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Spin-on deposition of amorphous zeolitic imidazolate framework films for lithography applications

Nature Chemical Engineering volume 2, pages 594–607 (2025)Cite this article

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Abstract

Amorphous zeolitic imidazolate framework (aZIF) films have been recently introduced as resists for electron beam and extreme ultraviolet lithography. aZIFs are also being considered for separation applications, including thin film membranes. However, the reported methods for aZIF deposition are currently based on highly empirical trial-and-error approaches that hinder control of film composition, thickness and uniformity as well as scale-up and transferability to different coating geometries. This work presents a method for depositing aZIF films with controllable thickness using dilute precursors mixed immediately before encountering the substrate. Importantly, the method is amenable to quantitative analysis by computational fluid dynamics to extract intrinsic deposition rates and limiting reactant transport diffusivities, enabling predictive physics-based modeling of the deposition process. This allows the deposition method to be adapted for spin coating on silicon wafers to prepare high-quality aZIF films with consistently controlled thickness. Using this approach, high-resolution resist performance and wafer-scale use for beyond extreme-ultraviolet lithography of aZIF films is demonstrated.

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Fig. 1: Flow coating of aZIF-Zn/2mIm films.
Fig. 2: Computational model for flow coating and comparison with experiments.
Fig. 3: Spin coating simulations and experiments.
Fig. 4: CLD of aZIF films with various compositions.
Fig. 5: EBL patterning of aZIF films.

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Data availability

All data generated during this study are included in the article and the Supplementary Information and/or from the corresponding authors on request. Data, models and code generated or used during the CFD simulation are available from L.Z. on request. Source data are provided with this paper.

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Acknowledgements

All experimental work, except EBL and BEUVL experiments, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-SC0021212. IRRAS, XPS and XRD experiments were carried out at the Center for Functional Nanomaterials at Brookhaven National Laboratory, supported by the US Department of Energy, Office of Basic Energy Sciences, under contract no. DE-SC0012704. We thank D. Nykypanchuk and X. Tong for support with XRD and XPS. We thank K. Gaskell and Y. Niu for their support with XPS experiments. L.Z. acknowledges financial support (for the computational modeling-CFD simulations) from the National Natural Science Foundation of China (22078091) and Shanghai Pujiang Program (2022PJD016). Additional support to M.T. to perform EBL experiments was provided by the Bloomberg Distinguished Professorship Program at JHU. Support for some EBL and the BEUVL experiments was provided by the National Science Foundation (NSF ECCS-2428276). We acknowledge Blue-X Resist sub-TWG for access to BEUV, and D. L. Goldfarb (IBM T.J. Watson Research Center) for coordinating the BEUV experiments. This research utilized resources of the Advanced Light Source, which is a US DOE Office of Science User Facility, under contract no. DE-AC02-05CH11231.

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Author notes

  1. These authors contributed equally: Shunyi Zheng, Kayley E. Waltz, Mueed Ahmad.

Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering and Institute for NanoBioTechnology, Johns Hopkins University, Baltimore, MD, USA

    Yurun Miao, Kayley E. Waltz, Xinpei Zhou & Michael Tsapatsis

  2. School of Chemical Engineering, East China University of Science and Technology, Shanghai, China

    Shunyi Zheng, Yegui Zhou, Heting Wang & Liwei Zhuang

  3. Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY, USA

    Mueed Ahmad & J. Anibal Boscoboinik

  4. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, USA

    Mueed Ahmad & J. Anibal Boscoboinik

  5. College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China

    Qi Liu

  6. Laboratory of Advanced Separations, École Polytechnique Fédérale de Lausanne, Sion, Switzerland

    Kumar Varoon Agrawal

  7. Center for X-Ray Optics, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Oleg Kostko

  8. Applied Physics Laboratory, Johns Hopkins University, Laurel, MD, USA

    Michael Tsapatsis

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  1. Yurun Miao
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Contributions

Y.M. designed and made the CLD flow reactor and performed all flow and spin coating depositions and characterizations by AFM and SEM and some of the XPS experiments. S.Z. performed and analyzed all CFD simulations aided by Y.Z. and H.W. under the direction of L.Z. K.E.W. and X.Z. contributed to the negative tone EBL and BEUVL experiments, MLD depositions and vapor phase development experiments. M.A. contributed the IRRAS, XPS and XRD characterization under the direction of J.A.B. K.V.A. and Q.L. contributed conceptualization of deposition under ultradilute conditions and film characterization. O.K. performed the BEUVL exposures and contributed to BEUV data analysis. L.Z. directed all CFD simulation aspects. M.T. conceived the CLD concept, developed the approximate analysis of the flow coating experiments and directed the overall project. Y.M., L.Z., S.Z. and M.T. wrote the paper with input from all co-authors. All authors discussed the results and contributed to the final paper.

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Correspondence to Liwei Zhuang or Michael Tsapatsis.

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Miao, Y., Zheng, S., Waltz, K.E. et al. Spin-on deposition of amorphous zeolitic imidazolate framework films for lithography applications. Nat Chem Eng 2, 594–607 (2025). https://doi.org/10.1038/s44286-025-00273-z

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