Martin Fruhnert

Dynamically self-assembled silver nanoparticles as a thermally tunable metamaterial

The availability of metamaterials with properties that can be actively tuned is crucial for the future development of various metamaterial-based technologies. Here we show that by using silver nanoparticles equipped with a thermally responsive organic coating a metamaterial is obtained with reversibly switchable properties. The material investigated exhibits dynamic self-assembly resulting from temperature-dependent changes of organic coating shape, which translates to a switchable spatial distribution of the silver nanoparticles. This in turn strongly influences the optical properties of the entire material. The measured optical characteristics of the material are in excellent agreement with theoretical calculations, which allow us to use the latter to predict a dynamically tunable epsilon-near-zero behaviour of the metamaterial. The suggested methodology opens new routes for tunable metamaterials that operate in the visible region and will enable various applications for soft-matter-based optical devices.

Towards negative index self-assembled metamaterials

We investigate the magnetic response of meta-atoms that can be fabricated by a bottom-up technique. Usually such meta-atoms consist of a dielectric core surrounded by a large number of solid metallic nanoparticles. In contrast to those meta-atoms considered thus far, we study here for the first time hollow metallic nanoparticles (shells). In doing so we solve one of the most pertinent problems of current self-assembled metamaterials, namely implementing meta-atoms with sufficiently large resonance strength and small absorption. Both conditions have to be met for deep sub-wavelength meta-atoms to obtain effectively homogeneous metamaterials which may be meaningfully described by negative material parameters. Eventually we show that by using these findings self-assembled negative index materials come in reach.

Dual and chiral objects for optical activity in general scattering directions

Optically active artificial structures have attracted tremendous research attention. Such structures must meet two requirements: Lack of spatial inversion symmetries and, a condition usually not explicitly considered, the structure shall preserve the helicity of light, which implies that there must be a vanishing coupling between the states of opposite polarization handedness among incident and scattered plane waves. Here, we put forward and demonstrate that a unit cell made from chiraly arranged electromagnetically dual scatterers serves exactly this purpose. We prove this by demonstrating optical activity of such unit cell in general scattering directions.

Objects of Maximum Electromagnetic Chirality

We introduce a definition of the electromagnetic chirality of an object and show that it has an upper bound. Reciprocal objects attain the upper bound if and only if they are transparent for all the fields of one polarization handedness (helicity). Additionally, electromagnetic duality symmetry, i.e., helicity preservation upon interaction, turns out to be a necessary condition for reciprocal objects to attain the upper bound. We use these results to provide requirements for the design of such extremal objects. The requirements can be formulated as constraints on the polarizability tensors for dipolar objects or on the material constitutive relations for continuous media. We also outline two applications for objects of maximum electromagnetic chirality: a twofold resonantly enhanced and background-free circular dichroism measurement setup, and angle-independent helicity filtering glasses. Finally, we use the theoretically obtained requirements to guide the design of a specific structure, which we then analyze numerically and discuss its performance with respect to maximal electromagnetic chirality.

Tunable scattering cancellation cloak with plasmonic ellipsoids in the visible

The scattering cancellation technique is a powerful tool to reduce the scattered field from electrically small objects in a specific frequency window. The technique relies on covering the object of interest with a shell that scatters light into the far field of equal strength as the object, but

Refraction limit of miniaturized optical systems: a ball-lens example

\pi

Optical force and torque on dipolar dual chiral particles

out-of-phase. The resulting destructive interference prohibits its detection in measurements that probe the scattered light. Whereas at radio or microwave frequencies feasible designs have been proposed that allow to tune the operational frequency upon request, similar capabilities have not yet been explored in the visible. However, such ability is decisive to capitalize on the technique in many envisioned applications. Here, we solve the problem and study the use of small metallic nanoparticles with an ellipsoidal shape as the material from which the shell is made to build an isotropic geometry. Changing the aspect ratio of the ellipsoids allows to change the operational frequency. The basic functionality is explored with two complementary analytical approaches. Additionally, we present a powerful multiscattering algorithm that can be used to perform full wave simulations of clusters of arbitrary particles. We utilize this method to analyze the scattering of the presented designs numerically. Hereby we provide useful guidelines for the fabrication of this cloak with self-assembly methods by investigating the effects of disorder.

Plasmonic nanoparticle clusters with tunable plasmonic resonances in the visible spectral region

We study experimentally and theoretically the electromagnetic field in amplitude and phase behind ball-lenses across a wide range of diameters, ranging from a millimeter scale down to a micrometer. Based on the observation, we study the transition between the refraction and diffraction regime. The former regime is dominated by observables for which it is sufficient to use a ray-optical picture for an explanation, e.g., a cusp catastrophe and caustics. A wave-optical picture, i.e. Mie theory, is required to explain the features, e.g., photonic nanojets, in the latter regime. The vanishing of the cusp catastrophe and the emergence of the photonic nanojet is here understood as the refraction limit. Three different criteria are used to identify the limit: focal length, spot size, and amount of cross-polarization generated in the scattering process. We identify at a wavelength of 642 nm and while considering ordinary glass as the ball-lens material, a diameter of approximately 10 µm as the refraction limit. With our study, we shed new light on the means necessary to describe micro-optical system. This is useful when designing optical devices for imaging or illumination.

Computing the T-matrix of a scattering object with multiple plane wave illuminations

On the one hand, electromagnetic dual particles preserve the helicity of light upon interaction. On the other hand, chiral particles respond differently to light of opposite helicity. These two properties on their own constitute a source of fascination. Their combined action, however, is less explored. Here, we study on analytical grounds the force and torque as well as the optical cross sections of dual chiral particles in the dipolar approximation exerted by a particular wave of well-defined helicity: A circularly polarized plane wave. We put emphasis on particles that possess a maximally electromagnetic chiral and hence dual response. Besides the analytical insights, we also investigate the exerted optical force and torque on a real particle using the example of a metallic helix that is designed to approach the maximal electromagnetic chirality condition. Various applications in the context of optical sorting but also nanorobotics can be foreseen considering the particles studied in this contribution.

Correction: Computing the T-matrix of a scattering object with multiple plane wave illuminations

The seeded growth of poly(ethylene imine) – gold nanoparticle clusters enables the formation of particle assemblies with tunable optical properties. Clusters with increasing particle sizes, filling factors and assemblies consisting of PEI–gold–silver core shell particles can be synthesized in this way. Profound structural characterization is carried out via TEM imaging and FIB milling which allows visualizing the cross-section of the clusters. Determination of the optical properties was performed via UV-Vis spectroscopy and spectral dark field microscopy of individual particles. Additionally, numerical calculations were carried out based on the Mie theory. The results are in good agreement with the experimental findings and reveal the contribution of different multipoles to the spectra which cannot be resolved by UV-Vis spectroscopy in solution. The isotropic nature and adjustable properties of these clusters could render them versatile building blocks for metamaterials.