TY - JOUR A1 - Fritsch, Tobias A1 - Kurpiers, Jona A1 - Roland, Steffen A1 - Tokmoldin, Nurlan A1 - Shoaee, Safa A1 - Ferron, Thomas A1 - Collins, Brian A. A1 - Janietz, Silvia A1 - Vandewal, Koen A1 - Neher, Dieter T1 - On the interplay between CT and singlet exciton emission in organic solar cells with small driving force and its impact on voltage loss JF - Advanced energy materials N2 - 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. KW - external quantum efficiency KW - organic photovoltaics KW - ternary blends KW - voltage losses Y1 - 2022 U6 - https://doi.org/10.1002/aenm.202200641 SN - 1614-6832 SN - 1614-6840 VL - 12 IS - 31 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Vollbrecht, Joachim A1 - Brus, Viktor V. T1 - On the recombination order of surface recombination under open circuit conditions JF - Organic electronics : physics, materials and applications N2 - Understanding the recombination dynamics of organic and perovskite solar cells has been a crucial prerequisite in the steadily increasing performance of these promising new types of photovoltaics. Surface recombination in particular has turned out to be one of the last remaining roadblocks, which specifically reduces the open circuit voltage. In this study, the relationship between the rate of surface recombination and the density of charge carriers is analyzed, revealing a cubic dependence between these two parameters. This hypothesis is then tested and verified with the recombination dynamics of an organic solar cell known to exhibit significant surface recombination and a high energy proton irradiated CH3NH3PbI3 pemvskite solar cell during white light illumination. Incidentally, these results can also explain recombination orders exceeding the commonly known threshold for bimolecular recombination that have been observed in some studies without the need for a charge carrier dependent bimolecular recombination coefficient. KW - surface recombination KW - recombination order KW - organic photovoltaics KW - Perovskite solar cells KW - charge carrier density KW - Shockley-Read-Hall KW - statistics Y1 - 2020 U6 - https://doi.org/10.1016/j.orgel.2020.105905 SN - 1566-1199 SN - 1878-5530 VL - 86 PB - Elsevier Science CY - Amsterdam [u.a.] ER - TY - JOUR A1 - Vollbrecht, Joachim A1 - Brus, Viktor V. T1 - On charge carrier density in organic solar cells obtained via capacitance spectroscopy JF - Advanced electronic materials N2 - The determination of the voltage-dependent density of free charge carriers via capacitance spectroscopy is considered an important step in the analysis of emerging photovoltaic technologies, such as organic and perovskite solar cells. In particular, an intimate knowledge of the density of free charge carriers is required for the determination of crucial parameters such as the effective mobility, charge carrier lifetime, nongeminate recombination coefficients, average extraction times, and competition factors. Hence, it is paramount to verify the validity of the commonly employed approaches to obtain the density of free charge carriers. The advantages, drawbacks, and limitations of the most common approaches are investigated in detail and strategies to mitigate misleading values are explored. To this end, two types of nonfullerene organic solar cells based on a PTB7-Th:ITIC-2F blend and a PM6:Y6 blend, respectively, are used as a case study to assess how subsequent analyses of the nongeminate recombination dynamics depend on the chosen approach to calculate the density of free charge carriers via capacitance spectroscopy. KW - bulk-heterojunction solar cells KW - capacitance spectroscopy KW - charge KW - carrier density KW - impedance spectroscopy KW - organic photovoltaics Y1 - 2020 U6 - https://doi.org/10.1002/aelm.202000517 SN - 2199-160X VL - 6 IS - 10 PB - Wiley CY - Hoboken ER - TY - JOUR A1 - Sini, Gjergji A1 - Schubert, Marcel A1 - Risko, Chad A1 - Roland, Steffen A1 - Lee, Olivia P. A1 - Chen, Zhihua A1 - Richter, Thomas V. A1 - Dolfen, Daniel A1 - Coropceanu, Veaceslav A1 - Ludwigs, Sabine A1 - Scherf, Ullrich A1 - Facchetti, Antonio A1 - Frechet, Jean M. J. A1 - Neher, Dieter T1 - On the Molecular Origin of Charge Separation at the Donor-Acceptor Interface JF - Advanced energy materials N2 - 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. KW - donor-acceptor interfaces KW - energy gradients KW - geometrical deformations KW - nonfullerene acceptors KW - organic photovoltaics KW - photocurrent generation KW - polymer solar cells Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201702232 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 12 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Cardinaletti, Ilaria A1 - Kesters, Jurgen A1 - Bertho, Sabine A1 - Conings, Bert A1 - Piersimoni, Fortunato A1 - Lutsen, Laurence A1 - Nesladek, Milos A1 - Van Mele, Bruno A1 - Van Assche, Guy A1 - Vandewal, Koen A1 - Salleo, Alberto A1 - Vanderzande, Dirk A1 - Maes, Wouter A1 - Manca, Jean V. T1 - Toward bulk heterojunction polymer solar cells with thermally stable active layer morphology JF - Journal of photonics for energy N2 - When state-of-the-art bulk heterojunction organic solar cells with ideal morphology are exposed to prolonged storage or operation at elevated temperatures, a thermally induced disruption of the active layer blend can occur, in the form of a separation of donor and acceptor domains, leading to diminished photovoltaic performance. Toward the long-term use of organic solar cells in real-life conditions, an important challenge is, therefore, the development of devices with a thermally stable active layer morphology. Several routes are being explored, ranging from the use of high glass transition temperature, cross-linkable and/or side-chain functionalized donor and acceptor materials, to light-induced dimerization of the fullerene acceptor. A better fundamental understanding of the nature and underlying mechanisms of the phase separation and stabilization effects has been obtained through a variety of analytical, thermal analysis, and electro-optical techniques. Accelerated aging systems have been used to study the degradation kinetics of bulk heterojunction solar cells in situ at various temperatures to obtain aging models predicting solar cell lifetime. The following contribution gives an overview of the current insights regarding the intrinsic thermally induced aging effects and the proposed solutions, illustrated by examples of our own research groups. (C) The Authors. Published by SPIE under a Creative Commons Attribution 3.0 Unported License. KW - organic photovoltaics KW - bulk heterojunction KW - thermal stability KW - phase separation KW - lifetime Y1 - 2014 U6 - https://doi.org/10.1117/1.JPE.4.040997 SN - 1947-7988 VL - 4 PB - SPIE CY - Bellingham ER - TY - JOUR A1 - Schubert, Marcel A1 - Dolfen, Daniel A1 - Frisch, Johannes A1 - Roland, Steffen A1 - Steyrleuthner, Robert A1 - Stiller, Burkhard A1 - Chen, Zhihua A1 - Scherf, Ullrich A1 - Koch, Norbert A1 - Facchetti, Antonio A1 - Neher, Dieter T1 - Influence of aggregation on the performance of All-Polymer Solar Cells containing Low-Bandgap Naphthalenediimide Copolymers JF - dvanced energy materials N2 - 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. KW - aggregation KW - morphology KW - naphthalenediimide KW - organic semiconductors KW - organic photovoltaics Y1 - 2012 U6 - https://doi.org/10.1002/aenm.201100601 SN - 1614-6832 VL - 2 IS - 3 SP - 369 EP - 380 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Gao, Feng A1 - Wang, Jianpu A1 - Blakesley, James C. A1 - Hwang, Inchan A1 - Li, Zhe A1 - Greenham, Neil C. T1 - Quantifying loss mechanisms in polymer Fullerene photovoltaic devices JF - dvanced energy materials KW - organic photovoltaics KW - recombination KW - bulk heterojunctions KW - loss mechanisms KW - drift-diffusion models Y1 - 2012 U6 - https://doi.org/10.1002/aenm.201200073 SN - 1614-6832 VL - 2 IS - 8 SP - 956 EP - 961 PB - Wiley-VCH CY - Weinheim ER -