Relation between growth dynamics and the spatial distribution of intrinsic defects in self-assembled colloidal crystal films

Herein we establish a clear relation between the parameters that govern the growth dynamics and the structural quality of colloidal crystal films. We report an optical analysis of the spatial distribution of intrinsic defects in colloidal crystal films and correlate our results with a theoretical model describing the growth dynamics of such lattices. We find that the amount of defects fluctuates periodically and decreases along the growth direction of the lattice. We demonstrate that these spatial variations are a direct consequence of the temporal oscillations of the crystal film formation velocity, which are inherent to the colloidal particle deposition process.Ministerio de Ciencia y Educación MAT2004-0302

Molding with nanoparticle-based one-dimensional photonic crystals: A route to flexible and transferable Bragg mirrors of high dielectric contrast

Self-standing, flexible Bragg mirror films of high refractive index contrast and showing intense and wide Bragg peaks are herein presented. Nanoparticle-based one-dimensional photonic crystals are used as templates to infiltrate a polymer, which provides the multilayer with mechanical stability while preserving the dielectric contrast existing in the mold. Such films can be lifted off the substrate and used to coat another surface of arbitrary shapeMinisterio de Ciencia y Educación MAT2008-02166Junta de Andalucía FQM-357

Towards a full understanding of the growth dynamics and optical response of self-assembled photonic colloidal crystal films

Recent advances in the comprehension of the growth dynamics of colloidal crystal films opens the door to rational design of experiments aiming at fabricating lattices in which the density of intrinsic defects is minimized. Since such imperfections have a dramatic effect on scattered light of wavelength smaller than the lattice constant, the evaluation of the experimental optical response at those energy ranges, based on the comparison to rigorous calculations, is identified as the most sensitive guide to accurately evaluate the progress towards the actual realization of defect-free colloidal crystals.Ministerio de Ciencia y Educación MAT200503028Consejo Superior de Investigaciones Científicas 2005AR007

Interplay between crystal-size and disorder effects in the high-energy optical response of photonic crystal slabs

Experimental reflectance spectra have been obtained for colloidal crystals whose widths ranged from one to several sphere monolayers, and their features in the higher order band energy range have been reproduced theoretically. In order to fit the measured data, optical extinction has been introduced in the theoretical model, which accounts for structure imperfections and disorder, the main sources of losses in an actual measurement. A complex spectrum in the high frequency region is observed even for one ordered monolayer, being this peak structure gradually modified as more layers are piled up. This allowed us to identify which peaks are reminiscent of the optical reflectance features of a single close-packed layer and which are the result of building up a three dimensional periodicity. A clear correlation between the amount of extinction introduced in the fitting and the slab width has been found, which demonstrates that wider real crystals produce less diffusely scattered light. At the same time, we find that the optical response of thinner crystals is more robust against the introduction of extinction than that of thicker ones, for which the effect is dramatic.Consejo Superior de Investigaciones Científicas 2005AR0070Universidad de Buenos Aires ANPCYT-BID 802Agencia Nacional de Promoción Científica y Tecnológica OC-AR03-14099Ministerio de Ciencia y Educación MAT2005-0302

Physical origin of the high energy optical response of three-dimensional photonic crystals

The physical origin of the optical response observed in three-dimensional photonic crystals when the photon wavelength is equal or lower than the lattice parameter still remains unsatisfactorily explained and is the subject of an intense and interesting debate. Herein we demonstrate for the first time that all optical spectra features in this high energy region of photonic crystals arise from electromagnetic resonances within the ordered array, modified by the interplay between these resonances with the opening of diffraction channels, the presence of imperfections and finite size effects. AU these four phenomena are taken into account in our theoretical approach to the problem, which allows us to provide a full description of the observed optical response based on fundamental phenomena as well as to attain fair fittings of experimental results.Consejo Superior de Investigaciones Científicas 2005AR0070Universidad de Buenos Aires ANPCYT-BID 802Agencia Nacional de Promoción Científica y Tecnológica OC-AR03-14099Ministerio de Ciencia y Educación MAT2005-0302

Tailor-made directional emission in nanoimprinted plasmonic-based light-emitting devices

We demonstrate an enhanced and tailor-made directional emission of light-emitting devices using nanoimprinted hexagonal arrays of aluminum nanoparticles. Fourier microscopy reveals that the luminescence of the device is not only determined by the material properties of the organic dye molecules but is also strongly influenced by the coherent scattering resulting from periodically arranged metal nanoparticles. Emitters can couple to lattice-induced hybrid plasmonic–photonic modes sustained by plasmonic arrays. Such modes enhance the spatial coherence of an emitting layer, allowing the efficient beaming of the emission along narrow angular and spectral ranges. We show that tailoring the separation of the nanoparticles in the array yields an accurate angular distribution of the emission. This combination of large-area metal nanostructures fabricated by nanoimprint lithography and light-emitting devices is beneficial for the design and optimization of solid-state lighting systems

Design and Realization of a Novel Optically Disordered Material: A Demonstration of a Mie Glass

Herein, a diffusive material presenting optical disorder is introduced, which represents an example of a Mie glass. Comprising spherical crystalline TiO nanoparticles randomly dispersed in a mesoporous TiO matrix, it is proved that the scattering of light in this inhomogeneous solid can be predicted in an unprecedented manner from single-particle considerations employing Mie theory. To that aim, a study of the dependence of the key parameters employed is performed to describe light propagation in random media, i.e., the scattering mean free path and the transport mean free path, as a function of the size and concentration of the spherical inclusions based on a comparison between experimental results and analytical calculations. It is also demonstrated that Mie glasses enable enhanced fluorescence intensity due to a combined absorptance enhancement of the excitation light combined with an improved outcoupling of the emitted light. The method offers the possibility to perform a deterministic design for the realization of a light diffuser with tailor-made scattering properties.European Union 307081Ministerio de Economía y Competitividad MAT2014-54852-

Modified emission of extended light emitting layers by selective coupling to collective lattice resonances

We demonstrate that the coupling between light emitters in extended polymer layers and modes supported by arrays of plasmonic particles can be selectively enhanced by accurate positioning of the emitters in regions where the electric field intensity of a given mode is maximized. The enhancement, which we measure to reach up to 70%, is due to the improved spatial overlap and coupling between the optical mode and emitters. This improvement of the coupling leads to a modification of the emission spectrum and the luminous efficacy of the sample

Metallic nanostructures for efficient LED lighting

Light-emitting diodes (LEDs) are driving a shift toward energy-efficient illumination. Nonetheless, modifying the emission intensities, colors and directionalities of LEDs in specific ways remains a challenge often tackled by incorporating secondary optical components. Metallic nanostructures supporting plasmonic resonances are an interesting alternative to this approach due to their strong light–matter interaction, which facilitates control over light emission without requiring external secondary optical components. This review discusses new methods that enhance the efficiencies of LEDs using nanostructured metals. This is an emerging field that incorporates physics, materials science, device technology and industry. First, we provide a general overview of state-of-the-art LED lighting, discussing the main characteristics required of both quantum wells and color converters to efficiently generate white light. Then, we discuss the main challenges in this field as well as the potential of metallic nanostructures to circumvent them. We review several of the most relevant demonstrations of LEDs in combination with metallic nanostructures, which have resulted in light-emitting devices with improved performance. We also highlight a few recent studies in applied plasmonics that, although exploratory and eminently fundamental, may lead to new solutions in illuminatio

Symmetry analysis of the numerical instabilities in the transfer matrix method

This paper discusses the numerical exponential instability of the transfer matrix method (TMM) in the framework of the symmetry formalism. This numerical weakness is attributed to a series of increasingly extreme exponentials that appear in the TMM when it is applied to geometries involving total internal reflection (TIR) or very high absorption. We design a TMM formalism that identifies the internal symmetries of the multilayer geometry. These symmetries suggest particular transformations of a reference system in the TMM that improve its ill-conditioned exponentials. To illustrate the numerical improvements, we present examples with calculations of electric fields.Nordic Innovation Center 09053Ministerio de Economía y Competitividad MAT2011-23593, CSD2007-00007Junta de Andalucía FQM- 3579, FQM-524