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Double-helical assembly of heterodimeric nanoclusters into supercrystals

Author

Listed:
  • Yingwei Li

    (Carnegie Mellon University)

  • Meng Zhou

    (University of Miami)

  • Yongbo Song

    (Anhui Medical University)

  • Tatsuya Higaki

    (Carnegie Mellon University)

  • He Wang

    (University of Miami)

  • Rongchao Jin

    (Carnegie Mellon University)

Abstract

DNA has long been used as a template for the construction of helical assemblies of inorganic nanoparticles1–5. For example, gold nanoparticles decorated with DNA (or with peptides) can create helical assemblies6–9. But without such biological ligands, helices are difficult to achieve and their mechanism of formation is challenging to understand10,11. Atomically precise nanoclusters that are protected by ligands such as thiolate12,13 have demonstrated hierarchical structural complexity in their assembly at the interparticle and intraparticle levels, similar to biomolecules and their assemblies14. Furthermore, carrier dynamics can be controlled by engineering the structure of the nanoclusters15. But these nanoclusters usually have isotropic structures16,17 and often assemble into commonly found supercrystals18. Here we report the synthesis of homodimeric and heterodimeric gold nanoclusters and their self-assembly into superstructures. While the homodimeric nanoclusters form layer-by-layer superstructures, the heterodimeric nanoclusters self-assemble into double- and quadruple-helical superstructures. These complex arrangements are the result of two different motif pairs, one pair per monomer, where each motif bonds with its paired motif on a neighbouring heterodimer. This motif pairing is reminiscent of the paired interactions of nucleobases in DNA helices. Meanwhile, the surrounding ligands on the clusters show doubly or triply paired steric interactions. The helical assembly is driven by van der Waals interactions through particle rotation and conformational matching. Furthermore, the heterodimeric clusters have a carrier lifetime that is roughly 65 times longer than that of the homodimeric clusters. Our findings suggest new approaches for increasing complexity in the structural design and engineering of precision in supercrystals.

Suggested Citation

  • Yingwei Li & Meng Zhou & Yongbo Song & Tatsuya Higaki & He Wang & Rongchao Jin, 2021. "Double-helical assembly of heterodimeric nanoclusters into supercrystals," Nature, Nature, vol. 594(7863), pages 380-384, June.
  • Handle: RePEc:nat:nature:v:594:y:2021:i:7863:d:10.1038_s41586-021-03564-6
    DOI: 10.1038/s41586-021-03564-6
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    Citations

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    Cited by:

    1. Yuan Wang & Dian Niu & Guanghui Ouyang & Minghua Liu, 2022. "Double helical π-aggregate nanoarchitectonics for amplified circularly polarized luminescence," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Yongbo Song & Yingwei Li & Meng Zhou & Hao Li & Tingting Xu & Chuanjun Zhou & Feng Ke & Dayujia Huo & Yan Wan & Jialong Jie & Wen Wu Xu & Manzhou Zhu & Rongchao Jin, 2022. "Atomic structure of a seed-sized gold nanoprism," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    3. Li-Juan Liu & Fahri Alkan & Shengli Zhuang & Dongyi Liu & Tehseen Nawaz & Jun Guo & Xiaozhou Luo & Jian He, 2023. "Atomically precise gold nanoclusters at the molecular-to-metallic transition with intrinsic chirality from surface layers," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Chang Liu & Yan Zhao & Tai-Song Zhang & Cheng-Bo Tao & Wenwen Fei & Sheng Zhang & Man-Bo Li, 2023. "Asymmetric transformation of achiral gold nanoclusters with negative nonlinear dependence between chiroptical activity and enantiomeric excess," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Liang Qiao & Nia Pollard & Ravithree D. Senanayake & Zhi Yang & Minjung Kim & Arzeena S. Ali & Minh Tam Hoang & Nan Yao & Yimo Han & Rigoberto Hernandez & Andre Z. Clayborne & Matthew R. Jones, 2023. "Atomically precise nanoclusters predominantly seed gold nanoparticle syntheses," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    6. Jun Guo & Yulong Duan & Yunling Jia & Zelong Zhao & Xiaoqing Gao & Pai Liu & Fangfang Li & Hongli Chen & Yutong Ye & Yujiao Liu & Meiting Zhao & Zhiyong Tang & Yi Liu, 2024. "Biomimetic chiral hydrogen-bonded organic-inorganic frameworks," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    7. Zhan-Hua Zhao & Bao-Liang Han & Hai-Feng Su & Qi-Lin Guo & Wen-Xin Wang & Jing-Qiu Zhuo & Yong-Nan Guo & Jia-Long Liu & Geng-Geng Luo & Ping Cui & Di Sun, 2024. "Buckling cluster-based H-bonded icosahedral capsules and their propagation to a robust zeolite-like supramolecular framework," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    8. Yuan Zhong & Jiangwei Zhang & Tingting Li & Wenwu Xu & Qiaofeng Yao & Min Lu & Xue Bai & Zhennan Wu & Jianping Xie & Yu Zhang, 2023. "Suppression of kernel vibrations by layer-by-layer ligand engineering boosts photoluminescence efficiency of gold nanoclusters," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    9. Nan Xia & Jianpei Xing & Di Peng & Shiyu Ji & Jun Zha & Nan Yan & Yan Su & Xue Jiang & Zhi Zeng & Jijun Zhao & Zhikun Wu, 2022. "Assembly-induced spin transfer and distance-dependent spin coupling in atomically precise AgCu nanoclusters," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    10. Hao Li & Tian Wang & Jiaojiao Han & Ying Xu & Xi Kang & Xiaosong Li & Manzhou Zhu, 2024. "Fluorescence resonance energy transfer in atomically precise metal nanoclusters by cocrystallization-induced spatial confinement," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    11. Xue-Jing Zhai & Meng-Yu Luo & Xi-Ming Luo & Xi-Yan Dong & Yubing Si & Chong Zhang & Zhen Han & Runping Han & Shuang-Quan Zang & Thomas C. W. Mak, 2024. "Hierarchical assembly of Ag40 nanowheel ranging from building blocks to diverse superstructure regulation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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