Audible sound-controlled spatiotemporal patterns in out-of-equilibrium systems

Abstract

Naturally occurring spatiotemporal patterns typically have a predictable pattern design and are reproducible over several cycles. However, the patterns obtained from artificially designed out-of-equilibrium chemical oscillating networks (such as the Belousov–Zhabotinsky reaction for example) are unpredictable and difficult to control spatiotemporally, albeit reproducible over subsequent cycles. Here, we show that it is possible to generate reproducible spatiotemporal patterns in out-of-equilibrium chemical reactions and self-assembling systems in water in the presence of sound waves, which act as a guiding physical stimulus. Audible sound-induced liquid vibrations control the dissolution of atmospheric gases (such as O2 and CO2) in water to generate spatiotemporal chemical patterns in the bulk of the fluid, segregating the solution into spatiotemporal domains having different redox properties or pH values. It further helps us in the organization of transiently formed supramolecular aggregates in a predictable spatiotemporal manner.

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Fig. 1: Sound-controlled spatiotemporal patterns.
Fig. 2: Sound-controlled redox-specific domains and spatiotemporal patterns.
Fig. 3: Sound-controlled pH-specific domains and spatiotemporal patterns.
Fig. 4: Sound-controlled organization of supramolecular aggregates in spatiotemporal patterns.

Data availability

The authors declare that the data supporting the findings of this study are available within the paper and its Supplementary Information files.

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Acknowledgements

We thank I.S. Kang (POSTECH) and S. Shin (Hongik University) for helpful discussions on fluid dynamics and the Faraday instability. This work was supported by the Institute for Basic Science (IBS) [IBS-R007-D1].

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Affiliations

Authors

Contributions

I.H., R.D.M. and K.K. conceived the idea and designed the experiments. S.-Y.K., I.H., P.D. and S.C. synthesized the materials. P.D., R.D.M., S.C. and I.H. participated in pattern generation and other associated experiments. Y.H.K. helped in NMR experiments. K.B. performed cryo-transmission electron microscopy experiments. All authors discussed the results, analysed the data and commented on the manuscript. K.K. supervised the overall research.

Corresponding authors

Correspondence to Ilha Hwang or Rahul Dev Mukhopadhyay or Kimoon Kim.

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The authors declare no competing interests.

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Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Synthesis and characterization of compounds, Supplementary Figs. 1–20 and references.

Supplementary Video 1

Pattern generation with the MV2+/MV•+ redox couple at 40Hz. The video is played 20 times faster than real time.

Supplementary Video 2

Pattern generation with the SF0/SF+ redox couple at 40Hz. The video is played two times slower than real time.

Supplementary Video 3

Pattern generation experiments under the inert atmosphere and in air. No pattern was observed in an inert atmosphere, but a spatiotemporal pattern was generated from air exposure.

Supplementary Video 4

Slow motion video of surface wave pattern at 40Hz. The video was recorded at 960 frames per second and is played 128 times slower than real time.

Supplementary Video 5

Self-healing behaviour of the pattern. The preformed pattern was disturbed with a syringe needle while keeping the sound source on and the collapsed pattern was recovered after a while.

Supplementary Video 6

Dynamic interchange between patterns. As the vibration frequency of the solution changes, the resulting patterns also change accordingly.

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Hwang, I., Mukhopadhyay, R.D., Dhasaiyan, P. et al. Audible sound-controlled spatiotemporal patterns in out-of-equilibrium systems. Nat. Chem. 12, 808–813 (2020). https://doi.org/10.1038/s41557-020-0516-2

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