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AbstractOrganic semiconductors are in general known to have an inherently lower charge carrier mobility compared to their inorganic counterparts. Bimolecular recombination of holes and electrons is an important loss mechanism and can often be described by the Langevin recombination model. Here, the device physics of bulk heterojunction solar cells based on a nonfullerene acceptor (IDTBR) in combination with poly(3‐hexylthiophene) (P3HT) are elucidated, showing an unprecedentedly low bimolecular recombination rate. The high fill factor observed (above 65%) is attributed to non‐Langevin behavior with a Langevin prefactor (β/βL) of 1.9 × 10−4. The absence of parasitic recombination and high charge carrier lifetimes in P3HT:IDTBR solar cells inform an almost ideal bimolecular recombination behavior. This exceptional recombination behavior is explored to fabricate devices with layer thicknesses up to 450 nm without significant performance losses. The determination of the photoexcited carrier mobility by time‐of‐flight measurements reveals a long‐lived and nonthermalized carrier transport as the origin for the exceptional transport physics. The crystalline microstructure arrangement of both components is suggested to be decisive for this slow recombination dynamics. Further, the thickness‐independent power conversion efficiency is of utmost technological relevance for upscaling production and reiterates the importance of understanding material design in the context of low bimolecular recombination.

The transfer from P3HT based fullerene free OPV lab cells with IDTBR as acceptor material to fully solution processed roll-to-roll compatible modules is reported.

The molecular weight of an electron donor‐conjugated polymer is as essential as other well‐known parameters in the chemical structure of the polymer, such as length and the nature of any side groups (alkyl chains) positioned on the polymeric backbone, as well as their placement, relative strength, the ratio of the donor and acceptor moieties in the backbone of donor–acceptor (D–A)‐conjugated polymers, and the arrangement of their energy levels for organic photovoltaic performance. Finding the “optimal” molecular weight for a specific conjugated polymer is an important aspect for the development of novel photovoltaic polymers. Therefore, it is evident that the chemistry of functional conjugated polymers faces major challenges and materials have to adopt a broad range of specifications in order to be established for high photovoltaic performance. In this review, the approaches followed for enhancing the molecular weight of electron‐donor polymers are presented in detail, as well as how this influences the optoelectronic properties, charge transport properties, structural conformation, morphology, and the photovoltaic performance of the active layer. image

In recent years the concept of ternary blend bulk heterojunction (BHJ) solar cells based on organic semiconductors has been widely used to achieve a better match to the solar irradiance spectrum, and power conversion efficiencies beyond 10% have been reported. However, the fill factor of organic solar cells is still limited by the competition between recombination and extraction of free charges. Here, we design advanced material composites leading to a high fill factor of 77% in ternary blends, thus demonstrating how the recombination thresholds can be overcome. Extending beyond the typical sensitization concept, we add a highly ordered polymer that, in addition to enhanced absorption, overcomes limits predicted by classical recombination models. An effective charge transfer from the disordered host system onto the highly ordered sensitizer effectively avoids traps of the host matrix and features an almost ideal recombination behaviour. Carrier recombination in organic solar cells usually limits their optoelectronic performance, in particular their fill factor. Gasparini et al show that adding an ordered polymer to a ternary blend reduces carrier recombination, achieving a fill factor of 77%.

Semi‐transparent organic solar cells (ST‐OSCs) show a unique potential to be integrated in windows due to their outstanding characteristics such as high transparency and color‐adjustability. In order to achieve both, high transparency and high efficiency, the use of dielectric mirrors is an excellent concept. However, such a mirror will not only improve the photocurrent generated by a solar cell but also cause losses in transparency. In this work, a theoretical model is developed that predicts the effect of the dielectric mirror on the balance between photocurrent enhancement and transparency loss depending on the spectral shape of the ST‐OSC absorption. Experimental investigations with three fully printed ST‐OSCs showing different absorption characteristics underline the validity of these studies. It is concluded that ST‐OSCs with broad absorption spectra ranging from the short wavelength region over the visible to at least 950 nm are most suitable for the implementation of a dielectric mirror. A narrower absorption spectrum or a shift of the spectrum toward longer wavelengths makes an increase in photoactive layer thickness more beneficial than the attachment of a dielectric mirror. Moreover, the dielectric mirror approach is an excellent strategy to obtain high photocurrents for materials which cannot be processed at high active layer thicknesses.

Low-bandgap near-infrared polymers are usually synthesized using the common donor-acceptor (D-A) approach. However, recently polymer chemists are introducing more complex chemical concepts for better fine tuning of their optoelectronic properties. Usually these studies are limited to one or two polymer examples in each case study so far, though. In this study, the dependence of optoelectronic and macroscopic (device performance) properties in a series of six new D-A1 -D-A2 low bandgap semiconducting polymers is reported for the first time. Correlation between the chemical structure of single-component polymer films and their optoelectronic properties has been achieved in terms of absorption maxima, optical bandgap, ionization potential, and electron affinity. Preliminary organic photovoltaic results based on blends of the D-A1 -D-A2 polymers as the electron donor mixed with the fullerene derivative [6,6]-phenyl-C71 -butyric acid methyl ester demonstrate power conversion efficiencies close to 4% with short-circuit current densities (J sc ) of around 11 mA cm-2 , high fill factors up to 0.70, and high open-circuit voltages (V oc s) of 0.70 V. All the devices are fabricated in an inverted architecture with the photoactive layer processed in air with doctor blade technique, showing the compatibility with roll-to-roll large-scale manufacturing processes.