Stefan Mühlig

Engineering photonic nanojets

Photonic Nanojets are highly localized wave fields emerging directly behind dielectric microspheres; if suitably illuminated. In this contribution we reveal how different illumination conditions can be used to engineer the photonic Nanojets by measuring them in amplitude and phase with a high resolution interference microscope. We investigate how the wavelength, the amplitude distribution of the illumination, its polarization, or a break in symmetry of the axial-symmetric structure and the illumination affect the position, the localization and the shape of the photonic Nanojets. Various fascinating properties are systematically revealed and their implications for possible applications are discussed.

Self-assembled plasmonic core shell clusters with an isotropic magnetic dipole response in the visible range

We theoretically analyze, fabricate, and characterize a three-dimensional plasmonic nanostructure that exhibits a strong and isotropic magnetic response in the visible spectral domain. Using two different bottom-up approaches that rely on self-organization and colloidal nanochemistry, we fabricate clusters consisting of dielectric core spheres, which are smaller than the wavelength of the incident radiation and are decorated by a large number of metallic nanospheres. Hence, despite having a complicated inner geometry, such a core-shell particle is sufficiently small to be perceived as an individual object in the far field. The optical properties of such complex plasmonic core-shell particles are discussed for two different core diameters.

Cloaking dielectric spherical objects by a shell of metallic nanoparticles

We show that dielectric spheres can be cloaked by a shell of amorphously arranged metallic nanoparticles. The shell represents an artificial medium with tunable effective properties that can be adjusted such that the scattered signals of shell and sphere almost cancel each other. We provide an analytical model for the cloak design and prove numerically that the cloak operates as desired. We show that more than 70% of the scattered signal of the sphere can be suppressed at the design wavelength. Advantages and disadvantages of such a cloak when compared to other implementations are disclosed.

Optical properties of a fabricated self-assembled bottom-up bulk metamaterial

We investigate the optical properties of a true three-dimensional metamaterial that was fabricated using a self-assembly bottom-up technology. The metamaterial consists of closely packed spherical clusters being formed by a large number of non-touching gold nanoparticles. After presenting experimental results, we apply a generalized Mie theory to analyze its spectral response revealing that it is dominated by a magnetic dipole contribution. By using an effective medium theory we show that the fabricated metamaterial exhibits a dispersive effective permeability, i.e. artificial magnetism. Although this metamaterial is not yet left-handed it might serve as a starting point for achieving bulk metamaterials by using bottom-up approaches.

A bottom-up approach to fabricate optical metamaterials by self-assembled metallic nanoparticles

We introduce a novel bottom-up approach to fabricate by self assembly a metamaterial from metallic nanoparticles in a two-step process. In the first step, a metamaterial made of densely packed silver nanoparticles is required. The material dispersion with increasing nanoparticle densities, from dispersed to randomly packed nanoparticles, was measured by spectroscopic ellipsometry, demonstrating high permittivity values in the visible. In the second step, this material was used to prepare spherical clusters by a method based on oil-in-water emulsion. The optical properties of these clusters were equally investigated by spectroscopic means. Comparisons with rigorous numerical simulations clearly indicate that, depending on the cluster size, their spectral response can be unambiguously associated with the excitation of a magnetic dipole resonance. As a consequence, such spherical clusters are promising building blocks for future metamaterials possessing a magnetic response in the visible range.

Controlling the dynamics of quantum mechanical systems sustaining dipole-forbidden transitions via optical nanoantennas

We suggest to excite dipole-forbidden transitions in quantum mechanical systems by using appropriately designed optical nanoantennas. The antennas are tailored such that their near field contains sufficiently strong contributions of higher-order multipole moments. The strengths of these moments exceed their free-space analogs by several orders of magnitude. The impact of such excitation enhancement is exemplarily investigated by studying the dynamics of a three-level system. It decays upon excitation by an electric quadrupole transition via two electric dipole transitions. Since one dipole transition is assumed to be radiative, the enhancement of this emission serves as a figure of merit. Such self-consistent treatment of excitation, emission, and internal dynamics as developed in this contribution is the key to predict any observable quantity. The suggested scheme may represent a blueprint for future experiments and will find many obvious spectroscopic and sensing applications.

Gouy phase anomaly in photonic nanojets

We investigate in real space amplitude and phase distributions of light in photonic nanojets emerging from micrometer-sized dielectric spheres with a high-resolution interference microscope. Strong localization of light and a Gouy phase anomaly are witnessed. We show that the phase advance of photonic nanojets significantly deviates from a plane wave due to the sudden transition from a converging to a diverging wave front. Understanding such phase anomalies and verifying the presence of photonic nanojets promises to pave the way to prospective applications that may exploit the ability to localize light in spatial domains smaller than the usual resolution limit.

Self-assembled plasmonic metamaterials

Abstract Nowadays for the sake of convenience most plasmonic nanostructures are fabricated by top-down nanofabrication technologies. This offers great degrees of freedom to tailor the geometry with unprecedented precision. However, it often causes disadvantages as well. The structures available are usually planar and periodically arranged. Therefore, bulk plasmonic structures are difficult to fabricate and the periodic arrangement causes undesired effects, e.g., strong spatial dispersion is observed in metamaterials. These limitations can be mitigated by relying on bottom-up nanofabrication technologies. There, self-assembly methods and techniques from the field of colloidal nanochemistry are used to build complex functional unit cells in solution from an ensemble of simple building blocks, i.e., in most cases plasmonic nanoparticles. Achievable structures are characterized by a high degree of nominal order only on a short-range scale. The precise spatial arrangement across larger dimensions is not possible in most cases; leading essentially to amorphous structures. Such self-assembled nanostructures require novel analytical means to describe their properties, innovative designs of functional elements that possess a desired near- and far-field response, and entail genuine nanofabrication and characterization techniques. Eventually, novel applications have to be perceived that are adapted to the specifics of the self-assembled nanostructures. This review shall document recent progress in this field of research. Emphasis is put on bottom-up amorphous metamaterials. We document the state-of-the-art but also critically assess the problems that have to be overcome.

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.

The spectral shift between near- and far-field resonances of optical nano-antennas.

Within the past several years a tremendous progress regarding optical nano-antennas could be witnessed. It is one purpose of optical nano-antennas to resonantly enhance light-matter interactions at the nanoscale, e.g. the interaction of an external illumination with molecules. In this specific, but in almost all schemes that take advantage of resonantly enhanced electromagnetic fields in the vicinity of nano-antennas, the precise knowledge of the spectral position of resonances is of paramount importance to fully exploit their beneficial effects. Thus far, however, many nano-antennas were only optimized with respect to their far-field characteristics, i.e. in terms of their scattering or extinction cross sections. Although being an emerging feature in many numerical simulations, it was only recently fully appreciated that there exists a subtle but very important difference in the spectral position of resonances in the near-and the far-field. With the purpose to quantify this shift, Zuloaga et al. suggested a Lorentzian model to estimate the resonance shift. Here, we devise on fully analytical grounds a strategy to predict the resonance in the near-field directly from that in the far-field and disclose that the issue is involved and multifaceted, in general. We outline the limitations of our theory if more sophisticated optical nano-antennas are considered where higher order multipolar contributions and higher order antenna resonances become increasingly important. Both aspects are highlighted by numerically studying relevant nano-antennas.