期刊
NANO LETTERS
卷 11, 期 12, 页码 5564-5573出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl203559s
关键词
Gold nanoparticles; polypeptides; folding; helix-loop-helix; small angle X-ray scattering (SAXS)
类别
资金
- Knut and Alice Wallenberg Foundation (KAW)
- EPSRC
- ERC
- Swedish Research Council (VR)
- Swedish Foundation for Strategic Research (SSF)
- Ministerio de Ciencia e Innovacion of Spain
- Australian synchrotron [AS093/SAXS1875]
- EPSRC [EP/E007627/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/E007627/1] Funding Source: researchfish
Responsive hybrid nanomaterials with well-defined properties are of significant interest for the development of biosensors with additional applications in tissue engineering and drug delivery. Here, we present a detailed characterization using UV-vis spectroscopy and small angle X-ray scattering of a hybrid material comprised of polypeptide-decorated gold nanoparticles with highly controllable assembly properties. The assembly is triggered by a folding-dependent bridging of the particles mediated by the heteroassociation of immobilized helix-loop-helix polypeptides and a complementary nonlinear polypeptide present in solution. The polypeptides are de novo designed to associate and fold into a heterotrimeric complex comprised of two disulfide-linked four-helix bundles. The particles form structured assemblies with a highly defined interparticle gap (4.8 +/- 0.4 nm) that correlates to the size of the folded polypeptides. Transitions in particle aggregation dynamics, mass-fractal dimensions and ordering, as a function of particle size and the concentration of the bridging polypeptide, are observed; these have significant effects on the optical properties of the assemblies. The assembly and ordering of the particles are highly complex processes that are affected by a large number of variables including the number of polypeptides bridging the particles and the particle mobility within the aggregates. A fundamental understanding of these processes is of paramount interest for the development of novel hybrid nanomaterials with tunable structural and optical properties and for the optimization of nanoparticle-based colorimetric biodetection strategies.
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