Dorothea Scheunemann

Semitransparent Polymer-Based Solar Cells with Aluminum-Doped Zinc Oxide Electrodes

With the use of two transparent electrodes, organic polymer-fullerene solar cells are semitransparent and may be combined to parallel-connected multijunction devices or used for innovative applications like power-generating windows. A challenging issue is the optimization of the electrodes, to combine high transparency with adequate electric properties. In the present work, we study the potential of sputter-deposited aluminum-doped zinc oxide as an alternative to the widely used but relatively expensive indium tin oxide (ITO) as cathode material in semitransparent polymer-fullerene solar cells. Concerning the anode, we utilized an insulator-metal-insulator structure based on ultrathin Au films embedded between two evaporated MoO3 layers, with the outer MoO3 film (capping layer) serving as a light coupling layer. The performance of the ITO-free semitransparent polymer-fullerene solar cells was systematically studied as dependent on the thickness of the capping layer and the active layer as well as the illumination direction. These variations were found to have strong impact on the obtained photocurrent densities. We performed optical simulations of the electric field distribution within the devices using the transfer-matrix method, to analyze the origin of the current density variations in detail and provide deep insight into the device physics. With the conventional absorber materials studied here, optimized ITO-free and semitransparent devices reached 2.0% power conversion efficiency and a maximum optical transmission of 60%, with the device concept being potentially transferable to other absorber materials.

Towards depleted heterojunction solar cells with CuInS2 and ZnO nanocrystals

Colloidal quantum dot solar cells have shown remarkable improvements in performance during the last few years. Until now, mostly Pb- or Cd-based nanocrystals were used as absorber material, which might limit the potential application of nanocrystal solar cells due to toxicity issues. A promising, potentially less-toxic alternative are CuInS2 (CIS) nanocrystals. Here, we report about the realization of solar cells based on a heterojunction formed by solution-producible layers of colloidal CIS and ZnO nanocrystals. Device performance was found to be sensitive to illumination conditions, i.e., the presence of UV light. Although, power conversion efficiencies remain limited in this work, we modeled the possible photocurrents and show that the CIS nanocrystals have a high potential for light-harvesting in quantum dot solar cells.

Three-dimensional morphology of CuInS2:P3HT hybrid blends for photovoltaic applications

Despite potential advantages, the performance of hybrid solar cells with colloidal nanocrystals remains low compared to pure organic solar cells, in particular, when Cd- and Pb-free nanocrystals are employed. To understand this discrepancy, we analyzed possible limiting factors of the performance of hybrid solar cells with CuInS2 nanoparticles and the polymer poly(3-hexylthiophene) (P3HT). Optimizing the thickness of the active layer indicated that charge transport limits the performance of the solar cells. Since charge transport is among others influenced by the morphology of the bulk heterojunction layer, we performed a detailed analysis of the blend morphology. Therefore, we used electron tomography which provides three-dimensional information on the interpenetrating network formed by the hybrid CuInS2:P3HT system. Using statistical methods, we analyzed the distribution of the nanoparticles inside the polymer matrix and the structure of the percolation paths. We found that the morphology appears well s...

Schottky Solar Cells with CuInS2 Nanocrystals as Absorber Material

Abstract Colloidal semiconductor nanocrystals with tunable optical properties are promising materials for light harvesting in solar cells. So far, in particular cadmium and lead chalcogenide nanocrystals were intensively studied in this respect, and the device performance has made rapid progress in recent years. In contrast, less research efforts were undertaken to develop solar cells based on Cd- and Pb-free nanoparticles as absorber material. In the present work, we report on Schottky solar cells with the absorber layer made of colloidal copper indium disulfide nanocrystals. Absorber films with up to ∼ 500 nm thickness were realized by a solution-based layer-by-layer deposition technique. The device performance was systematically studied dependent on the absorber layer thickness. Decreasing photocurrent densities with increasing thickness revealed charge transport to be a limiting factor for the device performance.

Investigation of the Spatially Dependent Charge Collection Probability in CuInS2/ZnO Colloidal Nanocrystal Solar Cells

Solar cells with a heterojunction between colloidal CuInS2 and ZnO nanocrystals are an innovative concept in solution-processed photovoltaics (Appl. Phys. Lett. 2013, 103, 133902), but the conversion efficiency cannot compete yet with devices employing lead chalcogenide quantum dots. Here we present a detailed study on the charge collection in CuInS2/ZnO solar cells. An inverted device architecture was utilized, in which the ZnO played an additional role as optical spacer layer. Variations of the ZnO thickness were exploited to create different charge generation profiles within the light-harvesting CuInS2 layer, which strongly affected both the external and internal quantum efficiency. By the reconstruction of these experimental findings with the help of a purely optical model, we were able to draw conclusions on the spatial dependency of the charge collection probability. We provide evidence that only carriers generated within a narrow zone of ∼40 nm near the CuInS2/ZnO interface contribute to the extern...

Revealing the recombination dynamics in squaraine-based bulk heterojunction solar cells

We combine steady-state with transient optoelectronic characterization methods to understand the operation of photovoltaic devices based on a benchmark model squaraine blended with a fullerene acceptor. These devices suffer from a gradual decrease in the fill factor when increasing the active layer thickness and incident light intensity. Using transient photocurrent, transient photovoltage, and bias-assisted charge extraction measurements, we show that the fill factor deteriorates due to slow charge carrier collection competing with bimolecular recombination. Under normal operating conditions, we find a bimolecular recombination rate constant of ∼10–17 m3 s−1, which corresponds to a reduction of one to two orders of magnitude compared to the Langevin model.

The effect of polymer molecular weight on the performance of PTB7-Th:O-IDTBR non-fullerene organic solar cells

Recent advances in the development of non-fullerene acceptors have increased the power conversion efficiency of organic solar cells to approximately 13%. Fullerene-derivatives and non-fullerene acceptors possess distinctively different structural, optical and electronic properties, which also change the requirements on the polymer donor in non-fullerene organic solar cells. Therefore, in this study, the effect of the molecular weight of the conjugated polymer on the photovoltaic performance, charge carrier mobility, crystallization properties, film morphology, and non-geminate recombination dynamics is systematically investigated in polymer:small molecule organic solar cells using the low bandgap polymer PTB7-Th as the donor and the non-fullerene indacenodithiophene-based small molecule O-IDTBR as the acceptor. Among the examined polymer samples (50–300 kDa), high molecular weights of PTB7-Th (with an optimum molecular weight of 200 kDa) are advantageous to achieve high efficiencies up to 10%, which can be correlated with an increased crystallinity, an improved field-effect hole mobility (1.05 × 10−2 cm2 V−1 s−1), lower charge carrier trapping and a reduced activation energy of charge transport (98 meV). Bias-assisted charge extraction and transient photovoltage measurements reveal higher carrier concentrations (1016 cm−3) and long lifetimes (4.5 μs) as well as lower non-geminate recombination rate constants in the corresponding devices, supporting the high photocurrents (ca. 15.2 mA cm−2) and fill factors (>60%).