Laquai, Frederic},
  title     = {Efficiency-limiting processes in low-bandgap polymer:Perylene diimide photovoltaic blends},
  series = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  volume    = {118},
  journal   = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  number    = {35},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1932-7447},
  doi       = {10.1021/jp503366m},
  pages     = {20077 -- 20085},
  year      = {2014},
  abstract  = {The charge generation and recombination processes following photo-excitation of a low-bandgap polymer:perylene diimide photovoltaic blend are investigated by transient absorption pump-probe spectroscopy covering a dynamic range from femto-to microseconds to get insight into the efficiency-limiting photophysical processes. The several tens of picoseconds, and its efficiency is only half of that in a polymer:fullerene photoinduced electron transfer from the polymer to the perylene acceptor takes up to blend. This reduces the short-circuit current. Time-delayed collection field experiments reveal that the subsequent charge separation is strongly field-dependent, limiting the fill factor and lowering the short-circuit current in polymer:PDI devices. Upon excitation of the acceptor in the low-bandgap polymer blend, the PDI exciton undergoes charge transfer on a time scale of several tens of picoseconds. However, a significant fraction of the charges generated at the interface are quickly lost because of fast geminate recombination. This reduces the short-circuit current even further, leading to a scenario in which only around 2596 of the initial photoexcitations generate free charges that can potentially contribute to the photocurrent. In summary, the key photophysical limitations of perylene diimide as an acceptor in low-bandgap polymer blends appear at the interface between the materials, with the kinetics of both charge generation and separation inhibited as compared to that of fullerenes.},
  language  = {en}
}
@article{RolandSchubertCollinsetal.2014,
  author    = {Roland, Steffen and Schubert, Marcel and Collins, Brian A. and Kurpiers, Jona and Chen, Zhihua and Facchetti, Antonio and Ade, Harald W. and Neher, Dieter},
  title     = {Fullerene-free polymer solar cells with highly reduced bimolecular recombination and field-independent charge carrier generation},
  series = {The journal of physical chemistry letters},
  volume    = {5},
  journal   = {The journal of physical chemistry letters},
  number    = {16},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1948-7185},
  doi       = {10.1021/jz501506z},
  pages     = {2815 -- 2822},
  year      = {2014},
  abstract  = {Photogeneration, recombination, and transport of free charge carriers in all-polymer bulk heterojunction solar cells incorporating poly(3-hexylthiophene) (P3HT) as donor and poly([N,N'-bis(2-octyldodecyl)-naphthelene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'-(2,2'-bithiophene)) (P(NDI2OD-T2)) as acceptor polymer have been investigated by the use of time delayed collection field (TDCF) and time-of-flight (TOF) measurements. Depending on the preparation procedure used to dry the active layers, these solar cells comprise high fill factors (FFs) of up to 67\%. A strongly reduced bimolecular recombination (BMR), as well as a field-independent free charge carrier generation are observed, features that are common to high performance fullerene-based solar cells. Resonant soft X-ray measurements (R-SoXS) and photoluminescence quenching experiments (PQE) reveal that the BMR is related to domain purity. Our results elucidate the similarities of this polymeric acceptor with the superior recombination properties of fullerene acceptors.},
  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{RolandNeubertAlbrechtetal.2015,
  author    = {Roland, Steffen and Neubert, Sebastian and Albrecht, Steve and Stannowski, Bernd and Seger, Mark and Facchetti, Antonio and Schlatmann, Rutger and Rech, Bernd and Neher, Dieter},
  title     = {Hybrid Organic/Inorganic Thin-Film Multijunction Solar Cells Exceeding 11\% Power Conversion Efficiency},
  series = {Advanced materials},
  volume    = {27},
  journal   = {Advanced materials},
  number    = {7},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {0935-9648},
  doi       = {10.1002/adma.201404698},
  pages     = {1262 -- 1267},
  year      = {2015},
  abstract  = {Hybrid multijunction solar cells comprising hydrogenated amorphous silicon and an organic bulk heterojunction are presented, reaching 11.7\% power conversion efficiency. The benefits of merging inorganic and organic subcells are pointed out, the optimization of the cells, including optical modeling predictions and tuning of the recombination contact are described, and an outlook of this technique is given.},
  language  = {en}
}
@phdthesis{Roland2017,
  author    = {Roland, Steffen},
  title     = {Charge carrier recombination and open circuit voltage in organic solar cells},
  url       = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-397721},
  school      = {Universit{\"a}t Potsdam},
  pages     = {VI, 145},
  year      = {2017},
  abstract  = {Tremendous progress in the development of thin film solar cell techniques has been made over the last decade. The field of organic solar cells is constantly developing, new material classes like Perowskite solar cells are emerging and different types of hybrid organic/inorganic material combinations are being investigated for their physical properties and their applicability in thin film electronics. Besides typical single-junction architectures for solar cells, multi-junction concepts are also being investigated as they enable the overcoming of theoretical limitations of a single-junction. In multi-junction devices each sub-cell operates in different wavelength regimes and should exhibit optimized band-gap energies. It is exactly this tunability of the band-gap energy that renders organic solar cell materials interesting candidates for multi-junction applications. Nevertheless, only few attempts have been made to combine inorganic and organic solar cells in series connected multi-junction architectures. Even though a great diversity of organic solar cells exists nowadays, their open circuit voltage is usually low compared to the band-gap of the active layer. Hence, organic low band-gap solar cells in particular show low open circuit voltages and the key factors that determine the voltage losses are not yet fully understood. Besides open circuit voltage losses the recombination of charges in organic solar cells is also a prevailing research topic, especially with respect to the influence of trap states. The exploratory focus of this work is therefore set, on the one hand, on the development of hybrid organic/inorganic multi-junctions and, on the other hand, on gaining a deeper understanding of the open circuit voltage and the recombination processes of organic solar cells. In the first part of this thesis, the development of a hybrid organic/inorganic triple-junction will be discussed which showed at that time (Jan. 2015) a record power conversion efficiency of 11.7\%. The inorganic sub-cells of these devices consist of hydrogenated amorphous silicon and were delivered by the Competence Center Thin-Film and Nanotechnology for Photovoltaics in Berlin. Different recombination contacts and organic sub-cells were tested in conjunction with these inorganic sub-cells on the basis of optical modeling predictions for the optimal layer thicknesses to finally reach record efficiencies for this type of solar cells. In the second part, organic model systems will be investigated to gain a better understanding of the fundamental loss mechanisms that limit the open circuit voltage of organic solar cells. First, bilayer systems with different orientation of the donor and acceptor molecules were investigated to study the influence of the donor/acceptor orientation on non-radiative voltage loss. Secondly, three different bulk heterojunction solar cells all comprising the same amount of fluorination and the same polymer backbone in the donor component were examined to study the influence of long range electrostatics on the open circuit voltage. Thirdly, the device performance of two bulk heterojunction solar cells was compared which consisted of the same donor polymer but used different fullerene acceptor molecules. By this means, the influence of changing the energetics of the acceptor component on the open circuit voltage was investigated and a full analysis of the charge carrier dynamics was presented to unravel the reasons for the worse performance of the solar cell with the higher open circuit voltage. In the third part, a new recombination model for organic solar cells will be introduced and its applicability shown for a typical low band-gap cell. This model sheds new light on the recombination process in organic solar cells in a broader context as it re-evaluates the recombination pathway of charge carriers in devices which show the presence of trap states. Thereby it addresses a current research topic and helps to resolve alleged discrepancies which can arise from the interpretation of data derived by different measurement techniques.},
  language  = {en}
}
@article{KellyRolandZhangetal.2017,
  author    = {Kelly, Mary Allison and Roland, Steffen and Zhang, Qianqian and Lee, Youngmin and Kabius, Bernd and Wang, Qing and Gomez, Enrique D. and Neher, Dieter and You, Wei},
  title     = {Incorporating Fluorine Substitution into Conjugated Polymers for Solar Cells},
  series = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  volume    = {121},
  journal   = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  number    = {4},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1932-7447},
  doi       = {10.1021/acs.jpcc.6b10993},
  pages     = {2059 -- 2068},
  year      = {2017},
  abstract  = {Fluorinating conjugated polymers is a proven strategy for creating high performance materials in polymer solar cells, yet few studies have investigated the importance of the fluorination method. We compare the performance of three fluorinated systems: a poly(benzodithieno-dithienyltriazole) (PBnDT-XTAZ) random copolymer where 50\% of the acceptor units are difluorinated, PBnDT-mFTAZ where every acceptor unit is monofluorinated, and a 1:1 physical blend of the difluorinated and nonfluorinated polymer. All systems have the same degree of fluorination (50\%) yet via different methods (chemically vs physically, random vs regular). We show that these three systems have equivalent photovoltaic behavior:,similar to 5.2\% efficiency with a short-circuit current (J(sc)) at,similar to 11 mA cm(-2), an open-circuit voltage (v(oc)) at 0.77 V, and a fill factor (FF) of similar to 60\%. Further investigation of these three systems demonstrates that the charge generation, charge extraction, and charge transfer state are essentially identical for the three studied systems. Transmission electron microscopy shows no significant differences in the morphologies. All these data illustrate that it is possible to improve performance not only via regular or random fluorination but also by physical addition via a ternary blend. Thus, our results demonstrate the versatility of incorporating fluorine in the active layer of polymer solar cells to enhance device performance.},
  language  = {en}
}
@article{RolandYanZhangetal.2017,
  author    = {Roland, Steffen and Yan, Liang and Zhang, Qianqian and Jiao, Xuechen and Hunt, Adrian and Ghasemi, Masoud and Ade, Harald and You, Wei and Neher, Dieter},
  title     = {Charge Generation and Mobility-Limited Performance of Bulk Heterojunction Solar Cells with a Higher Adduct Fullerene},
  series = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  volume    = {121},
  journal   = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1932-7447},
  doi       = {10.1021/acs.jpcc.7b02288},
  pages     = {10305 -- 10316},
  year      = {2017},
  abstract  = {Alternative electron acceptors are being actively explored in order to advance the development of bulk-heterojunction (BHJ) organic solar cells (OSCs). The indene-C-60 bisadduct (ICBA) has been regarded as a promising candidate, as it provides high open-circuit voltage in BHJ solar cells; however, the photovoltaic performance of such ICBA-based devices is often inferior when compared to cells with the omnipresent PCBM electron acceptor. Here, by pairing the high performance polymer (FTAZ) as the donor with either PCBM or ICBA as the acceptor, we explore the physical mechanism behind the reduced performance of the ICBA-based device. Time delayed collection field (TDCF) experiments reveal reduced, yet field-independent free charge generation in the FTAZ:ICBA system, explaining the overall lower photocurrent in its cells. Through the analysis of the photoluminescence, photogeneration, and electroluminescence, we find that the lower generation efficiency is neither caused by inefficient exciton splitting, nor do we find evidence for significant energy back-transfer from the CT state to singlet excitons. In fact, the increase in open circuit voltage when replacing PCBM by ICBA is entirely caused by the increase in the CT energy, related to the shift in the LUMO energy, while changes in the radiative and nonradiative recombination losses are nearly absent. On the other hand, space charge limited current (SCLC) and bias-assisted charge extraction (BACE) measurements consistently reveal a severely lower electron mobilitiy in the FTAZ:ICBA blend. Studies of the blends with resonant soft X-ray scattering (R-SoXS), grazing incident wide-angle X-ray scattering (GIWAXS), and scanning transmission X-ray microscopy (STXM) reveal very little differences in the mesoscopic morphology but significantly less nanoscale molecular ordering of the fullerene domains in the ICBA based blends, which we propose as the main cause for the lower generation efficiency and smaller electron mobility. Calculations of the JV curves with an analytical model, using measured values, show good agreement with the experimentally determined JV characteristics, proving that these devices suffer from slow carrier extraction, resulting in significant bimolecular recombination losses. Therefore, this study highlights the importance of high charge carrier mobility for newly synthesized acceptor materials, in addition to having suitable energy levels.},
  language  = {en}
}
@article{RanRolandLoveetal.2017,
  author    = {Ran, Niva A. and Roland, Steffen and Love, John A. and Savikhin, Victoria and Takacs, Christopher J. and Fu, Yao-Tsung and Li, Hong and Coropceanu, Veaceslav and Liu, Xiaofeng and Bredas, Jean-Luc and Bazan, Guillermo C. and Toney, Michael F. and Neher, Dieter and Thuc-Quyen Nguyen,},
  title     = {Impact of interfacial molecular orientation on radiative recombination and charge generation efficiency},
  series = {Nature Communications},
  volume    = {8},
  journal   = {Nature Communications},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {2041-1723},
  doi       = {10.1038/s41467-017-00107-4},
  pages     = {9},
  year      = {2017},
  abstract  = {A long standing question in organic electronics concerns the effects of molecular orientation at donor/acceptor heterojunctions. Given a well-controlled donor/acceptor bilayer system, we uncover the genuine effects of molecular orientation on charge generation and recombination. These effects are studied through the point of view of photovoltaics-however, the results have important implications on the operation of all optoelectronic devices with donor/ acceptor interfaces, such as light emitting diodes and photodetectors. Our findings can be summarized by two points. First, devices with donor molecules face-on to the acceptor interface have a higher charge transfer state energy and less non-radiative recombination, resulting in larger open-circuit voltages and higher radiative efficiencies. Second, devices with donor molecules edge-on to the acceptor interface are more efficient at charge generation, attributed to smaller electronic coupling between the charge transfer states and the ground state, and lower activation energy for charge generation.},
  language  = {en}
}
@article{SiniSchubertRiskoetal.2018,
  author    = {Sini, Gjergji and Schubert, Marcel and Risko, Chad and Roland, Steffen and Lee, Olivia P. and Chen, Zhihua and Richter, Thomas V. and Dolfen, Daniel and Coropceanu, Veaceslav and Ludwigs, Sabine and Scherf, Ullrich and Facchetti, Antonio and Frechet, Jean M. J. and Neher, Dieter},
  title     = {On the Molecular Origin of Charge Separation at the Donor-Acceptor Interface},
  series = {Advanced energy materials},
  volume    = {8},
  journal   = {Advanced energy materials},
  number    = {12},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {1614-6832},
  doi       = {10.1002/aenm.201702232},
  pages     = {15},
  year      = {2018},
  abstract  = {Fullerene-based acceptors have dominated organic solar cells for almost two decades. It is only within the last few years that alternative acceptors rival their dominance, introducing much more flexibility in the optoelectronic properties of these material blends. However, a fundamental physical understanding of the processes that drive charge separation at organic heterojunctions is still missing, but urgently needed to direct further material improvements. Here a combined experimental and theoretical approach is used to understand the intimate mechanisms by which molecular structure contributes to exciton dissociation, charge separation, and charge recombination at the donor-acceptor (D-A) interface. Model systems comprised of polythiophene-based donor and rylene diimide-based acceptor polymers are used and a detailed density functional theory (DFT) investigation is performed. The results point to the roles that geometric deformations and direct-contact intermolecular polarization play in establishing a driving force ( energy gradient) for the optoelectronic processes taking place at the interface. A substantial impact for this driving force is found to stem from polymer deformations at the interface, a finding that can clearly lead to new design approaches in the development of the next generation of conjugated polymers and small molecules.},
  language  = {en}
}
@article{KurpiersFerronRolandetal.2018,
  author    = {Kurpiers, Jona and Ferron, Thomas and Roland, Steffen and Jakoby, Marius and Thiede, Tobias and Jaiser, Frank and Albrecht, Steve and Janietz, Silvia and Collins, Brian A. and Howard, Ian A. and Neher, Dieter},
  title     = {Probing the pathways of free charge generation in organic bulk heterojunction solar cells},
  series = {Nature Communications},
  volume    = {9},
  journal   = {Nature Communications},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {2041-1723},
  doi       = {10.1038/s41467-018-04386-3},
  pages     = {11},
  year      = {2018},
  abstract  = {The fact that organic solar cells perform efficiently despite the low dielectric constant of most photoactive blends initiated a long-standing debate regarding the dominant pathways of free charge formation. Here, we address this issue through the accurate measurement of the activation energy for free charge photogeneration over a wide range of photon energy, using the method of time-delayed collection field. For our prototypical low bandgap polymer:fullerene blends, we find that neither the temperature nor the field dependence of free charge generation depend on the excitation energy, ruling out an appreciable contribution to free charge generation though hot carrier pathways. On the other hand, activation energies are on the order of the room temperature thermal energy for all studied blends. We conclude that charge generation in such devices proceeds through thermalized charge transfer states, and that thermal energy is sufficient to separate most of these states into free charges.},
  language  = {en}
}
@article{HosseiniRolandKurpiersetal.2019,
  author    = {Hosseini, Seyed Mehrdad and Roland, Steffen and Kurpiers, Jona and Chen, Zhiming and Zhang, Kai and Huang, Fei and Armin, Ardalan and Neher, Dieter and Shoaee, Safa},
  title     = {Impact of Bimolecular Recombination on the Fill Factor of Fullerene and Nonfullerene-Based Solar Cells},
  series = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  volume    = {123},
  journal   = {The journal of physical chemistry : C, Nanomaterials and interfaces},
  number    = {11},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1932-7447},
  doi       = {10.1021/acs.jpcc.8b11669},
  pages     = {6823 -- 6830},
  year      = {2019},
  abstract  = {Power conversion efficiencies of donor/acceptor organic solar cells utilizing nonfullerene acceptors have now increased beyond the record of their fullerene-based counterparts. There remain many fundamental questions regarding nanomorphology, interfacial states, charge generation and extraction, and losses in these systems. Herein, we present a comparative study of bulk heterojunction solar cells composed of a recently introduced naphthothiadiazole-based polymer (NT812) as the electron donor and two different acceptor molecules, namely, [6,6]-phenyl-C71-butyric acid methyl ester (PCBM)[70] and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC). A comparison between the photovoltaic performance of these two types of solar cells reveals that the open-circuit voltage (Voc) of the NT812:ITIC-based solar cell is larger, but the fill factor (FF) is lower than that of the NT812:PCBM[70] device. We find the key reason behind this reduced FF in the ITIC-based device to be faster nongeminate recombination relative to the NT812:PCBM[70] system.},
  language  = {en}
}
@article{RolandKniepertLoveetal.2019,
  author    = {Roland, Steffen and Kniepert, Juliane and Love, John A. and Negi, Vikas and Liu, Feilong and Bobbert, Peter and Melianas, Armantas and Kemerink, Martijn and Hofacker, Andreas and Neher, Dieter},
  title     = {Equilibrated Charge Carrier Populations Govern Steady-State Nongeminate Recombination in Disordered Organic Solar Cells},
  series = {The journal of physical chemistry letters},
  volume    = {10},
  journal   = {The journal of physical chemistry letters},
  number    = {6},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1948-7185},
  doi       = {10.1021/acs.jpclett.9b00516},
  pages     = {1374 -- 1381},
  year      = {2019},
  abstract  = {We employed bias-assisted charge extraction techniques to investigate the transient and steady-state recombination of photogenerated charge carriers in complete devices of a disordered polymer-fullerene blend. Charge recombination is shown to be dispersive, with a significant slowdown of the recombination rate over time, consistent with the results from kinetic Monte Carlo simulations. Surprisingly, our experiments reveal little to no contributions from early time recombination of nonequilibrated charge carriers to the steady-state recombination properties. We conclude that energetic relaxation of photogenerated carriers outpaces any significant nongeminate recombination under application-relevant illumination conditions. With equilibrated charges dominating the steady-state recombination, quasi-equilibrium concepts appear suited for describing the open-circuit voltage of organic solar cells despite pronounced energetic disorder.},
  language  = {en}
}
@article{SchwarzeSchellhammerOrtsteinetal.2019,
  author    = {Schwarze, Martin and Schellhammer, Karl Sebastian and Ortstein, Katrin and Benduhn, Johannes and Gaul, Christopher and Hinderhofer, Alexander and Perdigon-Toro, Lorena and Scholz, Reinhard and Kublitski, Jonas and Roland, Steffen and Lau, Matthias and Poelking, Carl and Andrienko, Denis and Cuniberti, Gianaurelio and Schreiber, Frank and Neher, Dieter and Vandewal, Koen and Ortmann, Frank and Leo, Karl},
  title     = {Impact of molecular quadrupole moments on the energy levels at organic heterojunctions},
  series = {Nature Communications},
  volume    = {10},
  journal   = {Nature Communications},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {2041-1723},
  doi       = {10.1038/s41467-019-10435-2},
  pages     = {9},
  year      = {2019},
  abstract  = {The functionality of organic semiconductor devices crucially depends on molecular energies, namely the ionisation energy and the electron affinity. Ionisation energy and electron affinity values of thin films are, however, sensitive to film morphology and composition, making their prediction challenging. In a combined experimental and simulation study on zinc-phthalocyanine and its fluorinated derivatives, we show that changes in ionisation energy as a function of molecular orientation in neat films or mixing ratio in blends are proportional to the molecular quadrupole component along the p-p-stacking direction. We apply these findings to organic solar cells and demonstrate how the electrostatic interactions can be tuned to optimise the energy of the charge-transfer state at the donor-acceptor interface and the dissociation barrier for free charge carrier generation. The confirmation of the correlation between interfacial energies and quadrupole moments for other materials indicates its relevance for small molecules and polymers.},
  language  = {en}
}
@article{UllbrichBenduhnJiaetal.2019,
  author    = {Ullbrich, Sascha and Benduhn, Johannes and Jia, Xiangkun and Nikolis, Vasileios C. and Tvingstedt, Kristofer and Piersimoni, Fortunato and Roland, Steffen and Liu, Yuan and Wu, Jinhan and Fischer, Axel and Neher, Dieter and Reineke, Sebastian and Spoltore, Donato and Vandewal, Koen},
  title     = {Emissive and charge-generating donor-acceptor interfaces for organic optoelectronics with low voltage losses},
  series = {Nature materials},
  volume    = {18},
  journal   = {Nature materials},
  number    = {5},
  publisher = {Nature Publ. Group},
  address   = {London},
  issn      = {1476-1122},
  doi       = {10.1038/s41563-019-0324-5},
  pages     = {459 -- 464},
  year      = {2019},
  abstract  = {Intermolecular charge-transfer states at the interface between electron donating (D) and accepting (A) materials are crucial for the operation of organic solar cells but can also be exploited for organic light-emitting diodes(1,2). Non-radiative charge-transfer state decay is dominant in state-of-the-art D-A-based organic solar cells and is responsible for large voltage losses and relatively low power-conversion efficiencies as well as electroluminescence external quantum yields in the 0.01-0.0001\% range(3,4). In contrast, the electroluminescence external quantum yield reaches up to 16\% in D-A-based organic light-emitting diodes(5-7). Here, we show that proper control of charge-transfer state properties allows simultaneous occurrence of a high photovoltaic and emission quantum yield within a single, visible-light-emitting D-A system. This leads to ultralow-emission turn-on voltages as well as significantly reduced voltage losses upon solar illumination. These results unify the description of the electro-optical properties of charge-transfer states in organic optoelectronic devices and foster the use of organic D-A blends in energy conversion applications involving visible and ultraviolet photons(8-11).},
  language  = {en}
}
@article{PoelkingBenduhnSpoltoreetal.2022,
  author    = {Poelking, Carl and Benduhn, Johannes and Spoltore, Donato and Schwarze, Martin and Roland, Steffen and Piersimoni, Fortunato and Neher, Dieter and Leo, Karl and Vandewal, Koen and Andrienko, Denis},
  title     = {Open-circuit voltage of organic solar cells},
  series = {Communications physics},
  volume    = {5},
  journal   = {Communications physics},
  number    = {1},
  publisher = {Nature portfolio},
  address   = {Berlin},
  issn      = {2399-3650},
  doi       = {10.1038/s42005-022-01084-x},
  pages     = {7},
  year      = {2022},
  abstract  = {Organic photovoltaics (PV) is an energy-harvesting technology that offers many advantages, such as flexibility, low weight and cost, as well as environmentally benign materials and manufacturing techniques. Despite growth of power conversion efficiencies to around 19 \% in the last years, organic PVs still lag behind inorganic PV technologies, mainly due to high losses in open-circuit voltage. Understanding and improving open circuit voltage in organic solar cells is challenging, as it is controlled by the properties of a donor-acceptor interface where the optical excitations are separated into charge carriers. Here, we provide an electrostatic model of a rough donor-acceptor interface and test it experimentally on small molecule PV materials systems. The model provides concise relationships between the open-circuit voltage, photovoltaic gap, charge-transfer state energy, and interfacial morphology. In particular, we show that the electrostatic bias generated across the interface reduces the photovoltaic gap. This negative influence on open-circuit voltage can, however, be circumvented by adjusting the morphology of the donor-acceptor interface. Organic solar cells, despite their high power conversion efficiencies, suffer from open circuit voltage losses making them less appealing in terms of applications. Here, the authors, supported with experimental data on small molecule photovoltaic cells, relate open circuit voltage to photovoltaic gap, charge-transfer state energy, and donor-acceptor interfacial morphology.},
  language  = {en}
}
@article{FritschKurpiersRolandetal.2022,
  author    = {Fritsch, Tobias and Kurpiers, Jona and Roland, Steffen and Tokmoldin, Nurlan and Shoaee, Safa and Ferron, Thomas and Collins, Brian A. and Janietz, Silvia and Vandewal, Koen and Neher, Dieter},
  title     = {On the interplay between CT and singlet exciton emission in organic solar cells with small driving force and its impact on voltage loss},
  series = {Advanced energy materials},
  volume    = {12},
  journal   = {Advanced energy materials},
  number    = {31},
  publisher = {Wiley-VCH},
  address   = {Weinheim},
  issn      = {1614-6832},
  doi       = {10.1002/aenm.202200641},
  pages     = {11},
  year      = {2022},
  abstract  = {The interplay between free charge carriers, charge transfer (CT) states and singlet excitons (S-1) determines the recombination pathway and the resulting open circuit voltage (V-OC) of organic solar cells. By combining a well-aggregated low bandgap polymer with different blend ratios of the fullerenes PCBM and ICBA, the energy of the CT state (E-CT) is varied by 130 meV while leaving the S-1 energy of the polymer (ES1\[{E_{{{\rm{S}}_1}}}\]) unaffected. It is found that the polymer exciton dominates the radiative properties of the blend when ECT\[{E_{{\rm{CT}}}}\] approaches ES1\[{E_{{{\rm{S}}_1}}}\], while the V-OC remains limited by the non-radiative decay of the CT state. It is concluded that an increasing strength of the exciton in the optical spectra of organic solar cells will generally decrease the non-radiative voltage loss because it lowers the radiative V-OC limit (V-OC,V-rad), but not because it is more emissive. The analysis further suggests that electronic coupling between the CT state and the S-1 will not improve the V-OC, but rather reduce the V-OC,V-rad. It is anticipated that only at very low CT state absorption combined with a fairly high CT radiative efficiency the solar cell benefit from the radiative properties of the singlet excitons.},
  language  = {en}
}