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1.
Faraday Discuss ; 191: 159-176, 2016 10 06.
Artigo em Inglês | MEDLINE | ID: mdl-27411967

RESUMO

We demonstrate a template-assisted colloidal self-assembly approach for magnetic metasurfaces on macroscopic areas. The choice of anisotropic colloidal particle geometry, assembly pattern and metallic film is based on rational design criteria, taking advantage of mirror-charge effects for gold nanorods placed on gold film. Monodisperse gold nanorods prepared utilizing wet-chemistry are arranged with high precision on wrinkled templates to form linear array-type assemblies and subsequently transferred to a thin gold film. Due to the obtained particle-to-film distance of 1.1 nm, the plasmonic mode of the nanorod is able to couple efficiently with the supporting metallic film, giving rise to a magnetic mode in the visible spectrum (721 nm). Conventional UV-vis-NIR measurements in close correlation with electromagnetic simulations provide evidence for the presence of a magnetic resonance on the macroscopic area. The herein presented scalable lithography-free fabrication process paves the road towards colloidal functional metasurfaces with an optical response in the effective magnetic permeability.

2.
ACS Nano ; 16(2): 3383-3393, 2022 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-35112848

RESUMO

Polymer brushes, consisting of densely end-tethered polymers to a surface, can exhibit rapid and sharp conformational transitions due to specific stimuli, which offer intriguing possibilities for surface-based sensing of the stimuli. The key toward unlocking these possibilities is the development of methods to readily transduce signals from polymer conformational changes. Herein, we report on single-fluorophore integrated ultrathin (<40 nm) polymer brush surfaces that exhibit changing fluorescence properties based on polymer conformation. The basis of our methods is the change in occupied volume as the polymer brush undergoes a collapse transition, which enhances the effective concentration and aggregation of the integrated fluorophores, leading to a self-quenching of the fluorophores' fluorescence and thereby reduced fluorescence lifetimes. By using fluorescence lifetime imaging microscopy, we reveal spatial details on polymer brush conformational transitions across complex interfaces, including at the air-water-solid interface and at the interface of immiscible liquids that solvate the surface. Furthermore, our method identifies the swelling of polymer brushes from outside of a direct droplet (i.e., the polymer phase with vapor above), which is controlled by humidity. These solvation-sensitive surfaces offer a strong potential for surface-based sensing of stimuli-induced phase transitions of polymer brushes with spatially resolved output in high resolution.

3.
Nanoscale ; 11(38): 17655-17663, 2019 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-31535119

RESUMO

The optical properties of nanoparticle assemblies can be tailored via hybridization of plasmon modes. Isotropic core/satellite superstructures made of spherical nanoparticles are known to exhibit coupled modes with a strongly scattering (radiative) character, and provide hot spots yielding high activity in surface-enhanced Raman scattering (SERS). However, to complement this functionality with plasmonic heating, additional absorbing (non-radiative) modes are required. We introduce herein anisotropic superstructures formed by decorating a central nanorod with spherical satellite nanoparticles, which feature two coupled modes that allow application for both SERS and heating. On the basis of diffuse reflectance spectroscopy, small-angle X-ray scattering (SAXS), and electromagnetic simulations, the origin of the coupled modes is disclosed and thus serves as a basis toward alternative designs of functional superstructures. This work represents a proof-of-principle for the combination of high SERS efficiency with efficient plasmonic heating by near-infrared irradiation.

4.
Nanoscale ; 9(27): 9376-9385, 2017 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-28656183

RESUMO

Nanorattles are metallic core-shell particles with core and shell separated by a dielectric spacer. These nanorattles have been identified as a promising class of nanoparticles, due to their extraordinary high electric-field enhancement inside the cavity. Limiting factors are reproducibility and loss of axial symmetry owing to the movable metal core; movement of the core results in fluctuation of the nanocavity dimensions and commensurate variations in enhancement factor. We present a novel synthetic approach for the robust fixation of the central gold rod within a well-defined box, which results in an axisymmetric nanorattle. We determine the structure of the resulting axisymmetric nanorattles by advanced transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS). Optical absorption and scattering cross-sections obtained from UV-vis-NIR spectroscopy quantitatively agree with finite-difference time-domain (FDTD) simulations based on the structural model derived from SAXS. The predictions of high and homogenous field enhancement are evidenced by scanning TEM electron energy loss spectroscopy (STEM-EELS) measurement on single-particle level. Thus, comprehensive understanding of structural and optical properties is achieved for this class of nanoparticles, paving the way for photonic applications where a defined and robust unit cell is crucial.

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