Modeling of surface-induced second-harmonic generation from multilayer structures by the transfer matrix method.

We analytically and numerically investigate surface second-harmonic generation (SHG) from a stack of dielectric layers. We develop a theoretical formalism based on the transfer matrix method for the calculation of the surface-driven second-harmonic radiation from multilayer structures and elaborate it for the case of ultrathin dielectric layers using a power series expansion to derive the effective surface nonlinear tensor for the whole stack. We show that for deeply subwavelength thicknesses of the layers the surface responses from all interfaces can efficiently sum up, leading to largely enhanced efficiency of SHG. As a result, such surface-driven nonlinearity can become comparable to the bulk nonlinearity in noncentrosymmetric semiconductors and can yield high performance for nonlinear nanophotonic applications.

Far-field polarization signatures of surface optical nonlinearity in noncentrosymmetric semiconductors.

We analyse possibilities to quantitatively evaluate the surface second-order optical nonlinearity in noncentrosymmetric materials based on polarization-resolved analysis of far-field radiation patterns of second-harmonic generation. We analytically demonstrate that for plane-wave illumination the contribution to the second-harmonic signal from the surface of a nonlinear medium exhibits different polarization properties and angular dependencies compared to the contribution from the bulk. In view of this, we optimize the illumination geometry in order to enable the most efficient separation and comparison of both nonlinearities. Furthermore, we consider the illumination of an AlGaAs slab by a tightly-focused linearly-polarized Gaussian beam as an alternative measurement geometry. It is found that the reliable separation of the surface nonlinearity contribution as well as a wide range of detectable values can be achieved with this geometry as well.

Disorder-Induced Phase Transitions in the Transmission of Dielectric Metasurfaces.

Light interaction with disordered materials is both complex and fascinating at the same time. Here, we reveal disorder-induced phase transitions in a dielectric Huygens' metasurface made from silicon nanocylinders that simultaneously support an electric and magnetic dipole resonance. Depending on the degree of positional disorder and the spectral detuning of the two resonances, the phase angle of the transmission coefficient exhibits a clear phase transition from normal to anomalous dispersion. Combined with the considerations of whether the resonances of spectrally detuned particles appear as separated or overlapping, we distinguish four different phase states. We study this phenomenon analytically by employing dipole particles and disclose the entire phase diagram, support our insights with full-wave simulations of actual structures, and corroborate the findings with experimental results. Unveiling this phenomenon is a milestone simultaneously in the growing fields of metamaterial-inspired silicon nanophotonics, photonics in disordered media, and the fundamental physics of phase transitions.

High resolution XUV Fourier transform holography on a table top.

Today, coherent imaging techniques provide the highest resolution in the extreme ultraviolet (XUV) and X-ray regions. Fourier transform holography (FTH) is particularly unique, providing robust and straightforward image reconstruction at the same time. Here, we combine two important advances: First, our experiment is based on a table-top light source which is compact, scalable and highly accessible. Second, we demonstrate the highest resolution ever achieved with FTH at any light source (34 nm) by utilizing a high photon flux source and cutting-edge nanofabrication technology. The performance, versatility and reliability of our approach allows imaging of complex wavelength-scale structures, including wave guiding effects within these structures, and resolving embedded nanoscale features, which are invisible for electron microscopes. Our work represents an important step towards real-world applications and a broad use of XUV imaging in many areas of science and technology. Even nanoscale studies of ultra-fast dynamics are within reach.

Strong coupling in hybrid metal-dielectric nanoresonators.

We study resonant photonic-plasmonic coupling between a gold dipole nanoantenna and a silicon nanodisc supporting electric and magnetic dipolar Mie-type resonances. Specifically, we consider two different cases for the mode structure of the silicon nanodisc, namely spectrally separate and spectrally matching electric and magnetic dipolar Mie-type resonances. In the latter case, the dielectric nanoparticle scatters the far fields of a unidirectional Huygens' source. Our results reveal an anticrossing of the plasmonic dipole resonance and the magnetic Mie-type dipole resonance of the silicon nanodisc, accompanied by a clear signature of photonic-plasmonic mode hybridization in the corresponding mode profiles. These characteristics show that strong coupling is established between the two different resonant systems in the hybrid nanostructure. Furthermore, our results demonstrate that in comparison with purely metallic or dielectric nanostructures, hybrid metal-dielectric nanoresonators offer higher flexibility in tailoring the fractions of light which are transmitted, absorbed and reflected by the nanostructure over a broad range of parameters without changing its material composition. As a special case, highly asymmetric reflection and absorption properties can be achieved.This article is part of the themed issue 'New horizons for nanophotonics'.

Electro-optically spectrum narrowed, multiline intracavity optical parametric oscillators.

We report on the first building of an active spectral narrowing mechanism in a pulsed, multiline optical parametric oscillator (OPO) based on a novel aperiodically poled lithium niobate (APPLN) device constructed using the aperiodic optical superlattice technique. The APPLN device functions simultaneously in the system as a multi-channel optical parametric down converter (OPDC) and an electro-optic (EO) gain spectral filter working on the corresponding (multiple) signal bands. When the APPLN OPO was installed in a diode pumped Nd:YVO4 laser system, highly narrowed dual-wavelength signal lines (at 1540 and 1550 nm) were observed at the output of the system through EO control of the APPLN. Correspondingly, an enhancement of the power spectral density of the source by a factor of ~7.8 with respect to the system operated in passive mode was found.

High speed and high resolution table-top nanoscale imaging.

We present a table-top coherent diffractive imaging (CDI) experiment based on high-order harmonics generated at 18 nm by a high average power femtosecond fiber laser system. The high photon flux, narrow spectral bandwidth, and high degree of spatial coherence allow for ultrahigh subwavelength resolution imaging at a high numerical aperture. Our experiments demonstrate a half-pitch resolution of 15 nm, close to the actual Abbe limit of 12 nm, which is the highest resolution achieved from any table-top extreme ultraviolet (XUV) or x-ray microscope. In addition, sub-30 nm resolution was achieved with only 3 s of integration time, bringing live diffractive imaging and three-dimensional tomography on the nanoscale one step closer to reality. The current resolution is solely limited by the wavelength and the detector size. Thus, table-top nanoscopes with only a few-nanometer resolutions are in reach and will find applications in many areas of science and technology.

Image formation properties and inverse imaging problem in aperture based scanning near field optical microscopy.

Aperture based scanning near field optical microscopes are important instruments to study light at the nanoscale and to understand the optical functionality of photonic nanostructures. In general, a detected image is affected by both the transverse electric and magnetic field components of light. The discrimination of the individual field components is challenging as these four field components are contained within two signals in the case of a polarization resolved measurement. Here, we develop a methodology to solve the inverse imaging problem and to retrieve the vectorial field components from polarization and phase resolved measurements. Our methodology relies on the discussion of the image formation process in aperture based scanning near field optical microscopes. On this basis, we are also able to explain how the relative contributions of the electric and magnetic field components within detected images depend on the chosen probe. We can therefore also describe the influence of geometrical and material parameters of individual probes within the image formation process. This allows probes to be designed that are primarily sensitive either to the electric or magnetic field components of light.

Adiabatic light transfer in titanium diffused lithium niobate waveguides.

We report on the realization of adiabatic light transfer in lithium niobate (LiNbO3) waveguides. This peculiar adiabatic tunneling scheme was implemented in a three-waveguide coupling configuration with the intermediate waveguide being inclined with respect to the outer waveguides to facilitate the adiabatic passage process. We have investigated and determined the adiabatic conditions of the LiNbO3 device in terms of the structure configuration of the waveguide system and found optimal structure parameters by both simulation and experimental approaches. Broadband adiabatic couplings of bandwidth ~456 and 185 nm and peak coupling efficiencies of >0.96 have been obtained with a 2-cm long device for TE- and TM-polarized fundamental modes, respectively. Longer (5 cm) devices were also studied and found to be useful in increasing the adiabaticity of the device, especially for the TM-polarized mode.

Electro-optically spectrum tailorable intracavity optical parametric oscillator.

We report a unique, pulsed intracavity optical parametric oscillator (IOPO) whose output spectrum is electro-optically (EO) tailorable based on an aperiodically poled lithium niobate (APPLN) working simultaneously as an optical parametric gain medium and an active gain spectrum filter in the system. We have successfully obtained from the IOPO the emission of single to multiple narrow-line signal spectral peaks in a near-infrared (1531 nm) band simply by electro-optic control. The power spectral density of the EO tailored signal can be enhanced by up to 10 times over the original (nontailored) signal.

Resonant metasurfaces at oblique incidence: interplay of order and disorder.

Understanding the impact of order and disorder is of fundamental importance to perceive and to appreciate the functionality of modern photonic metasurfaces. Metasurfaces with disordered and amorphous inner arrangements promise to mitigate problems that arise for their counterparts with strictly periodic lattices of elementary unit cells such as, e.g., spatial dispersion, and allows the use of fabrication techniques that are suitable for large scale and cheap fabrication of metasurfaces. In this study, we analytically, numerically and experimentally investigate metasurfaces with different lattice arrangements and uncover the influence of lattice disorder on their electromagnetic properties. The considered metasurfaces are composed of metal-dielectric-metal elements that sustain both electric and magnetic resonances. Emphasis is placed on understanding the effect of the transition of the lattice symmetry from a periodic to an amorphous state and on studying oblique illumination. For this scenario, we develop a powerful analytical model that yields, for the first time, an adequate description of the scattering properties of amorphous metasurfaces, paving the way for their integration into future applications.

Core-shell potassium niobate nanowires for enhanced nonlinear optical effects.

We demonstrate the synthesis as well as the optical characterization of core-shell nanowires. The wires consist of a potassium niobate (KNbO3) core and a gold shell. The nonlinear optical properties of the core are combined with the plasmonic resonance of the shell and offer an enhanced optical signal in the near infrared spectral range. We compare two different functionalization schemes of the core material prior to the shell growth process: silanization and polyelectrolyte. We show that the latter leads to a smoother and complete core-shell nanostructure and an easier-to-use synthesis process. A Mie-theory based theoretical approach is presented to model the enhanced second-harmonic generated (SHG) signal of the core-shell wires, illustrating the influence of the fabrication-induced varying geometrical factors of wire radius and shell thickness. A spectroscopic measurement on a core-shell nanowire shows a strong localized surface plasmon resonance close to 900 nm, which matches with the SHG resonance obtained from nonlinear optical experiments with the same nanowire. According to the simulation, this corresponds to a wire radius of 35 nm and a shell thickness of 7.5 nm. By comparing SHG signals measured from an uncoated nanowire and the coated one, we obtain a 250 times enhancement factor. This is less than the calculated enhancement, which considers a cylindrical nanowire with a perfectly smooth shell. Thus, we explain this discrepancy mainly with the roughness of the synthesized gold shell.

Combining randomly textured surfaces and photonic crystals for the photon management in thin film microcrystalline silicon solar cells.

Photon management aims at optimizing the solar cell efficiency by, e.g., incorporating supporting optical nanostructures for absorption enhancement. Their geometrical design, however, is usually a compromise since requirements in different spectral domains need to be accommodated. This issue can be mitigated if multiple optical nanostructures are integrated. Here, we present a photon management scheme that combines the benefits of a randomly textured surface and an opaline photonic crystal. Moreover, upon considering the device with an increasing complexity, we show that a structure that respects the mutual fabrication constraints has the best performance, i.e., a device where the photonic crystal is not perfect but to some extent amorphous as enforced by the presence of the texture.

Single and multilayer metamaterials fabricated by nanoimprint lithography.

We demonstrate for the first time a fast and easy nanoimprint lithography (NIL) based stacking process of negative index structures like fishnet and Swiss-cross metamaterials. The process takes a few seconds, is cheap and produces three-dimensional (3D) negative index materials (NIMs) on a large area which is suitable for mass production. It can be performed on all common substrates even on flexible plastic foils. This work is therefore an important step toward novel and breakthrough applications of NIMs such as cloaking devices, perfect lenses and magnification of objects using NIM prisms. The optical properties of the fabricated samples were measured by means of transmission and reflection spectroscopy. From the measured data we retrieved the effective refractive index which is shown to be negative for a wavelength around 1.8 µm for the fishnet metamaterial while the Swiss-cross metamaterial samples show a distinct resonance at wavelength around 1.4 µm.

Optical properties of metamaterials based on asymmetric double-wire structures.

We performed theoretical and experimental investigations of the magnetic properties of metamaterials based on asymmetric double-wire structures. Using the multipole model for the description of metamaterials, we investigated the influence of the geometrical asymmetry of the structure on the macroscopic effective parameters. The results show that the larger wire in the system dominates the dynamics of the structure and defines the orientation and the strength of the microscopic currents. As a result the magnetization of the structure can be significantly enhanced for certain asymmetric configurations of the double-wire structure.

Asymmetric transmission of linearly polarized light at optical metamaterials.

We experimentally demonstrate a three-dimensional chiral optical metamaterial that exhibits an asymmetric transmission for forwardly and backwardly propagating linearly polarized light. The observation of this novel effect requires a metamaterial composed of three-dimensional chiral meta-atoms without any rotational symmetry. Our analysis is supported by a systematic investigation of the transmission matrices for arbitrarily complex, generally lossy media that allows deriving a simple criterion for asymmetric transmission in an arbitrary polarization base. Contrary to physical intuition, in general the polarization eigenstates in such three-dimensional and low-symmetry metamaterials do not obey fixed relations and the associated transmission matrices cannot be symmetrized.

Understanding the electric and magnetic response of isolated metaatoms by means of a multipolar field decomposition.

We introduce a technique to decompose the scattered near field of two-dimensional arbitrary metaatoms into its multipole contributions. To this end we expand the scattered field upon plane wave illumination into cylindrical harmonics as known from Mie's theory. By relating these cylindrical harmonics to the field radiated by Cartesian multipoles, the contribution of the lowest order electric and magnetic multipoles can be identified. Revealing these multipoles is essential for the design of metamaterials because they largely determine the character of light propagation. In particular, having this information at hand it is straightforward to distinguish between effects that result either from the arrangement of the metaatoms or from their particular design.

Doubly resonant optical nanoantenna arrays for polarization resolved measurements of surface-enhanced Raman scattering.

We report that rhomb-shaped metal nanoantenna arrays support multiple plasmonic resonances, making them favorable bio-sensing substrates. Besides the two localized plasmonic dipole modes associated with the two principle axes of the rhombi, the sample supports an additional grating-induced surface plasmon polariton resonance. The plasmonic properties of all modes are carefully studied by far-field measurements together with numerical and analytical calculations. The sample is then applied to surface-enhanced Raman scattering measurements. It is shown to be highly efficient since two plasmonic resonances of the structure were simultaneously tuned to coincide with the excitation and the emission wavelength in the SERS experiment. The analysis is completed by measuring the impact of the polarization angle on the SERS signal.

Three-dimensional light bullets in arrays of waveguides.

We report the first experimental observation of three-dimensional light bullets, excited by femtosecond pulses in a system featuring quasi-instantaneous cubic nonlinearity and a periodic, transversally modulated refractive index. Stringent evidence of the excitation of light bullets is based on time-gated images and spectra which perfectly match our numerical simulations. Furthermore, we reveal a novel evolution mechanism forcing the light bullets to follow varying dispersion or diffraction conditions, until they leave their existence range and decay.

Observation of three-dimensional discrete-continuous x waves in photonic lattices.

We report on the generation of three-dimensional discrete X waves in a femtosecond laser-written waveguide array. Our measurements constitute the first experimental observation of temporally localized three-dimensional discrete-continuous entities. The X waves spontaneously emerge from a single-site excitation due to the discrete diffraction of the lattice and the normally dispersive as well as cubically nonlinear properties of the fused silica used as host material.