Florian Machui

Scalable, ambient atmosphere roll-to-roll manufacture of encapsulated large area, flexible organic tandem solar cell modules

Inline printing and coating methods have been demonstrated to enable a high technical yield of fully roll-to-roll processed polymer tandem solar cell modules. We demonstrate generality by employing different material sets and also describe how the ink systems must be carefully co-developed in order to reach the ambitious objective of a fully printed and coated 14-layer flexible tandem solar cell stack. The roll-to-roll methodologies involved are flexographic printing, rotary screen printing, slot-die coating, X-ray scattering, electrical testing and UV-lamination. Their combination enables the manufacture of completely functional devices in exceptionally high yields. Critical to the ink and process development is a carefully chosen technology transfer to industry method where first a roll coater is employed enabling contactless stack build up, followed by a small roll-to-roll coater fitted to an X-ray machine enabling in situ studies of wet ink deposition and drying mechanisms, ultimately elucidating how a robust inline processed recombination layer is key to a high technical yield. Finally, the transfer to full roll-to-roll processing is demonstrated.

High shunt resistance in polymer solar cells comprising a MoO3 hole extraction layer processed from nanoparticle suspension

In this report, we present solution processed molybdenum trioxide (MoO3) layers incorporated as hole extraction layer (HEL) in polymer solar cells (PSCs) and demonstrate the replacement of the commonly employed poly(3,4-ethylene dioxythiophene):(polystyrene sulfonic acid) (PEDOT:PSS). MoO3 is known to have excellent electronic properties and to yield more stable devices compared to PEDOT:PSS. We demonstrate fully functional solar cells with up to 65 nm thick MoO3 HEL deposited from a nanoparticle suspension at low temperatures. The PSCs with an active layer comprising a blend of poly(3-hexylthiophene) and [6,6]-phenyl-C61 butyric acid methyl ester and a MoO3 HEL show comparable performance to reference devices with a PEDOT:PSS HEL. The best cells with MoO3 reach a fill factor of 66.7% and power conversion efficiency of 2.92%. Moreover, MoO3 containing solar cells exhibit an excellent shunt behavior with a parallel resistance of above 100 kΩ cm2.

Cost analysis of roll-to-roll fabricated ITO free single and tandem organic solar modules based on data from manufacture

We present a cost analysis based on state of the art printing and coating processes to fully encapsulated, flexible ITO- and vacuum-free polymer solar cell modules. Manufacturing data for both single junctions and tandem junctions are presented and analyzed. Within this calculation the most expensive layers and processing steps are identified. Based on large roll-to-roll coating experiments the exact material consumptions were determined. In addition to the data for the pilot scale experiment presented here, projections to medium and large scale scenarios serve as a guide to achieve cost targets of 5 €ct per Wp in a detailed material and cost analysis. These scenarios include the replacement of cost intensive layers, as well as process optimization steps. Furthermore, the cost structures for single and tandem devices are listed in detail and discussed. In an optimized model the material costs drop below 10 € per m2 which proves that OPV is a competitive alternative to established power generation technologies.

Towards 15% energy conversion efficiency: a systematic study of the solution-processed organic tandem solar cells based on commercially available materials

Owing to the lack of scalable high performance donor materials, studies on mass-produced organic photovoltaic (OPV) devices lag far behind that on lab-scale devices. In this work, we choose 6 already commercially available conjugated polymers and systematically investigate their potential in organic tandem solar cells. All the devices are processed under environmental conditions using doctor-blading, which is highly compatible with mass-production coating technologies. Power conversion efficiencies (PCE) of 6–7% are obtained for OPV devices based on different active layers. Optical simulations based on experimental data are performed for all realized tandem solar cells. An efficiency potential of ∼10% is estimated for these compounds in combination with phenyl-C61-butyric acid methyl ester (PCBM) as an acceptor. In addition, we assume a hypothetical, optimized acceptor to understand the limitation of donors. It is suggested that a PCE of >14% is realistic for tandem solar cells based on these commercially available donor materials. Along with the demonstration of novel intermediate layers we believe that this systematic study provides valuable insight for those attempting to realize the high efficiency potential of tandem architectures.

Influence of a ternary donor material on the morphology of a P3HT:PCBM blend for organic photovoltaic devices

A comparison of grazing incidence wide-angle X-ray scattering (GiWAXS) and differential scanning calorimetric measurements (DSC) was used to identify the influence of a dominantly amorphous small band gap polymer material poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b′]dithiophene)-alt-4,7(2,1,3-benzothiadiazole)] (PCPDTBT) on the crystallinity of a semi-crystalline polymer/fullerene composite. In binary blends the low band gap polymer does not influence the crystalline part of P3HT, but does influence the crystallinity of the fullerene. In ternary blends, a significant drop of the PCBM crystallinity is observed with increasing PCPDTBT content. Adding more than 20 wt% PCPDTBT to a P3HT:PCBM blend leads to a dramatic reduction of device efficiency, mainly due to short circuit current density and fill factor losses. This deterioration is attributed to the fact that addition of more than 20 wt% PCPDTBT to the host system strongly reduces crystallinity of the fullerene phase and electron transport in the ternary system.

Highly efficient, large area, roll coated flexible and rigid OPV modules with geometric fill factors up to 98.5% processed with commercially available materials

Highly efficient, large area OPV modules achieving full area efficiencies of up to 93% of the reference small area cells are reported. The way to a no-loss up-scaling process is highlighted: photoelectrical conversion efficiencies of 5.3% are achieved on rigid modules and of 4.2% on flexible, roll coated ones, employing a commercially available photoactive material. Exceptionally high geometric fill factors (98.5%), achieved via structuring by ultrashort laser pulses, with interconnection widths below 100 μm are demonstrated.

Air-processed organic tandem solar cells on glass: toward competitive operating lifetimes

Photovoltaic devices based on organic semiconductors (OPVs) hold great promise as a cost-effective renewable energy platform because they can be processed from solution and deposited on flexible plastics using roll-to-roll processing. Despite important progress and reported power conversion efficiencies of more than 10% the rather limited stability of this type of devices raises concerns towards future commercialization. The tandem concept allows for both absorbing a broader range of the solar spectrum and reducing thermalization losses. We designed an organic tandem solar cell with an inverted device geometry comprising environmentally stable active and charge-selecting layers. Under continuous white light irradiation, we demonstrate an extrapolated, operating lifetime in excess of one decade. We elucidate that for the current generation of organic tandem cells one critical requirement for long operating lifetimes consists of periodic UV light treatment. These results suggest that new material approaches towards UV-resilient active and interfacial layers may enable efficient organic tandem solar cells with lifetimes competitive with traditional inorganic photovoltaics.

Morphology analysis of near IR sensitized polymer/fullerene organic solar cells by implementing low bandgap heteroanalogue C-/Si-PCPDTBT

In the current work, we have investigated the morphological aspects of the ternary solar cells based on host matrices of P3HT:PCBM and P3HT:ICBA, using the low bandgap polymer analogues of C- and Si-bridged PCPDTBT as near IR sensitizers, which show noticeably different performance. A direct comparison of these well-functional and poorly functional ternary blend systems provides insights into the bottlenecks of device performance and enables us to set up an initial set of design rules for ternary organic solar cells. Our study reveals the importance of surface energy as a driving force controlling sensitizer location and morphology formation of ternary blends. The interfacial surface energy results indicate that Si-PCPDTBT locates at amorphous interfaces and P3HT crystallites, while C-PCPDTBT tends to accumulate at amorphous interfaces and semi-crystalline (or agglomerated) domains of the fullerene derivatives. GIWAXS and SCLC results support this prediction where adding high content of C-PCPDTBT influences mainly the semi-crystallinity (aggregation) of the fullerene and reduces the electron mobility, but Si-PCPDTBT impacts mainly the P3HT ordering and, in turn, deteriorates the hole mobility. These findings show that the disruption of the fullerene semi-crystalline domains is more detrimental to the device performance than the disruption of the polymer domains.

Classification of Additives for Organic Photovoltaic Devices

The use of additives to improve the performance of organic photovoltaic cells has been intensely researched in recent years. However, so far, no system has been reported for the classification of additives and their functions. In this report, a system for classifying additives according to the fundamental mechanism by which they influence microstructure formation for P3HT:PCBM is suggested. The major parameters used for their classification are solubility and drying kinetics. Both are discussed in detail and their consequences on processing are analyzed. Furthermore, a general mechanism to classify the impact of additives on structure formation is suggested and discussed for different materials relevant to organic photovoltaic devices.

Combined Computational Approach Based on Density Functional Theory and Artificial Neural Networks for Predicting The Solubility Parameters of Fullerenes

The solubility of organic semiconductors in environmentally benign solvents is an important prerequisite for the widespread adoption of organic electronic appliances. Solubility can be determined by considering the cohesive forces in a liquid via Hansen solubility parameters (HSP). We report a numerical approach to determine the HSP of fullerenes using a mathematical tool based on artificial neural networks (ANN). ANN transforms the molecular surface charge density distribution (σ-profile) as determined by density functional theory (DFT) calculations within the framework of a continuum solvation model into solubility parameters. We validate our model with experimentally determined HSP of the fullerenes C60, PC61BM, bisPC61BM, ICMA, ICBA, and PC71BM and through comparison with previously reported molecular dynamics calculations. Most excitingly, the ANN is able to correctly predict the dispersive contributions to the solubility parameters of the fullerenes although no explicit information on the van der Waals forces is present in the σ-profile. The presented theoretical DFT calculation in combination with the ANN mathematical tool can be easily extended to other π-conjugated, electronic material classes and offers a fast and reliable toolbox for future pathways that may include the design of green ink formulations for solution-processed optoelectronic devices.