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Predictive modelling of structure formation in semiconductor films produced by meniscus-guided coating

Nature Materials volume 20, pages 68–75 (2021)Cite this article

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A Publisher Correction to this article was published on 01 October 2020

A Publisher Correction to this article was published on 22 September 2020

An Author Correction to this article was published on 28 August 2020

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Abstract

Meniscus-guided coating methods, such as zone casting, dip coating and solution shearing, are scalable laboratory models for large-area solution coating of functional materials for thin-film electronics. Unfortunately, the general lack of understanding of how the coating parameters affect the dry-film morphology upholds trial-and-error experimentation and delays lab-to-fab translation. We present herein a model that predicts dry-film morphologies produced by meniscus-guided coating of a crystallizing solute. Our model reveals how the interplay between coating velocity and evaporation rate determines the crystalline domain size, shape anisotropy and regularity. If coating is fast, evaporation drives the system quickly past supersaturation, giving isotropic domain structures. If coating is slow, depletion due to crystallization stretches domains in the coating direction. The predicted morphologies have been experimentally confirmed by zone-casting experiments of the organic semiconductor 4-tolyl-bithiophenyl-diketopyrrolopyrrole. Although here we considered a small molecular solute, our model can be applied broadly to polymers and organic–inorganic hybrids such as perovskites.

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Fig. 1: Schematic representation of the computational domain and coating process.
Fig. 2: Computational and experimental morphologies.
Fig. 3: Order parameter profiles and approach to steady state.
Fig. 4: Mapping of the parameter space determined by coating speed and evaporation rate.
Fig. 5: Film thickness, initial concentration and simulated crystalline morphology as a function of coating speed and evaporation rate.
Fig. 6: Overview of the numerical simulations: domain statistics, order parameter profiles, parameter space mapping and aligned morphologies.

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Data availability

The data represented in Figs. 2c,d, 3, 5a–c and 6a,b are available online at https://edmond.mpdl.mpg.de/imeji/collection/uF7qtH6vi9ocht7q?q=. Other data from the current study are available from the corresponding author upon reasonable request.

Code availability

The code that support the findings of this study are available from the corresponding author upon reasonable request.

Change history

  • 21 August 2020

    In the PDF version of this Article originally published, some of the equations in the Methods section were incorrect. The HTML version, however, was correct. The PDF has now been updated.

  • 28 August 2020

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

  • 22 September 2020

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

  • 01 October 2020

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

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Acknowledgements

The authors acknowledge P. W. M. Blom for stimulating discussions. K.Z. acknowledges the China Scholarship Council (CSC) for financial support. T.M. acknowledges the Foundation for Polish Science financed by the European Union under the European Regional Development Fund (POIR.04.04.00-00-3ED8/17-01).

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Authors and Affiliations

  1. Max Planck Institute for Polymer Research, Mainz, Germany

    Jasper J. Michels, Ke Zhang, Wojciech Pisula & Tomasz Marszalek

  2. Physical Sciences and Engineering Division, KAUST Solar Center (KSC), King Abdullah University of Science and Technology (KAUST), Thuwal, Saudi Arabia

    Philipp Wucher & Pierre M. Beaujuge

  3. Department of Molecular Physics, Faculty of Chemistry, Lodz University of Technology, Lodz, Poland

    Wojciech Pisula & Tomasz Marszalek

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Contributions

J.J.M. developed the model, performed numerical simulations and analysed the results of calculations; K.Z. performed zone-casting experiments and morphological analysis; P.W. and P.M.B. synthesized and characterized DPP(Th2Bn)2; W.P. and T.M. assisted in the interpretation of the results of calculations; J.J.M., K.Z., W.P. and T.M. contributed to the writing of this manuscript.

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Correspondence to Jasper J. Michels.

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Supplementary information

Supplementary Information

Synthesis details and spectra, supplementary discussion, Figs. S1–S13 and Tables S1–S5.

Supplementary Video 1

Video of coating of aligned domains.

Supplementary Video 2

Video of coating of stretched domains.

Supplementary Video 3

Video of coating of isotropic domains.

Supplementary Video 4

Video of coating of isotropic domains for a large field-of-view.

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Michels, J.J., Zhang, K., Wucher, P. et al. Predictive modelling of structure formation in semiconductor films produced by meniscus-guided coating. Nat. Mater. 20, 68–75 (2021). https://doi.org/10.1038/s41563-020-0760-2

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