Controlling Nanoparticle Distance by On-Surface DNA-Origami Folding.

DNA origami is a flexible platform for the precise organization of nano-objects, enabling numerous applications from biomedicine to nano-photonics. Its huge potential stems from its high flexibility that allows customized structures to meet specific requirements. The ability to generate diverse final structures from a common base by folding significantly enhances design variety and is regularly occurring in liquid. This study describes a novel approach that combines top-down lithography with bottom-up DNA origami techniques to control folding of the DNA origami with the adsorption on pre-patterned surfaces. Using this approach, tunable plasmonic dimer nano-arrays are fabricated on a silicon surface. This involves employing electron beam lithography to create adsorption sites on the surface and utilizing self-organized adsorption of DNA origami functionalized with two gold nanoparticles (AuNPs). The desired folding of the DNA origami helices can be controlled by the size and shape of the adsorption sites. This approach can for example be used to tune the center-to-center distance of the AuNPs dimers on the origami template. To demonstrate this technique's efficiency, the Raman signal of dye molecules (carboxy tetramethylrhodamine, TAMRA) coated on the AuNPs surface are investigated. These findings highlight the potential of tunable DNA origami-based plasmonic nanostructures for many applications.

Positional control of DNA origami based gold dimer hybrid nanostructures on pre-structured surfaces.

This study explores important parameters for achieving a high-level positional control of DNA-nanoparticle hybrid structures by drop-casting onto a pre-structured silicon surface, in which the active adsorption sites were defined using electron beam lithography. By confining the adsorption sites to the scale of the DNA origami, we create multi-dimensional patterns and study the effect of diffusion and hybrid nanostructure concentration in the liquid on site occupation. We also propose a physical diffusion model that highlights the importance of surface diffusion in facilitating the adsorption of hybrid nanostructure onto active sites, particularly for two and one-dimensional adsorption sites. Our study shows prominent results of the hybrid nanostructure's selective adsorption, indicating high adsorption efficiency and precise control over the position, as well as the spatial orientation. We anticipate similar results in related systems, both in terms of different surfaces and similar DNA structures. Overall, our findings offer promising prospects for the development of large-scale nanoarrays on micrometer-scale surfaces with nanometer precision and orientation control.

Optical Tomography of Polymeric Microsphere Layers Using Confocal Raman Microscopy.

In confocal Raman microscopy, depth profiling is a key application that enables analysis of the structural and chemical composition and size of three-dimensional (3D) transparent objects. However, the precise interpretation of a probed sample's Raman depth profile measurement can be significantly affected by both its size and surrounding objects. This study provides a more comprehensive understanding of the observed optical effects at the interface between polymer spheres and different substrates. Ray- and wave-optical simulations support our results. We derive a correction factor that, depending on the instrumental configuration, allows us to determine the nominal dimensions of the scanned objects more accurately from Raman depth profiles. Our studies support the need for careful consideration when employing depth profiling in confocal Raman microscopy for nondestructive, quantitative tomography of 3D objects.

Confocal Raman Microscopy for the Analysis of the Three-Dimensional Shape of Polymeric Microsphere Layers.

The reconstruction of the three-dimensional (3D) morphology of polymeric microsphere layers based on confocal Raman microscopy was studied. Refraction of the Raman laser beam at the curved surface of the spheres broadens the focus volume inside the sphere. Compared to planar layers, the focus gets trapped inside the spheres such that the measured depth profiles are shifted and broadened. Additionally, the Raman signal of the underlying substrate is already observed for nominal focus positions above the microsphere layer. The results are successfully modeled with ray-optical simulations that allow for a clear understanding of the relevant mechanisms that lead to the generation of the Raman signals in the complex three-dimensional structures.

Nonlinear optical potassium niobate nanocrystals as harmonic markers: the role of precursors and stoichiometry in hydrothermal synthesis.

Nanocrystals of alkaline niobates are currently being discussed for various applications because of their diverse and remarkable properties. Although the growth of bulk niobate crystals is well established, little is known about respective nanocrystals and the optical properties of niobates below 100 nm. A systematic view of the hydrothermal synthesis of potassium niobate with respect to the precursor species reveals the sensitive dependence of the resulting crystalline phases and sizes on the educt modifications. With a variation of stoichiometry of the procedure, the product modification and crystallite size can be changed. By means of second harmonic generation, nanocrystalline potassium niobate offers the possibility for use as an optical marker in high resolution nonlinear microscopy. Redispersed particles show a significant second harmonic generation signal throughout the visible spectral range.