Several high performance polymer:fullerene bulk-heterojunction photo-active layers, deposited from the non-halogenated solvents o-xylene or anisole in combination with the eco-compatible additive p-anisaldehyde, are investigated. The respective solar cells yield excellent power conversion efficiencies up to 9.5%, outperforming reference devices deposited from the commonly used halogenated chlorobenzene/1,8-diiodooctane solvent/additive combination. The impact of the processing solvent on the bulk-heterojunction properties is exemplified on solar cells comprising benzodithiophenethienothiophene co-polymers and functionalized fullerenes (PTB7:PC71BM). The additive p-anisaldehyde improves film formation, enhances polymer order, reduces fullerene agglomeration and shows high volatility, thereby positively affecting layer deposition, improving charge carrier extraction and reducing drying time, the latter being crucial for future large area roll-to-roll device fabrication.

Imaging the phase distribution of amorphous or partially crystalline organic materials at the nanoscale and analyzing the local atomic structure of individual phases has been a long-time challenge. We propose a new approach for imaging the phase distribution and for analyzing the local structure of organic materials based on scanning transmission electron diffraction (4D-STEM) pair distribution function analysis (PDF). We show that electron diffraction based PDF analysis can be used to characterize the short- and medium-range order in aperiodically packed organic molecules. Moreover, we show that 4D-STEM-PDF does not only provide local structural information with a resolution of a few nanometers, but can also be used to image the phase distribution of organic composites. The distinct and thickness independent contrast of the phase image is generated by utilizing the structural difference between the different types of molecules and taking advantage of the dose efficiency due to use of the full scattering signal. Therefore, this approach is particularly interesting for imaging unstained organic or polymer composites without distinct valence states for electron energy loss spectroscopy. We explore the possibilities of this new approach using [6,6]-phenyl-C61- butyric acid methyl ester (PC61BM) and poly(3-hexylthiophene-2,5-diyl) (P3HT) as the archetypical and best-investigated semiconductor blend used in organic solar cells, compare our phase distribution with virtual dark-field analysis and validate our approach by electron energy loss spectroscopy.

Organic semiconductors find a wide range of applications, such as in organic light emitting diodes, organic solar cells, and organic field effect transistors. One of their most striking disadvantages in comparison to crystalline inorganic semiconductors is their low charge-carrier mobility, which manifests itself in major device constraints such as limited photoactive layer thicknesses. Trial-and-error attempts to increase charge-carrier mobility are impeded by the complex interplay of the molecular and electronic structure of the material with its morphology. Here, the viability of a multiscale simulation approach to rationally design materials with improved electron mobility is demonstrated. Starting from one of the most widely used electron conducting materials (Alq ), novel organic semiconductors with tailored electronic properties are designed for which an improvement of the electron mobility by three orders of magnitude is predicted and experimentally confirmed.

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Organic solar cells have come a long way from fundamental considerations of charge carrier dynamics in organic semiconductors to devices with laboratory power conversion efficiencies exceeding 17% and first power harvesting installations. Despite this story of success, these days, the scientific community witnesses a shift of research effort to other solar concepts, leaving behind a high‐potential solar technology with better applicability forecasts than ever before. Very compelling reasons still exist why organic solar cells can become the solar technology of the future that offers design versatility and enables unprecedented applications while offering the lowest energy payback times and ecologic sustainability. This perspective article highlights why organic solar cells remain a research field of the highest socioeconomic relevance, which challenges remain to be overcome in the future, and how organic solar cells can make a difference in the future energy landscape.

Earlier reports have discussed the manifold opportunities that arise from the use of eco-friendly organic semiconductor dispersions as inks for printed electronics and, in particular, organic photovoltaics. To date, poly(3-hexylthiophene)...

Organic semiconductor nanoparticle dispersions are electrostatically stabilized with the p‐doping agent 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4TCNQ), omitting the need for surfactants. Smallest amounts of F4TCNQ stabilize poly(3‐hexylthiophene) dispersions and reduce the size of the nanoparticles significantly. The concept is then readily transferred to synthesize dispersions from a choice of light‐harvesting benzodithiophene‐based copolymers. Dispersions from the corresponding polymer:fullerene blends are used to fabricate organic solar cells (OSCs). In contrast to the widely used stabilizing surfactants, small amounts of F4TCNQ show no detrimental effect on the device performance. This concept paves the way for the eco‐friendly fabrication of OSCs from nanoparticle dispersions of high‐efficiency light‐harvesting semiconductors by eliminating environmentally hazardous solvents from the deposition process.

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