Formation of vertical concentration gradients in poly(3-hexylthiophene-2,5-diyl): Phenyl-C₆₁-butyric acid methyl ester-graded bilayer solar cells

In the present work, we demonstrate that graded bilayer solar cells provide a very interesting alternative to the bulk heterojunction active layers commonly used in organic photovoltaic cells. One of the main advantages of this type of active layers is the possibility to optimize independently both donor and acceptor layers. Using various process methods, we obtain active layers that demonstrate a donor–acceptor vertical concentration gradient. These devices exhibit not only a high fill factor but also a remarkable increase in open-circuit voltage (V_oc). In order to understand the influence of the film morphology over the device parameters, we provide a complete study using energy-dispersive x-ray spectroscopy elemental mapping of the device cross sections, showing evidence that ideal donor–acceptor concentration gradient are required to obtain high fill factors. Furthermore, we use a simple equivalent electrical model to extrapolate device parameters such as reverse saturation current for a clearer understanding of the origin of the V_oc increase. - Highlights: • Various donor–acceptor concentration-graded devices were fabricated. • Improved donor–acceptor concentration gradient enhances the photovoltaic properties. • The increased open-circuit voltage results from lower reverse saturation currents. • Adjusting the dimensions of buffer and intermixed layers enhances fill factor. • Ideal active layer morphologies lead to an increase of 30% of the efficiency