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The influence of environmental factors on the degradation process of P3HT film has been investigated quantitatively. The decay kinetics of the polymer absorption during variation of intensity and spectral distribution of the incident light, oxygen concentration, humidity level as well as temperature are monitored using infrared and UV/vis absorption spectroscopy. Additionally, the oxygen diffusion into the polymer film has been investigated using fluorescence spectroscopy under the same experimental conditions. The degradation process is light initiated with a strong increase of the effectiveness toward the ultraviolet region of the spectrum. The observed photo oxidation is not oxygen diffusion limited although an activation energy of 26 kJmol -1 was observed for both degradation and oxygen diffusion. The observed kinetics, especially its dependence on wavelength of the incident light, point to a radical-based degradation process in the solid state rather than a singlet oxygen-based mechanism as it is observed in the liquid phase. Furthermore the presence of humidity strongly affects the degradation process although water itself does not decompose the polymer. Changing the structure of the polymer from regioregular to regiorandom significantly accelerates the degradation, probably due to the higher triplet yield of the regiorandom polymer.

Carbon bridged (C‐PCPDTBT) and silicon‐bridged (Si‐PCPDTBT) dithiophene donor–acceptor copolymers belong to a promising class of low bandgap materials. Their higher field‐effect mobility, as high as 10−2 cm2 V−1 s−1 in pristine films, and their more balanced charge transport in blends with fullerenes make silicon‐bridged materials better candidates for use in photovoltaic devices. Striking morphological changes are observed in polymer:fullerene bulk heterojunctions upon the substitution of the bridging atom. XRD investigation indicates increased π–π stacking in Si‐PCPDTBT compared to the carbon‐bridged analogue. The fluorescence of this polymer and that of its counterpart C‐PCPDTBT indicates that the higher photogeneration achieved in Si‐PCPDTBT:fullerene films (with either [C60]PCBM or [C70]PCBM) can be correlated to the inactivation of a charge‐transfer complex and to a favorable length of the donor–acceptor phase separation. TEM studies of Si‐PCPDTBT:fullerene blended films suggest the formation of an interpenetrating network whose phase distribution is comparable to the one achieved in C‐PCPDTBT:fullerene using 1,8‐octanedithiol as an additive. In order to achieve a balanced hole and electron transport, Si‐PCPDTBT requires a lower fullerene content (between 50 to 60 wt%) than C‐PCPDTBT (more than 70 wt%). The Si‐PCPDTBT:[C70]PCBM OBHJ solar cells deliver power conversion efficiencies of over 5%.

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An extended replacement circuit describing the current–voltage characteristics of bulk heterojunction polymer solar cells at different light bias levels is introduced and discussed. A one diode-model is expanded by an extraction model for photogenerated carriers taking into account the effective reduction of the mean distance which the charge carriers cover when sweeping the electrical bias through the fourth quadrant of the solar cell. The model properly describes the current–voltage behavior of bulk heterojunction solar cells over more than three orders in light intensity with one set of parameters.

Fundamental advances to increase the efficiency as well as stability of organic photovoltaics (OPVs) are achieved by designing ternary blends, which represents a clear trend toward multicomponent active layer blends. The development of high‐throughput and autonomous experimentation methods is reported for the effective optimization of multicomponent polymer blends for OPVs. A method for automated film formation enabling the fabrication of up to 6048 films per day is introduced. Equipping this automated experimentation platform with a Bayesian optimization, a self‐driving laboratory is constructed that autonomously evaluates measurements to design and execute the next experiments. To demonstrate the potential of these methods, a 4D parameter space of quaternary OPV blends is mapped and optimized for photostability. While with conventional approaches, roughly 100 mg of material would be necessary, the robot‐based platform can screen 2000 combinations with less than 10 mg, and machine‐learning‐enabled autonomous experimentation identifies stable compositions with less than 1 mg.

We present investigations of organic photovoltaic devices consisting of bulk heterojunction layers made from several material combinations. All of the investigated systems reveal close similarities to the behavior of classical pn-junction devices. The consequences of the pn-junction-like behavior on the device parameters and performance are presented. Furthermore, device characteristics and parameters of the pristine materials are correlated, resulting in a model that permits an identification of high potential materials, a performance prediction, and a device optimization. The resulting model is able to predict an open circuit voltage and a fill factor and their evolution with the light intensity or thickness of the active layer. It simplifies the identification of the internal morphology and therefore the choice of appropriate solvents. Necessary parameters concerning the choice of electrode materials are also provided.

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