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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