Charge carrier dynamics at organic interfaces for polymer photovoltaics

Mariateresa Scarongella
EPFL, 2015
Thèse EPFL

The increased energy demand and the importance to find renewable energy resources have been addressed by a scientific effort to improve the power conversion efficiency of organic solar cells. In particular, polymer-based solar cells have experienced a great increase in power conversion efficiency, which recently reached a value over 10%. The possibility to further improve the performance of polymer-based solar cells has encouraged the research to have a close look at the key parameters, which play an important role in the mechanism of charge generation. Specifically, the photo-physical processes and the time scales involved in converting excitons to charges are still poorly understood. Also, the microscopic origin and the nature of the driving force allowing interfacial electron-hole pairs to become free charges and the role played by the sample microstructure in a bulk heterojunction have to be clarified. We have used transient absorption spectroscopy, which provides information about the excited states dynamics with

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Mariateresa Scarongella
EPFL, 2015
Thèse EPFL

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https://infoscience.epfl.ch/record/209137?ln=fr

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PBDTTPD is one of the best conjugated polymers for solar cell applications (up to 8.5% efficiency). We have investigated the dynamics of charge generation in the blend with fullerene (PCBM) and addressed highly relevant topics such as the role of bulk heterojunction structure, fullerene excitation, and excess energy. We show that there are multiple charge separation pathways. These include electron transfer from photoexcited polymer, hole transfer from photoexcited PCBM, prompt (

Amer Chemical Soc2014

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The influence of microstructure on charge separation dynamics in organic bulk heterojunction materials for solar cell applications

Natalie Renuka Banerji, Jacques-Edouard Moser, Arun Aby Paraecattil, Mariateresa Scarongella, Natalie Stingelin

Light-induced charge formation is essential for the generation of photocurrent in organic solar cells. In order to gain a better understanding of this complex process, we have investigated the femtosecond dynamics of charge separation upon selective excitation of either the fullerene or the polymer in different bulk heterojunction blends with well-characterized microstructure. Blends of the pBTTT and PBDTTPD polymers with PCBM gave us access to three different scenarios: either a single intermixed phase, an intermixed phase with additional pure PCBM clusters, or a three-phase microstructure of pure polymer aggregates, pure fullerene clusters and intermixed regions. We found that ultrafast charge separation (by electron or hole transfer) occurs predominantly in intermixed regions, while charges are generated more slowly from excitons in pure domains that require diffusion to a charge generation site. The pure domains are helpful to prevent geminate charge recombination, but they must be sufficiently small not to become exciton traps. By varying the polymer packing, backbone planarity and chain length, we have shown that exciton diffusion out of small polymer aggregates in the highly efficient PBDTTPD:PCBM blend occurs within the same chain and is helped by delocalization.

Royal Soc Chemistry2014

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A Close Look at Charge Generation in Polymer:Fullerene Blends with Microstructure Control

Natalie Renuka Banerji, Jacques-Edouard Moser, Jelissa Risse, Mariateresa Scarongella, Natalie Stingelin

We reveal some of the key mechanisms during charge generation in polymer:fullerene blends exploiting our well-defined understanding of the microstructures obtained in pBTTT:PCBM systems via processing with fatty acid methyl ester additives. Based on ultrafast transient absorption, electro-absorption, and fluorescence up-conversion spectroscopy, we find that exciton diffusion through relatively phase-pure polymer or fullerene domains limits the rate of electron and hole transfer, while prompt charge separation occurs in regions where the polymer and fullerene are molecularly intermixed (such as the co-crystal phase where fullerenes intercalate between polymer chains in pBTTT:PCBM). We moreover confirm the importance of neat domains, which are essential to prevent geminate recombination of bound electron–hole pairs. Most interestingly, using an electro-absorption (Stark effect) signature, we directly visualize the migration of holes from intermixed to neat regions, which occurs on the subpicosecond time scale. This ultrafast transport is likely sustained by high local mobility (possibly along chains extending from the co-crystal phase to neat regions) and by an energy cascade driving the holes toward the neat domains.

Amer Chemical Soc2015

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