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DNA-mediated nanoparticle crystallization into Wulff polyhedra

机译：DNA介导的纳米颗粒结晶成Wulff多面体

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摘要

Crystallization is a fundamental and ubiquitous process much studied over the centuries. But although the crystallization of atoms is fairly well understood, it remains challenging to predict reliably the outcome of molecular crystallization processes that are complicated by various molecular interactions and solvent involvement. This difficulty also applies to nanoparticles: high-quality three-dimensional crystals are mostly produced using drying and sedimentation techniques that are often impossible to rationalize and control to give a desired crystal symmetry, lattice spacing and habit (crystal shape). In principle, DNA-mediated assembly of nanoparticles offers an ideal opportunity for studying nanoparticle crystallization: a well-defined set of rules have been developed to target desired lattice symmetries and lattice constants, and the occurrence of features such as grain boundaries and twinning in DNA superlattices and traditional crystals comprised of molecular or atomic building blocks suggests that similar principles govern their crystallization. But the presence of chafed biomolecules, interpar-tide spacings of tens of nanometres, and the realization so far of only polycrystalline DNA-interconnected nanoparticle superlattices, all suggest that DNA-guided crystallization may differ from traditional crystal growth. Here we show that very slow cooling, over several days, of solutions of complementary-DNA-modified nanoparticles through the melting temperature of the system gives the thermodynamic product with a specific and uniform crystal habit. We find that our nanoparticle assemblies have the Wulff equilibrium crystal structure that is predicted from theoretical considerations and molecular dynamics simulations, thus establishing that DNA hybridization can direct nanoparticle assembly along a pathway that mimics atomic crystallization.
机译：结晶是一个基本且普遍存在的过程，已有数百年的历史了。但是，尽管对原子的结晶已相当了解，但要可靠地预测因各种分子相互作用和溶剂参与而复杂化的分子结晶过程的结果仍然具有挑战性。这种困难也适用于纳米粒子：高质量的三维晶体大多是使用干燥和沉降技术生产的，而这些技术通常无法合理化和控制以提供所需的晶体对称性，晶格间距和习性（晶体形状）。原则上，DNA介导的纳米粒子组装为研究纳米粒子的结晶提供了理想的机会：已经开发出一套明确的规则以针对所需的晶格对称性和晶格常数，以及出现诸如晶界和孪晶之类的特征由分子或原子结构单元组成的超晶格和传统晶体表明，相似的原理控制着它们的结晶。但是，存在被摩擦的生物分子，数十纳米的粒子间距以及迄今为止仅实现了多晶DNA互连的纳米粒子超晶格的存在，所有这些都表明DNA引导的结晶可能与传统晶体的生长不同。在这里，我们显示了互补DNA修饰的纳米粒子溶液在几天内通过系统的熔融温度非常缓慢地冷却，使热力学产物具有特定且均匀的晶体习性。我们发现我们的纳米粒子组件具有Wulff平衡晶体结构，这是从理论考虑和分子动力学模拟预测的，从而确定了DNA杂交可以沿着模拟原子结晶的途径引导纳米粒子组件。

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  • 来源
    《Nature》 |2014年第7481期|73-77|共5页
  • 作者

    Evelyn Auyeung; Ting I. N. G. Li; Andrew J. Senesi; Abrin L. Schmucker; Bridget C. Pals; Monica Olvera de la Cruz; Chad A. Mirkin;

  • 作者单位

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA;

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA;

    International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA,Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA;

    International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA,Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA;

    International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA;

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA,Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA;

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,International Institute for Nanotechnology, Northwestern University, Evanston, Illinois 60208.USA,Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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