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Tying different knots in a molecular strand

Author

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  • David A. Leigh

    (East China Normal University
    University of Manchester)

  • Fredrik Schaufelberger

    (University of Manchester)

  • Lucian Pirvu

    (University of Manchester)

  • Joakim Halldin Stenlid

    (AlbaNova University Center, Stockholm University)

  • David P. August

    (University of Manchester)

  • Julien Segard

    (University of Manchester)

Abstract

The properties of knots are exploited in a range of applications, from shoelaces to the knots used for climbing, fishing and sailing1. Although knots are found in DNA and proteins2, and form randomly in other long polymer chains3,4, methods for tying5 different sorts of knots in a synthetic nanoscale strand are lacking. Molecular knots of high symmetry have previously been synthesized by using non-covalent interactions to assemble and entangle molecular chains6–15, but in such instances the template and/or strand structure intrinsically determines topology, which means that only one type of knot is usually possible. Here we show that interspersing coordination sites for different metal ions within an artificial molecular strand enables it to be tied into multiple knots. Three topoisomers—an unknot (01) macrocycle, a trefoil (31) knot6–15, and a three-twist (52) knot—were each selectively prepared from the same molecular strand by using transition-metal and lanthanide ions to guide chain folding in a manner reminiscent of the action of protein chaperones16. We find that the metal-ion-induced folding can proceed with stereoinduction: in the case of one knot, a lanthanide(iii)-coordinated crossing pattern formed only with a copper(i)-coordinated crossing of particular handedness. In an unanticipated finding, metal-ion coordination was also found to translocate an entanglement from one region of a knotted molecular structure to another, resulting in an increase in writhe (topological strain) in the new knotted conformation. The knot topology affects the chemical properties of the strand: whereas the tighter 52 knot can bind two different metal ions simultaneously, the looser 31 isomer can bind only either one copper(i) ion or one lutetium(iii) ion. The ability to tie nanoscale chains into different knots offers opportunities to explore the modification of the structure and properties of synthetic oligomers, polymers and supramolecules.

Suggested Citation

  • David A. Leigh & Fredrik Schaufelberger & Lucian Pirvu & Joakim Halldin Stenlid & David P. August & Julien Segard, 2020. "Tying different knots in a molecular strand," Nature, Nature, vol. 584(7822), pages 562-568, August.
  • Handle: RePEc:nat:nature:v:584:y:2020:i:7822:d:10.1038_s41586-020-2614-0
    DOI: 10.1038/s41586-020-2614-0
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    Cited by:

    1. Zhiyu Qu & Jing Fang & Yu-Xiang Wang & Yibin Sun & Yajie Liu & Wen-Hao Wu & Wen-Bin Zhang, 2023. "A single-domain green fluorescent protein catenane," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Jiaqi Liang & Shuai Lu & Yang Yang & Yun-Jia Shen & Jin-Ku Bai & Xin Sun & Xu-Lang Chen & Jie Cui & Ai-Jiao Guan & Jun-Feng Xiang & Xiaopeng Li & Heng Wang & Yu-Dong Yang & Han-Yuan Gong, 2023. "Thermally-induced atropisomerism promotes metal-organic cage construction," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Ling-Jun Kong & Weixuan Zhang & Peng Li & Xuyue Guo & Jingfeng Zhang & Furong Zhang & Jianlin Zhao & Xiangdong Zhang, 2022. "High capacity topological coding based on nested vortex knots and links," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    4. Jing Wang & Deshan Liang & Jing Ma & Yuanyuan Fan & Ji Ma & Hasnain Mehdi Jafri & Huayu Yang & Qinghua Zhang & Yue Wang & Changqing Guo & Shouzhe Dong & Di Liu & Xueyun Wang & Jiawang Hong & Nan Zhang, 2023. "Polar Solomon rings in ferroelectric nanocrystals," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    5. Zhiwen Li & Jingjing Zhang & Gao Li & Richard J. Puddephatt, 2024. "Self-assembly of the smallest and tightest molecular trefoil knot," Nature Communications, Nature, vol. 15(1), pages 1-6, December.

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