Solution-Processing of Organic Solar Cells: From In Situ Investigation to Scalable Manufacturing

  • Maged Abdelsamie

Student thesis: Doctoral Thesis


Photovoltaics provide a feasible route to fulfilling the substantial increase in demand for energy worldwide. Solution processable organic photovoltaics (OPVs) have attracted attention in the last decade because of the promise of low-cost manufacturing of sufficiently efficient devices at high throughput on large-area rigid or flexible substrates with potentially low energy and carbon footprints. In OPVs, the photoactive layer is made of a bulk heterojunction (BHJ) layer and is typically composed of a blend of an electron-donating (D) and an electron-accepting (A) materials which phase separate at the nanoscale and form a heterojunction at the D-A interface that plays a crucial role in the generation of charges. Despite the tremendous progress that has been made in increasing the efficiency of organic photovoltaics over the last few years, with power conversion efficiency increasing from 8% to 13% over the duration of this PhD dissertation, there have been numerous debates on the mechanisms of formation of the crucial BHJ layer and few clues about how to successfully transfer these lessons to scalable processes. This stems in large part from a lack of understanding of how BHJ layers form from solution. This lack of understanding makes it challenging to design BHJs and to control their formation in laboratory-based processes, such as spin-coating, let alone their successful transfer to scalable processes required for the manufacturing of organic solar cells. Consequently, the OPV community has in recent years sought out to better understand the key characteristics of state of the art lab-based organic solar cells and made efforts to shed light on how the BHJ forms in laboratory-based processes as well as in scalable processes. We take the view that understanding the formation of the solution-processed bulk heterojunction (BHJ) photoactive layer, where crucial photovoltaic processes take place, is the one of the most crucial steps to developing strategies towards the implementation of organic solar cells with high efficiency and manufacturability. In this dissertation, we investigate the mechanism of the BHJ layer formation during solution processing from common lab-based processes, such as spin-coating, with the aim of understanding the roles of materials, formulations and processing conditions and subsequently using this insight to enable the scalable manufacturing of high efficiency organic solar cells by such methods as wire-bar coating and blade-coating. To do so, we have developed state-of-the-art in situ diagnostics techniques to provide us with insight into the thin film formation process. As a first step, we have developed a modified spin-coater which allows us to perform in situ UV-visible absorption measurements during spin coating and provides key insight into the formation and evolution of polymer aggregates in solution and during the transformation to the solid state. Using this method, we have investigated the formation of organic BHJs made of a blend of poly (3-hexylthiophene) (P3HT) and fullerene, reference materials in the organic solar cell field. We show that process kinetics directly influence the microstructure and morphology of the bulk heterojunction, highlighting the value of in situ measurements. We have investigated the influence of crystallization dynamics of a wide-range of small-molecule donors and their solidification pathways on the processing routes needed for attaining high-performance solar cells. The study revealed the reason behind the need of empirically-adopted processing strategies such as solvent additives or alternatively thermal or solvent vapor annealing for achieving optimal performance. The study has provided a new perspective to materials design linking the need for solvent additives or annealing to the ease of crystallization of small-molecule donors and the presence or absence of transient phases before crystallization. From there, we have extended our investigation to small-molecule (p-DTS (FBTTh2)2) fullerene blend solar cells, where we have revealed new insight into the crucial role of solvent additives. Our work has also touched upon modern polymers, such as PBDTTPD, where we have found the choice of additives impacts the formation mechanism of the BHJ. Finally, we have performed a comparative study of the BHJ film formation dynamics during spin coating versus wire-bar coating of p-DTS(FBTTh2)2: fullerene blends that has helped in curbing the performance gap between lab-based and scalable techniques. This was done by implementing a new apparatus that combines the benefits of rapid thin film drying common to spin coating with scalability of wire-bar coating. Using the new apparatus, we successfully attain similar performance of solar cell devices to the ones fabricated by spin coating with dramatically reduced material waste.
Date of AwardDec 5 2016
Original languageEnglish (US)
Awarding Institution
  • Physical Sciences and Engineering
SupervisorAram Amassian (Supervisor)


  • Organic photovoltaics
  • In situ characterization
  • Microstructure evolution
  • Solution processing
  • Scalable processing
  • Highthroughput fabrication

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