Understanding chemical degradation at the interface between different layers in an organic photovoltaic device (OPV) is crucial to improving the long‐term stability of OPVs. Herein, molecular‐level insights are provided into the impact of different metal top electrodes on the interfacial morphology and stability of photoactive layers in PM6:Y6 bulk‐heterojunction (BHJ) OPVs. OPVs with an aluminum (Al) top electrode exhibit inferior stability compared to silver (Ag) electrode devices upon thermal annealing, whereby thermal stress induces the diffusion of both Al and Ag atoms to the PM6:Y6 BHJ layer. The diffused Al atoms cause surface recombination at the interface between the photoactive layer and an interlayer. Specifically, X‐ray photoelectron spectroscopy suggests the different local chemical environments of PM6 and Y6 moieties in PM6:Y6/Al‐contact devices. These results are corroborated by solid‐state nuclear magnetic resonance and electron paramagnetic resonance spectroscopy measurements, indicating the formation of ionic and organo‐metallic‐like species at the sub‐layers of the PM6:Y6 BHJ morphology, which are estimated to be less than 5 wt% of the PM6:Y6/Al blend. By comparison, the Ag atoms do not adversely affect PM6:Y6 BHJ morphology and the associated device physics. The investigation of reactive electrode‐BHJ interfaces by multiscale characterization techniques and device physics is expected to provide guidance to future interfacial engineering strategies to develop stable and efficient OPVs.
Casting of a donor:acceptor bulk‐heterojunction structure from a single ink has been the predominant fabrication method of organic photovoltaics (OPVs). Despite the success of such bulk heterojunctions, the task ofcontrolling the microstructure in a single casting process has been arduous and alternative approaches are desired. To achieve OPVs with a desirable microstructure, a facile and eco‐compatible sequential deposition approach is demonstrated for polymer/small‐molecule pairs. Using a nominally amorphous polymer as the model material, the profound influence of casting solvent is shown on the molecular ordering of the film, and thus the device performance and mesoscale morphology of sequentially deposited OPVs can be tuned. Static and in situ X‐ray scattering indicate that applying (R)‐(+)‐limonene is able to greatly promote the molecular order of weakly crystalline polymers and form the largest domain spacing exclusively, which correlates well with the best efficiency of 12.5% in sequentially deposited devices. The sequentially cast device generally outperforms its control device based on traditional single‐ink bulk‐heterojunction structure. More crucially, a simple polymer:solvent interaction parameter χ is positively correlated with domain spacing in these sequentially deposited devices. These findings shed light on innovative approaches to rationally create environmentally friendly and highly efficient electronics.
more » « less- Award ID(s):
- 1639429
- NSF-PAR ID:
- 10444677
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 31
- Issue:
- 17
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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