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Molecular crystallization directed by polymer size and overlap under dilute and crowded macromolecular conditions

Polymer Journal volume 53, pages 633–642 (2021)Cite this article

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Abstract

We demonstrate that dissolved polymers can direct molecular crystallization behavior under dilute and crowded conditions. Larger poly(ethylene glycol)s (PEGs) accelerated caffeine crystal formation in the dilute regime of PEG solutions, which was attributed to the depletion attraction that promoted caffeine cluster aggregation into crystal nuclei. Alternatively, in the semidilute regime, the caffeine crystal formation rate was insensitive to the molecular weight (MW) of PEGs. PEGs with various MWs appeared to induce depletion attraction to a similar extent as the properties of polymer solutions in the semidilute regime described by blobs, which are constant in size at a given polymer concentration irrespective of MW. This study highlights differences between in vitro polymer solutions and crowded intracellular environments composed of folded biomacromolecules and contributes to developing the use of in vitro macromolecular crowding for the control of molecular self-assembly.

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Acknowledgements

This work was supported by the Japan Society for the Promotion of Science (JSPS) KAKENHI, grant number JP20J01280 for YH. YH is grateful to JSPS for the Research Fellowship for Young Scientists. The XRD experiment was performed at SAXS-U (General User Program of Neutron Science Laboratory, Institute for Solid State Physics, The University of Tokyo) located in Ibaraki Quantum Beam Research Center, Tokai, Japan.

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  1. Department of Bioengineering, Graduate School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan

    Yuuki Hata, Ung-il Chung & Takamasa Sakai

  2. Division of Biomedical Engineering, National Defense Medical College Research Institute, 3-2 Namiki, Tokorozawa-shi, Saitama, 359-8513, Japan

    Yuuki Hata

  3. Institute for Solid State Physics, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa-shi, Chiba, 277-8581, Japan

    Xiang Li

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  1. Yuuki Hata
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Correspondence to Yuuki Hata or Takamasa Sakai.

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Hata, Y., Li, X., Chung, Ui. et al. Molecular crystallization directed by polymer size and overlap under dilute and crowded macromolecular conditions. Polym J 53, 633–642 (2021). https://doi.org/10.1038/s41428-021-00461-7

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