Quasiperiodic light.

Quasiperiodicity is a form of spatial order that has been observed in quasicrystalline matter but not light. We construct a quasicrystalline surface out of a light emitting diode. Using a nanoscale waveguide as a microscope (NSOM), we directly image the light field at the surface of the diode. Here we show, using reciprocal space representations of the images, that the light field is quasiperiodic. We explain the structure of the light field with wave superposition. Periodic ordering is limited to at most six-fold symmetry. The light field exhibits 12-fold quasisymmetry, showing order while disproving periodicity. This demonstrates that a new class, consisting of projections from hyperspace, exists in the taxonomy of light ordering.

Efficient light harvesting in hybrid quantum dot-interdigitated back contact solar cells via resonant energy transfer and luminescent downshifting.

In this paper, we propose a hybrid quantum dot (QD)/solar cell configuration to improve performance of interdigitated back contact (IBC) silicon solar cells, resulting in 39.5% relative boost in the short-circuit current (JSC) through efficient utilisation of resonant energy transfer (RET) and luminescent downshifting (LDS). A uniform layer of CdSe1-xSx/ZnS quantum dots is deposited onto the AlOx surface passivation layer of the IBC solar cell. QD hybridization is found to cause a broadband improvement in the solar cell external quantum efficiency. Enhancement over the QD absorption wavelength range is shown to result from LDS. This is confirmed by significant boosts in the solar cell internal quantum efficiency (IQE) due to the presence of QDs. Enhancement over the red and near-infrared spectral range is shown to result from the anti-reflection properties of the QD layer coating. A study on the effect of QD layer thickness on solar cell performance was performed and an optimised QD layer thickness was determined. Time-resolved photoluminescence (TRPL) spectroscopy was used to investigate the photoluminescence dynamics of the QD layer as a function of AlOx spacer layer thickness. RET can be evoked between the QD and Si layers for very thin AlOx spacer layers, with RET efficiencies of up to 15%. In the conventional LDS architecture, down-converters are deposited on the surface of an optimised anti-reflection layer, providing relatively narrowband enhancement, whereas the QDs in our hybrid architecture provide optical enhancement over the broadband wavelength range, by simultaneously utilising LDS, RET-mediated carrier injection, and antireflection effects, resulting in up to 40% improvement in the power conversion efficiency (PCE). Low-cost synthesis of QDs and simple device integration provide a cost-effective solution for boosting solar cell performance.

Colloidal Synthesis of CsX Nanocrystals (X = Cl, Br, I).

A facile colloidal synthesis of highly ionic cesium halide nanocrystals is reported. Colloidal nanocrystals of CsI, CsCl and CsBr with unprecedentedly small dimensions are obtained using oleylammonium halides and cesium oleate as precursors. The ease and adaptability of our method enables its universalization for the formation of other highly ionic nanocrystals.

Compliance-Free ZrO2/ZrO2 - x /ZrO2 Resistive Memory with Controllable Interfacial Multistate Switching Behaviour.

A controllable transformation from interfacial to filamentary switching mode is presented on a ZrO2/ZrO2 - x /ZrO2 tri-layer resistive memory. The two switching modes are investigated with possible switching and transformation mechanisms proposed. Resistivity modulation of the ZrO2 - x layer is proposed to be responsible for the switching in the interfacial switching mode through injecting/retracting of oxygen ions. The switching is compliance-free due to the intrinsic series resistor by the filaments formed in the ZrO2 layers. By tuning the RESET voltages, controllable and stable multistate memory can be achieved which clearly points towards the capability of developing the next-generation multistate high-performance memory.

Breakthrough to Non-Vacuum Deposition of Single-Crystal, Ultra-Thin, Homogeneous Nanoparticle Layers: A Better Alternative to Chemical Bath Deposition and Atomic Layer Deposition.

Most thin-film techniques require a multiple vacuum process, and cannot produce high-coverage continuous thin films with the thickness of a few nanometers on rough surfaces. We present a new "paradigm shift" non-vacuum process to deposit high-quality, ultra-thin, single-crystal layers of coalesced sulfide nanoparticles (NPs) with controllable thickness down to a few nanometers, based on thermal decomposition. This provides high-coverage, homogeneous thickness, and large-area deposition over a rough surface, with little material loss or liquid chemical waste, and deposition rates of 10 nm/min. This technique can potentially replace conventional thin-film deposition methods, such as atomic layer deposition (ALD) and chemical bath deposition (CBD) as used by the Cu(In,Ga)Se2 (CIGS) thin-film solar cell industry for decades. We demonstrate 32% improvement of CIGS thin-film solar cell efficiency in comparison to reference devices prepared by conventional CBD deposition method by depositing the ZnS NPs buffer layer using the new process. The new ZnS NPs layer allows reduction of an intrinsic ZnO layer, which can lead to severe shunt leakage in case of a CBD buffer layer. This leads to a 65% relative efficiency increase.

Effect of non-conformal gold deposition on SERS related plasmonic effects.

Recently, a comprehensive three dimensional computational model based on rigorous coupled wave analysis (RCWA) has been developed to investigate the properties of surface plasmons resident on metal coated arrays of inverted pyramidal pits used for SERS sensing applications in the form of 'klarite'. This simulation tool allows the identification of a variety of dispersive features including propagating and localized surface plasmons as well as simple diffraction relating to the influence of geometrical features. In this paper, we investigate the influence of non-conformality of the gold coating over the internal surfaces of the inverted pyramidal pits on plasmon dispersion. Modeling reveals very strong changes in plasmon behavior as a function of gold layer conformality. Dependent upon conformality of the gold coating we find that the nano-textured metallic surface can behave either as an efficient broadband mirror-like reflector or as an efficient broadband, wide angle absorber at infrared wavelengths. Creation of a broadband wide angle absorbing surface such as this has important implications for photovoltaic cells. For sensing applications, understanding the effect of metal layer conformality on plasmon dispersion gives clear insight into how to further improve the SERS enhancement factor.

Bridging the "green gap" of LEDs: giant light output enhancement and directional control of LEDs via embedded nano-void photonic crystals.

Green LEDs do not show the same level of performance as their blue and red cousins, greatly hindering the solid-state lighting development, which is the so-called "green gap". In this work, nano-void photonic crystals (NVPCs) were fabricated to embed within the GaN/InGaN green LEDs by using epitaxial lateral overgrowth (ELO) and nano-sphere lithography techniques. The NVPCs act as an efficient scattering back-reflector to outcouple the guided and downward photons, which not only boost the light extraction efficiency of LEDs with an enhancement of 78% but also collimate the view angle of LEDs from 131.5° to 114.0°. This could be because of the highly scattering nature of NVPCs which reduce the interference giving rise to Fabry-Perot resonance. Moreover, due to the threading dislocation suppression and strain relief by the NVPCs, the internal quantum efficiency was increased by 25% and droop behavior was reduced from 37.4% to 25.9%. The enhancement of light output power can be achieved as high as 151% at a driving current of 350 mA. Giant light output enhancement and directional control via NVPCs point the way towards a promising avenue of solid-state lighting.

Design and fabrication of a 3D-structured gold film with nanopores for local electric field enhancement in the pore.

Three-dimensionally structured gold membrane films with nanopores of defined, periodic geometries are designed and fabricated to provide the spatially localised enhancement of electric fields by manipulation of the plasmons inside nanopores. Square nanopores of different size and orientation relative to the pyramid are considered for films in aqueous and air environments, which allow for control of the position of electric fields within the structure. Designs suitable for use with 780 nm light were created. Here, periodic pyramidal cavities produced by potassium hydroxide etching to the {111} planes of (100) silicon substrates are used as templates for creating a periodic, pyramidal structured, free-standing thin gold film. Consistent with the findings from the theoretical studies, a nano-sized hole of 50 nm square was milled through the gold film at a specific location in the cavity to provide electric field control which can subsequently used for enhancement of fluorescence or Raman scattering of molecules in the nanopore.

Toward omnidirectional light absorption by plasmonic effect for high-efficiency flexible nonvacuum Cu(In,Ga)Se2 thin film solar cells.

We have successfully demonstrated a great advantage of plasmonic Au nanoparticles for efficient enhancement of Cu(In,Ga)Se2(CIGS) flexible photovoltaic devices. The incorporation of Au NPs can eliminate obstacles in the way of developing ink-printing CIGS flexible thin film photovoltaics (TFPV), such as poor absorption at wavelengths in the high intensity region of solar spectrum, and that occurs significantly at large incident angle of solar irradiation. The enhancement of external quantum efficiency and photocurrent have been systematically analyzed via the calculated electromagnetic field distribution. Finally, the major benefits of the localized surface plasmon resonances (LSPR) in visible wavelength have been investigated by ultrabroadband pump-probe spectroscopy, providing a solid evidence on the strong absorption and reduction of surface recombination that increases electron-hole generation and improves the carrier transportation in the vicinity of pn-juction.

Reflectance properties of silicon moth-eyes in response to variations in angle of incidence, polarisation and azimuth orientation.

We report a study of the optical properties of silicon moth-eye structures using a custom-made fully automated broadband spectroscopic reflectometry system (goniometer). This measurement system is able to measure specular reflectance as a function of wavelength, polar incidence angle and azimuth orientation angle, from normal to near-parallel polar incidence angle. The system uses a linear polarized broadband super-continuum laser light source. It is shown that a moth-eye structure composed of a regular array of protruding silicon rods, with finite sidewall angle reduces reflectance and sensitivity to incident wavelength in comparison to truly cylindrical rods with perpendicular sidewalls. It is also shown that moth-eye structures have omnidirectional reflectance properties in response to azimuth orientation of the sample. The importance of applying the reflectometer setup to study the optical properties of solar cell antireflective structures is highlighted.

Emission characteristics of photonic crystal light-emitting diodes.

Experimentally measured optical properties of photonic crystal LEDs are reported here. Photonic crystal and photonic quasi-crystal structures were fabricated on GaN epilayer LED wafer material using both direct-write electron beam lithography and nanoimprint lithography. Some of these structures were processed to make finished LEDs. Both electroluminescence and photoluminescence measurements were performed on these structures. Devices were characterized for their current-voltage characteristics, emission spectra, far-field emission pattern, and angular emission pattern. These results are useful for fabricating photonic crystal LEDs and assessing their operational properties.

Broadband stimulated four-wave parametric conversion on a tantalum pentoxide photonic chip.

We exploit the large third order nonlinear susceptibility (χ(3) or "Chi 3") of tantalum pentoxide (Ta(2)O(5)) planar waveguides and realize broadband optical parametric conversion on-chip. We use a co-linear pump-probe configuration and observe stimulated four wave parametric conversion when seeding either in the visible or the infrared. Pumping at 800 nm we observe parametric conversion over a broad spectral range with the parametric idler output spanning from 1200 nm to 1600 nm in infrared wavelengths and from 555 nm to 600 nm in visible wavelengths. Our demonstration of on-chip stimulated four wave parametric conversion introduces Ta(2)O(5) as a novel material for broadband integrated nonlinear photonic circuit applications.

A characterization of the Raman modes in a J-aggregate-forming dye: a comparison between theory and experiment.

J-Aggregates are a class of organic molecules that possess several interesting characteristics that make them attractive for a range of organic-based optoelectronic devices. We present experimental and computer-simulation studies of the Raman-active vibrational modes in the J-aggregate-forming dye 5,6-dichloro-2-[[5,6-dichloro-1-ethyl-3-(4-sulfobutyl)benzimidazol-2-ylidene]propenyl]-1-ethyl-3-(4-sulfobutyl)benzimidazolium hydroxide, sodium salt, inner salt. The molecular monomer and dimer are analyzed computationally and the Raman mode energies extracted. There is a good agreement between the energies of the theoretical and experimental Raman modes. Experimentally, an enhancement is seen in the intensity of two low frequency modes upon aggregation of the dye. This is attributed to aggregation-enhanced Raman scattering. An enhancement is also observed in certain modes of the calculated spectra upon changing from a monomer to dimeric arrangement. A link is suggested between the Raman-active vibrational modes of the molecule, and a time-dependent electronic coupling present over several molecules.

Chi 3 dispersion in planar tantalum pentoxide waveguides in the telecommunications window.

We report on the dispersion of the third-order nonlinear susceptibility (chi(3) or "Chi 3") in planar Ta2O5 waveguides in the telecommunications spectral window. We utilize the observation of third-harmonic generation under ultrashort pulsed excitation as a reference-free characterization method of chi(3) and obtain a large nonlinear coefficient, 2x10(-13) esu, at 1550 nm. Our observation of efficient third-harmonic generation in Ta2O5 waveguides in the telecoms window reveals the potential of this material system in high-speed integrated nonlinear optical switches.

Observation of the developing optical continuum along a nonlinear waveguide.

We describe what is to our knowledge the first nondestructive measurement of the evolution of an optical continuum as a function of distance along a nonlinear waveguide. Spectral mapping is achieved on a subwavelength scale by utilizing near-field microscopy to probe the waveguide's evanescent field. The measured continuum broadening along the waveguide agrees in general form with predictions of broadening from theoretical calculations, but differs in some important details. Subwavelength resolution measurements are made both along and across the waveguide to reveal spectral variations not seen before by other techniques.

Tuning localized plasmons in nanostructured substrates for surface-enhanced Raman scattering.

Comprehensive reflectivity mapping of the angular dispersion of nanostructured arrays comprising of inverted pyramidal pits is demonstrated. By comparing equivalently structured dielectric and metallic arrays, diffraction and plasmonic features are readily distinguished. While the diffraction features match expected theory, localised plasmons are also observed with severely flattened energy dispersions. Using pit arrays with identical pitch, but graded pit dimensions, energy scaling of the localized plasmon is observed. These localised plasmons are found to match a simple model which confines surface plasmons onto the pit sidewalls thus allowing an intuitive picture of the plasmons to be developed. This model agrees well with a 2D finite-difference time-domain simulation which shows the same dependence on pit dimensions. We believe these tuneable plasmons are responsible for the surface-enhancement of the Raman scattering (SERS) of an attached layer of benzenethiol molecules. Such SERS substrates have a wide range of applications both in security, chemical identification, environmental monitoring and healthcare.