Tailoring Iridescent Visual Appearance with Disordered Resonant Metasurfaces.

The nanostructures of natural species offer beautiful visual appearances with saturated and iridescent colors, and the question arises whether we can reproduce or even create unique appearances with man-made metasurfaces. However, harnessing the specular and diffuse light scattered by disordered metasurfaces to create attractive and prescribed visual effects is currently inaccessible. Here, we present an interpretive, intuitive, and accurate modal-based tool that unveils the main physical mechanisms and features defining the appearance of colloidal disordered monolayers of resonant meta-atoms deposited on a reflective substrate. The model shows that the combination of plasmonic and Fabry-Perot resonances offers uncommon iridescent visual appearances, differing from those classically observed with natural nanostructures or thin-film interferences. We highlight an unusual visual effect exhibiting only two distinct colors and theoretically investigate its origin. The approach can be useful in the design of visual appearance with easy-to-make and universal building blocks having a large resilience to fabrication imperfections and potential for innovative coatings and fine-art applications.

The visual appearances of disordered optical metasurfaces.

Nanostructured materials have recently emerged as a promising approach for material appearance design. Research has mainly focused on creating structural colours by wave interference, leaving aside other important aspects that constitute the visual appearance of an object, such as the respective weight of specular and diffuse reflectances, object macroscopic shape, illumination and viewing conditions. Here we report the potential of disordered optical metasurfaces to harness visual appearance. We develop a multiscale modelling platform for the predictive rendering of macroscopic objects covered by metasurfaces in realistic settings, and show how nanoscale resonances and mesoscale interferences can be used to spectrally and angularly shape reflected light and thus create unusual visual effects at the macroscale. We validate this property with realistic synthetic images of macroscopic objects and centimetre-scale samples observable with the naked eye. This framework opens new perspectives in many branches of fine and applied visual arts.

Controlling disorder in self-assembled colloidal monolayers via evaporative processes.

Monolayers of assembled nano-objects with a controlled degree of disorder hold interest in many optical applications, including photovoltaics, light emission, sensing, and structural coloration. Controlled disorder can be achieved through either top-down or bottom-up approaches, but the latter is more suited to large-scale, low-cost fabrication. Disordered colloidal monolayers can be assembled through evaporatively driven convective assembly, a bottom-up process with a wide range of parameters impacting particle placement. Motivated by the photonic applications of such monolayers, in this review we discuss the quantification of monolayer disorder, and the assembly methods that have been used to produce them. We review the impact of particle and solvent properties, as well as the use of substrate patterning, to create the desired spatial distributions of particles.

Non-Lorentzian Local Density of States in Coupled Photonic Crystal Cavities Probed by Near- and Far-Field Emission.

Recent theories proposed a deep revision of the well-known expression for the Purcell factor, with counterintuitive effects, such as complex modal volumes and non-Lorentzian local density of states. We experimentally demonstrate these predictions in tailored coupled cavities on photonic crystal slabs with relatively low optical losses. Near-field hyperspectral imaging of quantum dot photoluminescence is proved to be a direct tool for measuring the line shape of the local density of states. The experimental results clearly evidence non-Lorentzian character, in perfect agreement with numerical and theoretical predictions. Spatial maps with deep subwavelength resolution of the real and imaginary parts of the complex mode volumes are presented. The generality of these results is confirmed by an additional set of far-field and time-resolved experiments in cavities with larger modal volume and higher quality factors.

Global polarizability matrix method for efficient modeling of light scattering by dense ensembles of non-spherical particles in stratified media.

We introduce a numerical method that enables efficient modeling of light scattering by large, disordered ensembles of non-spherical particles incorporated in stratified media, including when the particles are in close vicinity to each other, to planar interfaces, and/or to localized light sources. The method consists of finding a small set of fictitious polarizable elements-or numerical dipoles-that quantitatively reproduces the field scattered by an individual particle for any excitation and at an arbitrary distance from the particle surface. The set of numerical dipoles is described by a global polarizability matrix that is determined numerically by solving an inverse problem relying on fullwave simulations. The latter are classical and may be performed with any Maxwell's equations solver. Spatial non-locality is an important feature of the numerical dipoles set, providing additional degrees of freedom compared to classical coupled dipoles to reconstruct complex scattered fields. Once the polarizability matrix describing scattering by an individual particle is determined, the multiple scattering problem by ensembles of such particles in stratified media can be solved using a Green tensor formalism and only a few numerical dipoles, thereby with a low physical memory usage, even for dense systems in close vicinity to interfaces. The performance of the method is studied with the example of large high-aspect-ratio high-index dielectric cylinders. The method is easy to implement and may offer new possibilities for the study of complex nanostructured surfaces, which are becoming widespread in emerging photonic technologies.

Visual Appearance of Chiral Nematic Cellulose-Based Photonic Films: Angular and Polarization Independent Color Response with a Twist.

Hydroxypropyl cellulose (HPC) is a biocompatible cellulose derivative capable of self-assembling into a lyotropic chiral nematic phase in aqueous solution. This liquid crystalline phase reflects right-handed circular polarized light of a specific color as a function of the HPC weight fraction. Here, it is demonstrated that, by introducing a crosslinking agent, it is possible to drastically alter the visual appearance of the HPC mesophase in terms of the reflected color, the scattering distribution, and the polarization response, resulting in an exceptional matte appearance in solid-state films. By exploiting the interplay between order and disorder, a robust and simple methodology toward the preparation of polarization and angular independent color is developed, which constitutes an important step toward the development of real-world photonic colorants.

Ultrafast perturbation maps as a quantitative tool for testing of multi-port photonic devices.

Advanced photonic probing techniques are of great importance for the development of non-contact wafer-scale testing of photonic chips. Ultrafast photomodulation has been identified as a powerful new tool capable of remotely mapping photonic devices through a scanning perturbation. Here, we develop photomodulation maps into a quantitative technique through a general and rigorous method based on Lorentz reciprocity that allows the prediction of transmittance perturbation maps for arbitrary linear photonic systems with great accuracy and minimal computational cost. Excellent agreement is obtained between predicted and experimental maps of various optical multimode-interference devices, thereby allowing direct comparison of a device under test with a physical model of an ideal design structure. In addition to constituting a promising route for optical testing in photonics manufacturing, ultrafast perturbation mapping may be used for design optimization of photonic structures with reconfigurable functionalities.

Lower bound for the spatial extent of localized modes in photonic-crystal waveguides with small random imperfections.

Light localization due to random imperfections in periodic media is paramount in photonics research. The group index is known to be a key parameter for localization near photonic band edges, since small group velocities reinforce light interaction with imperfections. Here, we show that the size of the smallest localized mode that is formed at the band edge of a one-dimensional periodic medium is driven instead by the effective photon mass, i.e. the flatness of the dispersion curve. Our theoretical prediction is supported by numerical simulations, which reveal that photonic-crystal waveguides can exhibit surprisingly small localized modes, much smaller than those observed in Bragg stacks thanks to their larger effective photon mass. This possibility is demonstrated experimentally with a photonic-crystal waveguide fabricated without any intentional disorder, for which near-field measurements allow us to distinctly observe a wavelength-scale localized mode despite the smallness (~1/1000 of a wavelength) of the fabrication imperfections.

Path length enhancement in disordered media for increased absorption.

We theoretically and numerically investigate the capability of disordered media to enhance the optical path length in dielectric slabs and augment their light absorption efficiency due to scattering. We first perform a series of Monte Carlo simulations of random walks to determine the path length distribution in weakly to strongly (single to multiple) scattering, non-absorbing dielectric slabs under normally incident light and derive analytical expressions for the path length enhancement in these two limits. Quite interestingly, while multiple scattering is expected to produce long optical paths, we find that media containing a vanishingly small amount of scatterers can still provide high path length enhancements due to the very long trajectories sustained by total internal reflection at the slab interfaces. The path length distributions are then used to calculate the light absorption efficiency of media with varying absorption coefficients. We find that maximum absorption enhancement is obtained at an optimal scattering strength, in-between the single-scattering and the diffusive (strong multiple-scattering) regimes. This study can guide experimentalists towards more efficient and potentially low-cost solutions in photovoltaic technologies.

Light diffusion in quenched disorder: role of step correlations.

We present a theoretical and experimental study of light transport in disordered media with strongly heterogeneous distribution of scatterers formed via nonscattering regions. Step correlations induced by quenched disorder are found to prevent diffusivity from diverging with increasing heterogeneity scale, contrary to expectations from annealed models. Spectral diffusivity is measured for a porous ceramic where nanopores act as scatterers and macropores render their distribution heterogeneous. Results agree well with Monte Carlo simulations and a proposed analytical model.

Engineering of light confinement in strongly scattering disordered media.

Disordered photonic materials can diffuse and localize light through random multiple scattering, offering opportunities to study mesoscopic phenomena, control light-matter interactions, and provide new strategies for photonic applications. Light transport in such media is governed by photonic modes characterized by resonances with finite spectral width and spatial extent. Considerable steps have been made recently towards control over the transport using wavefront shaping techniques. The selective engineering of individual modes, however, has been addressed only theoretically. Here, we experimentally demonstrate the possibility to engineer the confinement and the mutual interaction of modes in a two-dimensional disordered photonic structure. The strong light confinement is achieved at the fabrication stage by an optimization of the structure, and an accurate and local tuning of the mode resonance frequencies is achieved via post-fabrication processes. To show the versatility of our technique, we selectively control the detuning between overlapping localized modes and observe both frequency crossing and anti-crossing behaviours, thereby paving the way for the creation of open transmission channels in strongly scattering media.

Light transport and localization in two-dimensional correlated disorder.

Structural correlations in disordered media are known to affect significantly the propagation of waves. In this Letter, we theoretically investigate the transport and localization of light in 2D photonic structures with short-range correlated disorder. The problem is tackled semianalytically using the Baus-Colot model for the structure factor of correlated media and a modified independent scattering approximation. We find that short-range correlations make it possible to easily tune the transport mean free path by more than a factor of 2 and the related localization length over several orders of magnitude. This trend is confirmed by numerical finite-difference time-domain calculations. This study therefore shows that disorder engineering can offer fine control over light transport and localization in planar geometries, which may open new opportunities in both fundamental and applied photonics research.

Disordered photonic structures for light harvesting in solar cells.

The effect of periodic and disordered photonic structures on the absorption efficiency of amorphous and crystalline Silicon thin-film solar cells is investigated numerically. We show that disordered patterns possessing a short-range correlation in the position of the holes yield comparable, or even superior, absorption enhancements than periodic (photonic crystal) patterns. This work provides clear evidence that non-deterministic photonic structures represent a viable alternative strategy for photon management in thin-film solar cells, thereby opening the route towards more efficient and potentially cheaper photovoltaic technologies.

Two-dimensional disorder for broadband, omnidirectional and polarization-insensitive absorption.

The surface of thin-film solar cells can be tailored with photonic nanostructures to allow light trapping in the absorbing medium. This in turn increases the optical thickness of the film and thus enhances their absorption. Such a coherent light trapping is generally accomplished with deterministic photonic architectures. Here, we experimentally explore the use of a different nanostructure, a disordered one, for this purpose. We show that the disorder-induced modes in the film allow improvements in the absorption over a broad range of frequencies and impinging angles.

Holey random walks: optics of heterogeneous turbid composites.

We present a probabilistic theory of random walks in turbid media with nonscattering regions. It is shown that important characteristics such as diffusion constants, average step lengths, crossing statistics, and void spacings can be analytically predicted. The theory is validated using Monte Carlo simulations of light transport in heterogeneous systems in the form of random sphere packings and good agreement is found. The role of step correlations is discussed and differences between unbounded and bounded systems are investigated. Our results are relevant to the optics of heterogeneous systems in general and represent an important step forward in the understanding of media with strong (fractal) heterogeneity in particular.

Photon management in two-dimensional disordered media.

Elaborating reliable and versatile strategies for efficient light coupling between free space and thin films is of crucial importance for new technologies in energy efficiency. Nanostructured materials have opened unprecedented opportunities for light management, notably in thin-film solar cells. Efficient coherent light trapping has been accomplished through the careful design of plasmonic nanoparticles and gratings, resonant dielectric particles and photonic crystals. Alternative approaches have used randomly textured surfaces as strong light diffusers to benefit from their broadband and wide-angle properties. Here, we propose a new strategy for photon management in thin films that combines both advantages of an efficient trapping due to coherent optical effects and broadband/wide-angle properties due to disorder. Our approach consists of the excitation of electromagnetic modes formed by multiple light scattering and wave interference in two-dimensional random media. We show, by numerical calculations, that the spectral and angular responses of thin films containing disordered photonic patterns are intimately related to the in-plane light transport process and can be tuned through structural correlations. Our findings, which are applicable to all waves, are particularly suited for improving the absorption efficiency of thin-film solar cells and can provide a new approach for high-extraction-efficiency light-emitting diodes.

Weak localization of light in superdiffusive random systems.

Lévy flights constitute a broad class of random walks that occur in many fields of research, from biology to economy and geophysics. The recent advent of Lévy glasses allows us to study Lévy flights-and the resultant superdiffusion-using light waves. This raises several questions about the influence of interference on superdiffusive transport. Superdiffusive structures have the extraordinary property that all points are connected via direct jumps, which is expected to have a strong impact on interference effects such as weak and strong localization. Here we report on the experimental observation of weak localization in Lévy glasses and compare our results with a recently developed theory for multiple scattering in superdiffusive media. Experimental results are in good agreement with theory and allow us to unveil the light propagation inside a finite-size superdiffusive system.

Enhanced downconversion of UV light by resonant scattering of aluminum nanoparticles.

Metallic nanoparticles are known to enhance nonlinear optical processes due to a local enhancement of the optical field. This strategy has been proposed to enhance downconversion in thin film solar cells, but has various disadvantages, among which is the fact that the enhancement occurs only in a tiny volume close to the particles. We report on a very different physical mechanism that can lead to significant downconversion enhancement, namely, that of resonant light scattering, and which is a large volume effect. We show that only a tiny amount of resonantly scattering metallic (aluminum) nanoparticles is enough to create a significant enhancement of the fluorescence of dye molecules in the visible wavelength range. The strategy can be applied in general to increase the emission of UV-absorbing constituents, and is of particular use for solar energy.

Role of quenching on superdiffusive transport in two-dimensional random media.

Transport in random media is known to be affected by quenched disorder. From the point of view of random walks, quenching induces correlations between steps that may alter the dynamical properties of the medium. This paper is intended to provide more insight into the role of quenched disorder on superdiffusive transport in two-dimensional random media. The systems under consideration are disordered materials called Lévy glasses that exhibit large spatial fluctuations in the density of scattering elements. We show that in an ideal Lévy glass the influence of quenching can be neglected, in the sense that transport follows to very good approximation that of a standard Lévy walk. We also show that, by changing sample parameters, quenching effects can be increased intentionally, thereby making it possible to investigate systematically diverse regimes of transport. In particular, we find that strong quenching induces local trapping effects which slow down superdiffusion and lead to a transient subdiffusivelike transport regime close to the truncation time of the system.

Multiple scattering of light in superdiffusive media.

Light transport in superdiffusive media of finite size is studied theoretically. The intensity Green's function for a slab geometry is found by discretizing the fractional diffusion equation and employing the eigenfunction expansion method. Truncated step length distributions and complex boundary conditions are considered. The profile of a coherent backscattering cone is calculated in the superdiffusion approximation.