Xuezhi Zheng

Nonlinear superchiral meta-surfaces: Tuning chirality and disentangling non-reciprocity at the nanoscale

Circularly polarized light is incident on a nanostructured chiral meta-surface. In the nanostructured unit cells whose chirality matches that of light, superchiral light is forming and strong optical second harmonic generation can be observed.

The origin of second harmonic generation hotspots in chiral optical metamaterials [Invited]

Recently, a great amount of research has been triggered by the prediction, formulated by Pendry and co-authors, that novel and enhanced nonlinear optical phenomena could be observed in metamaterials.[1] This prediction is based on the fact that, in metamaterials, local field enhancements can have a dramatic influence over the optical properties of the material. One of the largest contributions to such local field enhancements is attributable to surface plasmon resonances. Plasmons are collective oscillations of the electrons under the influence of lights electromagnetic field. Plasmons occur naturally on the surfaces of homogeneous metal films, where they usually dissipate quickly and cancel each others influence. However, upon patterning the metal surface at the nanoscale, plasmons can be manipulated in a manner similar to classical waveguiding, whereby propagation or standing wave patterns can be achieved. In other words, artificial structuring allows for nanoengineering the position and intensity of the local fields. Incidentally, nonlinear optical effects, such as second-, third-, or forth-harmonic generation, scale as the second, third or fourth power of the electromagnetic intensity, respectively. Therefore, it is perfectly reasonable to assume that the large electromagnetic local field enhancements in metamaterials should yield large or previously unobserved nonlinear optical effects.

Plasmon-Enhanced Sub-Wavelength Laser Ablation: Plasmonic Nanojets

In response to the incident lights electric field, the electron density oscillates in the plasmonic hotspots producing an electric current. Associated Ohmic losses raise the temperature of the material within the plasmonic hotspot above the melting point. A nanojet and nanosphere ejection can then be observed precisely from the plasmonic hotspots.

U-Shaped Switches for Optical Information Processing at the Nanoscale

4–6 ] In such devices, light waves would be used instead of electrons. The possibility arises from the fact that light waves can couple to collective excitations of electrons at the surfaces of metallic nanostructures, a prop-erty referred to as surface plasmon resonance. Because these optically induced resonances occur at the surfaces and interfaces of the nanostructures, they can readily be investigated with a surface- and interface-specifi c optical technique, such as second-harmonic generation (SHG). SHG is a nonlinear optical technique that, within the dipole approximation, is forbidden in materials with a center of symmetry. Consequently, SHG is highly sensitive to regions with broken symmetry, such as surfaces (or interfaces), and it has been successfully applied to the study of plasmonic nano-materials with different geometries.

The role of chiral local field enhancements below the resolution limit of Second Harmonic Generation microscopy

While it has been demonstrated that, above its resolution limit, Second Harmonic Generation (SHG) microscopy can map chiral local field enhancements, below that limit, structural defects were found to play a major role. Here we show that, even below the resolution limit, the contributions from chiral local field enhancements to the SHG signal can dominate over those by structural defects. We report highly homogeneous SHG micrographs of star-shaped gold nanostructures, where the SHG circular dichroism effect is clearly visible from virtually every single nanostructure. Most likely, size and geometry determine the dominant contributions to the SHG signal in nanostructured systems.

Volumetric Method of Moments and Conceptual Multilevel Building Blocks for Nanotopologies

On the basis of the relationship between charge dimensionality and singular field behavior, it is proven that in a volumetric description of a volume current carrying topology, half rooftops of different binary hierarchical level are allowed without introducing numerical difficulties. This opens the possibility to use a very efficient multilevel hierarchical meshing scheme in a volumetric method-of-moments (V-MoM) algorithm. The new meshing scheme is validated by numerical calculations and experiments. It paves the way toward a much more efficient use of MoM in the description of arbitrarily shaped nanostructures at infrared and optical frequencies.

Distributing the Optical Near‐Field for Efficient Field‐Enhancements in Nanostructures

We are grateful to Saloomeh Shariati from the crypto group in the Universite Catholique de Louvain, for helpful discussion on the measures of the uniformity in images. We acknowledge financial support from the fund for scientific research Flanders (FWO-V), the K. U. Leuven (CREA, GOA), Methusalem Funding by the Flemish government and the Belgian Inter-University Attraction Poles IAP Programmes. V. K. V. and S. V. are grateful for the support from the FWO-Vlaanderen. B. DC. is thankful to the IWT.

Line Position and Quality Factor of Plasmonic Resonances Beyond the Quasi-Static Limit: A Full-Wave Eigenmode Analysis Route

In this study, we introduce a rigorous full-wave eigenmode analysis technique based on a volumetric method of moments to the optical spectrum. We first apply this technique to a nanorod as an example to illustrate how the real part of the eigenfrequency and the modal quality factor (defined as the ratio of the real part of the eigenfrequency to the imaginary part) together with the eigenmode determine the line position and quality factor of a resonance and the corresponding resonant mode. Then, the eigenfrequencies and eigenmodes of a composite plasmonic nanostructure, a Dolmen, and its two individual constituents, a dimer and a monomer, are extracted. The line position of the Fano dip in Dolmens spectrum is discussed by examining the relative positions of the eigenfrequencies of the dimer and the monomer in the complex plane. Further, the formation of the Fano dip is reinterpreted as the destructive interference between the nonorthogonal eigenmodes of the whole Dolmen structure. The proposed full-wave modal analysis brings a new perspective on understanding and designing the plasmonic response of nanoantennae beyond the quasi-static limit.

Revealing Nanostructures through Plasmon Polarimetry

Polarized optical dark-field spectroscopy is shown to be a versatile noninvasive probe of plasmonic structures that trap light to the nanoscale. Clear spectral polarization splittings are found to be directly related to the asymmetric morphology of nanocavities formed between faceted gold nanoparticles and an underlying gold substrate. Both experiment and simulation show the influence of geometry on the coupled system, with spectral shifts Δλ = 3 nm from single atoms. Analytical models allow us to identify the split resonances as transverse cavity modes, tightly confined to the nanogap. The direct correlation of resonance splitting with atomistic morphology allows mapping of subnanometre structures, which is crucial for progress in extreme nano-optics involving chemistry, nanophotonics, and quantum devices.

On the Use of Group Theory in Understanding the Optical Response of a Nanoantenna

Symmetry holds a prominent position in defining the optical response of a nanoantenna. In this work, we harness a mathematical tool, group representation theory, combine it with the eigenmode analysis for a nanoantenna, and illustrate how the symmetry allows or forbids the energetic coupling (i.e., interference) between a nanoantennas eigenmodes. We do this especially using a nanobar structure and a symmetric cross structure. Further, the consequence of symmetry-breaking is illustrated by an asymmetric cross-shaped nanostructure, i.e., a strong asymmetric Fano-type resonance line shape due to mode interference is observed with the physics behind elaborated. Both numerical and experimental evidences are provided.