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Chemical interface damping is a change in the effective collision frequency of conduction band electrons in metal originating from a chemical change of the metal interface. In this work, we present in-situ ellipsometric measurements that reveal the chemical interface damping effect from electrochemical oxidation of single crystal and polycrystalline gold films. We observe an increase in collision frequency of up to 21 meV for single-crystalline gold. To compare to results obtained with thiols and metal-oxides on gold nanoparticles, we normalize the collision frequency by the electron mean free path to the surface of the structure. We show that electrochemical gold oxidation provides a stronger effect on collision frequency than these coatings. Similar ellipsometric experiments have previously been conducted to investigate the optical properties of gold oxide, but without taking chemical interface damping into account. The change in reflection from oxidation of gold was solely attributed to the oxide coating. We also show that the chemical interface damping effect saturates at a larger effective oxide thickness, which is attributed to the stabilization of the gold-oxide interface.

The generation and utilization of hot charge carriers in plasmonic materials have emerged as a topic of significant importance, with profound implications across multiple disciplines, including optoelectronics, photovoltaics, photocatalysis, and sensing. In this study, we investigate the hot electron transfer from nanoporous gold (npAu) in dependence of the structure size, utilizing both the nanoscale feature size and the interconnected nature of this material. We employ photoelectron injection from nanoporous gold into the electrolyte under UV illumination as a test electron transfer process. Nanoporous gold thin films with sub-10 nm initial ligament diameter are stepwise coarsened by potential cycles in a photoelectrochemical setup, thereby allowing us to precisely probe the influence of ligament diameter on the photocurrent response. The resulting ligament diameter variations are confirmed by scanning electron microscopy (SEM) analysis. As the ligament diameter increased from 8 to 16 nm, there was a corresponding decrease in quantum efficiency proportional to the inverse ligament diameter squared. Such dependency is expected for electrons excited by surface collisions. For the small ligament diameter of 10 nm we estimate an emission efficiency of excited 6sp electrons as 3.14%, reaching 23% for the surface excited electrons., Comment: 30 pages, 13 figures

Significant suppression of radiation in 3D structured media with small refractive index 1.4-1.6, such as of glass or polymers, is a desirable feature yet to be obtained. For periodical structures this is realised at frequencies of the complete photonic band gap (CPBG), which up to now was demonstrated to open for materials with refractive index of at least 1.9. We present here a quasiperiodic 3D structure consisting of multiple overlapping gratings with a homogeneous distribution of Bragg peaks on a sphere in reciprocal space, which allows efficient suppression of emission. Recently we have presented the theoretical model, considering interaction with the neighbouring gratings only, that estimates a finite CPBG for arbitrarily small refractive indices and thus complete emission suppression in infinite structures. However, numerical simulations demonstrate a finite leakage of power from emitter not predicted by the model. Still the simulations show -10 dB suppression in 3D structures with optimised number of gratings. Astonishingly, as we show here, this limit is almost independent of the refractive index contrast. Also, the structures with a defined number of gratings show maximal suppression at certain refractive indices, losing the suppression even at higher refractive indices. The -10 dB suppression is demonstrated for refractive index contrast as low as 1.30.

An optical pulse asymptotically reaching zero group velocity in tapered waveguides can ultimately stop at a certain position in the taper accompanied by a strong spatial compression. This phenomenon can be also observed in spatio-temporal systems where the pulse velocity asymptotically reaches the velocity of a tapered front. The first system is well known from tapered plasmonic waveguides where adiabatic nano-focusing of light is observed. Its counterpart in the spatio-temporal system is the optical push broom effect where a nonlinear front collects and compresses the signal. Here, we use the slowly-varying envelope approximation to describe such systems. We demonstrate an analytical solution for the linear taper and the piecewise linear dispersion and show that the solution in this case resembles that of an optical lens in paraxial approximation. In particular, the spatial distribution of the focused light represents the Fourier transform of the signal at the input.

Here we report the first experimental demonstration of light trapping by a refractive index front in a silicon waveguide, the optical push broom effect. The front generated by a fast pump pulse collects and traps the energy of a CW signal with smaller group velocity and tuned near to the band gap of the Bragg grating introduced in the waveguide. This situation represents an optical analogue of light trapping in a tapered plasmonic waveguide where light is stopped without reflection. The energy of the CW signal is accumulated inside the front and distributed in frequency. In this experiment a 2 ps free carrier front was generated via two photon absorption of the pump in silicon waveguide. It collects approximately a 30 ps long packet of the CW signal. The presented effect can be utilized to compress signals in time and space.

The minimal refractive index contrast to obtain a complete photonic bandgap (CPBG) in structured media was not identified so far. We address this problem by considering distributed quasicrystals in with arbitrary number and positions of Bragg peaks in reciprocal space. For these structures an analytical estimation is derived which predicts that there is an optimal number of Bragg peaks for any refractive index contrast and finite CPBGs for an arbitrarily small refractive index contrast in 2D and 3D. Results of numerical simulations of dipole emission in 2D structures support our estimation. In 3D an emission suppression of almost 10 dB was demonstrated with a refractive index contrast of 1.6. The reason for residual leakage in 3D structures has to be further investigated.

The nonlinear Schr\"odinger equation based on slowly varying approximation is usually applied to describe the pulse propagation in nonlinear waveguides. However, for the case of the front induced transitions (FITs), the pump effect is well described by the dielectric constant perturbation in space and time. Thus, a linear Schr\"odinger equation can be used. Also, in waveguides with weak dispersion the spatial evolution of the pulse temporal profile is usually tracked. Such a formulation becomes impossible for optical systems for which the group index or higher dispersion terms diverge as is the case near the band edge of photonic crystals. For the description of FITs in such systems a linear Schr\"odinger equation can be used where temporal evolution of the pulse spatial profile is tracked instead of tracking the spatial evolution. This representation provides the same descriptive power and can easily deal with zero group velocities. Furthermore, the Schr\"odinger equation with temporal evolution can describe signal pulse reflection from both static and counter-propagating fronts, in contrast to the Schr\"odinger equation with spatial evolution which is bound to forward propagation. Here, we discuss the two approaches and demonstrate the applicability of the spatial evolution for the system close to the band edge where the group velocity vanishes by simulating intraband indirect photonic transitions.

Disordered structures producing a non-iridescent color impression have been shown to feature a spherically shaped Fourier transform of their refractive-index distribution. We determine the direction and efficiency of scattering from thin films made from such structures with the help of the Ewald sphere construction which follows from first-order scattering approximation. This way we present a simple geometrical argument why these structures are well suited for creating short wavelength colors like blue but are hindered from producing long wavelength colors like red. We also numerically synthesize a model structure dedicated to produce a sharp spherical shell in reciprocal space. The reflectivity of this structure as predicted by the first-order approximation is compared to direct electromagnetic simulations. The results indicate the Ewald sphere construction to constitute a simple geometrical tool that can be used to describe and to explain important spectral and directional features of the reflectivity. It is shown that total internal reflection in the film in combination with directed scattering can be used to obtain long wavelength structural colors.

Non-iridescent structural colors based on disordered arrangement of monodisperse spherical particles, also called photonic glass, show low color saturation due to gradual transition in reflectivity. No significant improvement is usually expected from particles optimization, as the Mie resonances are broad for small dielectric particles with moderate refractive index. Moreover, the short range order of a photonic glass alone is also insufficient to cause sharp spectral features. We show here, that the combination of a well-chosen particle geometry with the short range order of a photonic glass has strong synergetic effects. We demonstrate how core-shell particles can be used to obtain a sharp transition in the reflection spectrum of photonic glass which is essential to achieve a strong color saturation. The Fourier transform required for a highly saturated color can be achieved by shifting the first zero position of the motif Fourier transform to smaller wave numbers in respect to the peak of the lattice Fourier transform. We show that this can be obtained by choosing a non-monotonous refractive index distribution from the center of the particle through the shell and into the background material. The first-order theoretical predictions are confirmed by numerical simulations.

We present a full vectorial first-order approach to the scattering by arbitrary photonic structures with a low refractive index contrast. Our approach uses the first-order Born approximation and keeps the simple geometrical representation of the Ewald sphere construction. Via normalization to a representative sample volume, the approach can also predict the scattering by infinitely extended layers of scattering media. It can therefore be used to describe and efficiently calculate the scattering by structures where the linear first-order scattering terms dominate, e.g. in low index contrast disordered structures creating a color impression.

The orientational and translational order of a thermotropic ferroelectric liquid crystal (2MBOCBC) imbibed in self-organized, parallel, cylindrical pores with radii of 10, 15, or 20 nm in anodic aluminium oxide monoliths (AAO) are explored by high-resolution linear and circular optical birefringence as well as neutron diffraction texture analysis. The results are compared to experiments on the bulk system. The native oxidic pore walls do not provide a stable smectogen wall anchoring. By contrast, a polymeric wall grafting enforcing planar molecular anchoring results in a thermal-history independent formation of smectic C* helices and a reversible chevron-like layer buckling. An enhancement of the optical rotatory power by up to one order of magnitude of the confined compared to the bulk liquid crystal is traced to the pretransitional formation of helical structures at the smectic-A*-to-smectic-C* transformation. A linear electro-optical birefringence effect evidences collective fluctuations in the molecular tilt vector direction along the confined helical superstructures, i.e. the Goldstone phason excitations typical of the para-to-ferroelectric transition. Their relaxation frequencies increase with the square of the inverse pore radii as characteristic of plane-wave excitations and are two orders of magnitude larger than in the bulk, evidencing an exceptionally fast electro-optical functionality of the liquid-crystalline-AAO nanohybrids., Comment: 14 pages, 13 figures, 2 ancillary files, as submitted, Nanoscale (in press)

We consider emitting nanoparticles in dielectric nanocomposites with varying refractive index contrast and geometry. For that we develop a simple and universal method to calculate the emission enhancement in nanocomposites that employs solely the calculation of the effective refractive index and electric field distributions from three quasistatic calculations with orthogonal polarizations. The method is exemplified for dilute nanocomposites without electromagnetic interaction between emitting particles as well as for dense nanocomposites with strong particle interaction. We show that the radiative decay in dielectric nanocomposites is greatly affected by the shape and arrangement of its constituents and give guidelines for larger enhancement.

Reflection at relativistically moving plasma mirrors is a well-known approach for frequency conversion as an alternative to nonlinear techniques. A key issue with plasma mirrors is the need for a high carrier concentration, of order 10^21 cm^-3, to achieve an appreciable reflectivity. To generate such high carrier concentrations, short laser pulses with extreme power densities of the order >10^15 W/cm^2 are required. Here, we introduce a novel waveguide-based method for generating relativistically moving plasma mirrors that requires much lower pump powers and much less carrier concentration. Specifically, we achieve an experimental demonstration of 35% reflection for a carrier concentration of 5*10^17/cm^3 generated by a power density of only 1.2*10^9 W/cm^2. Both the plasma mirror and the signal are confined and propagating within a solid state silicon slow light photonic crystal waveguide. This extraordinary effect only becomes possible because we exploit an indirect intraband optical transition in a dispersion engineered slow light waveguide, where the incident light cannot couple to other states beyond the moving front and has to reflect from it. The moving free carrier (FC) plasma mirror is generated by two photon absorption of 6 ps long pump pulse with a peak power of 6.2 W. The reflection was demonstrated by the interaction of a continuous wave (CW) probe wave co-propagating with the relativistic FC plasma mirror inside a 400 micro-meter long slow light waveguide. Upon interaction with the FC plasma mirror, the probe wave packets, which initially propagate slower than the plasma mirror, are bounced and accelerated, finally escaping from the front in forward direction. The forward reflection of the probe wave packets are accompanied by a frequency upshift. The reflection efficiency is estimated for the part of the CW probe interacting with the pump pulse.

We report dielectric relaxation spectroscopy experiments on two rod-like liquid crystals of the cyanobiphenyl family (5CB and 6CB) confined in tubular nanochannels with 7 nm radius and 340 micrometer length in a monolithic, mesoporous silica membrane. The measurements were performed on composites for two distinct regimes of fractional filling: monolayer coverage at the pore walls and complete filling of the pores. For the layer coverage a slow surface relaxation dominates the dielectric properties. For the entirely filled channels the dielectric spectra are governed by two thermally-activated relaxation processes with considerably different relaxation rates: A slow relaxation in the interface layer next to the channel walls and a fast relaxation in the core region of the channel filling. The strengths and characteristic frequencies of both relaxation processes have been extracted and analysed as a function of temperature. Whereas the temperature dependence of the static capacitance reflects the effective (average) molecular ordering over the pore volume and is well described within a Landau-de Gennes theory, the extracted relaxation strengths of the slow and fast relaxation processes provide an access to distinct local molecular ordering mechanisms. The order parameter in the core region exhibits a bulk-like behaviour with a strong increase in the nematic ordering just below the paranematic-to-nematic transition temperature T_PN and subsequent saturation during cooling. By contrast, the surface ordering evolves continuously with a kink near T_PN. A comparison of the thermotropic behaviour of the monolayer with the complete filling reveals that the molecular order in the core region of the pore filling affects the order of the peripheral molecular layers at the wall., Comment: 12 pages, 7 figures

We report filling-fraction dependent dielectric spectroscopy measurements on the relaxation dynamics of the rod-like nematogen 7CB condensed in 13 nm silica nanochannels. In the film-condensed regime, a slow interface relaxation dominates the dielectric spectra, whereas from the capillary-condensed state up to complete filling an additional, fast relaxation in the core of the channels is found. The temperature-dependence of the static capacitance, representative of the averaged, collective molecular orientational ordering, indicates a continuous, paranematic-to-nematic (P-N) transition, in contrast to the discontinuous bulk behaviour. It is well described by a Landau-de-Gennes free energy model for a phase transition in cylindrical confinement. The large tensile pressure of 10 MPa in the capillary-condensed state, resulting from the Young-Laplace pressure at highly curved liquid menisci, quantitatively accounts for a downward-shift of the P-N transition and an increased molecular mobility in comparison to the unstretched liquid state of the complete filling. The strengths of the slow and fast relaxations provide local information on the orientational order: The thermotropic behaviour in the core region is bulk-like, i.e. it is characterized by an abrupt onset of the nematic order at the P-N transition. By contrast, the interface ordering exhibits a continuous evolution at the P-N transition. Thus, the phase behaviour of the entirely filled liquid crystal-silica nanocomposite can be quantitatively described by a linear superposition of these distinct nematic order contributions., Comment: 12 pages, 6 figures

The blackbody theory is revisited in the case of thermal electromagnetic fields inside uniaxial anisotropic media in thermal equilibrium with a heat bath. When these media are hyperbolic, we show that the spectral energy density of these fields radically differs from that predicted by Planck's blackbody theory. We demonstrate that the maximum of their spectral energy density is shifted towards frequencies smaller than Wien's frequency making these media apparently colder. Finally, we derive Stefan-Boltzmann's law for hyperbolic media which becomes a quadratic function of the heat bath temperature.

We compare super-Planckian thermal radiation between phonon-polaritonic media and hyperbolic metamaterials. In particular, we determine the penetration depth of thermal photons inside the absorbing medium for three different structures: two semi-infinite phonon-polaritonic media supporting surface modes, two multilayer hyperbolic metamaterials and two nanowire hyperbolic metamaterials. We show that for hyperbolic modes the penetration depth can be orders of magnitude larger than for surface modes suggesting that hyperbolic materials are much more preferable for near-field thermophotovoltaic applications than pure phonon-polaritonic materials.

The transport of heat mediated by thermal photons in hyperbolic multilayer metamaterials is studied using the fluctuational electrodynamics theory. We demonstrate that in comparison to bulk materials the flux inside layered hyperbolic materials can be transported at much longer distances, making these media very promising for thermal management and for near-field energy harvesting.

Wang et al. [1] demonstrated different power transmission coefficients for forward and backward propagation in simulation and experiment. From such a demonstration, the central claim of their paper is that "the spatial inversion symmetry breaking diode can construct an optical isolator in no conflict with any reciprocal principle". Their claim contradicts the Lorentz reciprocity theorem, from which it is well known that one cannot construct an isolator this way.

In the recent article by Feng et al. [Science 333, 729-733 (2011)] a system is proposed with a periodic spatial modulation of refractive index and absorption. It is claimed that this system is nonreciprocal and can be used as an optical isolator. The authors use an unconventional definition of reciprocity and thus make wrong conclusions on the applicability of the described phenomena for optical isolators. (Submitted to Science on October 7, 2011)