Aegerter, Christof M.
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The Structural Colors of Photonic Glasses
The color of materials usually originates from a combination of wavelength‐dependent absorption and scattering. Controlling the color without the use of absorbing dyes is of practical interest, not only because of undesired bleaching properties of dyes but also regarding minimization of environmental and health issues. Color control without dyes can be achieved by tuning the material's scattering properties in controlling size and spatial arrangement of scatterers. Herein, calibrated photonic glasses (PGs), which are isotropic materials made by random aggregation of nonabsorbing, monodisperse colloidal polystyrene spheres, are used to generate a wide spectral range of purely structural, angular‐independent colors. Experimental reflectance spectra for different sized spheres compare well with a recent theoretical model, which establishes the latter as a tool for color mapping in PGs. It allows to determine the range of visible colors accessible in PGs as function of size, packing fraction, and refractive index of scatterers. It also predicts color saturation on top of the white reflectance as function of the sample's optical thickness. Blue, green, and red are obtained even with low index, while saturated green, cyan, yellow, and magenta can be reached in higher index PGs over several orders of magnitude of sample thickness.
Coherent multiple light scattering in Faraday active materials
Wave propagation in multiple scattering media shows various kinds of coherent phenomena such as coherent backscattering [1, 2] or Anderson localization [3], both of which are intimately connected to the concept of reciprocity. Manipulating reciprocity in such media is a powerful tool to study these phenomena in experiments [4]. Here we discuss the manipulation of reciprocity in reflection and transmission geometry for the case of light propagation in magneto-optical media. We show new experiments on coherent backscattering and speckle correlations in strongly scattering samples containing Faraday active materials (CeF3) with transport mean free path in the μm range, at low temperatures (T < 10 K) and high fields (B = 18 T). Under such conditions we observe the effect of a Faraday rotation saturation in multiple scattering measurements.
Studying foam dynamics in levitated, dry and wet foams using diffusing wave spectroscopy
We use diffusing wave spectroscopy to study the microscopic dynamics of foams. These foams are lev-itated diamagnetically, such that very high liquid fractions can be achieved. We find that at low liquidfraction the dynamics is dominated by local rearrangements, whereas at high liquid fraction the move-ment of bubbles is ballistic and large scale rearrangements are absent. This change in the microscopicdynamics coincides with a change in the scaling of coarsening on increasing the liquid fraction that wehave found earlier.
Magnetic-field effects on one-dimensional Anderson localization of light
Transport of coherent waves in multiple-scattering media may exhibit fundamental, nonintuitive phenomena such as halt of diffusion by disorder called Anderson localization. For electromagnetic waves, this phenomenon was observed only in one and two dimensions so far. However, none of these experiments studied the contribution of reciprocal paths nor their manipulation by external fields. In order to weaken the effect of reciprocity of coherent wave transport on Anderson localization in one dimension, we studied light propagation through stacks of parallel Faraday-active glass slides exposed to magnetic fields up to 18 T. Measurements of light transmission statistics are presented and compared to one-dimensional (1D) transfer-matrix simulations. The latter reveals a self-organization of the polarization states in this system leading to a saturation of the Faraday rotation-induced reciprocity breaking, an increase of the localization length, and a decrease of transmission fluctuations when reciprocity is broken. This is confirmed experimentally for samples containing small numbers of slides while for larger samples a crossover from a 1D to a quasi-1D transport regime is found.
Resonant transport and near-field effects in photonic glasses
A fundamental quantity in multiple scattering is the transport mean free path the inverse of which describes the scattering strength of a sample. In this paper, we emphasize the importance of an appropriate description of the effective refractive index neff in multiple light scattering to accurately describe the light transport in dense photonic glasses. Using neff as calculated by the energy-density coherent-potential approximation we are able to predict the transport mean free path of monodisperse photonic glasses. This model without any fit parameter is in qualitative agreement with numerical simulations and in fair quantitative agreement with spectrally resolved coherent backscattering measurements on new specially synthesized polystyrene photonic glasses. These materials exhibit resonant light scattering perturbed by strong near-field coupling, all captured within the model. Our model might be used to maximize the scattering strength of high index photonic glasses, which are a key in the search for Anderson localization of light in three dimensions.
Probing Anderson localization of light by weak non-linear effects
Breakdown of wave transport due to strong disorder is a universal phenomenon known as Anderson localization (AL). It occurs because of the macroscopic population of reciprocal multiple scattering paths, which in three dimensional systems happens at a critical scattering strength. Intensities on these random loops should thus be highly increased relative to those of a diffusive sample. In order to highlight localized modes of light, we exploit the optical nonlinearities of TiO2. Power dependent and spectrally resolved time of flight distribution measurements in transmission through slabs of TiO2 powders at various turbidities reveal that mostly long loops are affected by nonlinearities and that the deviations from diffusive transport observed at long times are due to these localized modes. Our data are a first step in the experimental investigation of the interplay between nonlinear effects and AL in 3D.
Tunable high-index photonic glasses
Materials with extreme photonic properties such as maximum diffuse reflectance, high albedo, or tunable band gaps are essential in many current and future photonic devices and coatings. While photonic crystals, periodic anisotropic structures, are well established, their disordered counterparts, photonic glasses (PGs), are less understood despite their most interesting isotropic photonic properties. Here, we introduce a controlled high index model PG system. It is made of monodisperse spherical TiO2 colloids to exploit strongly resonant Mie scattering for optimal turbidity. We report spectrally resolved combined measurements of turbidity and light energy velocity from large monolithic crack-free samples. This material class reveals pronounced resonances enabled by the possibility to tune both the refractive index of the extremely low polydisperse constituents and their radius. All our results are rationalized by a model based on the energy coherent potential approximation, which is free of any fitting parameter. Surprisingly good quantitative agreement is found even at high index and elevated packing fraction. This class of PGs may be the key to optimized tunable photonic materials and also central to understand fundamental questions such as isotropic structural colors, random lasing or strong light localization in 3D.
Can 3D light localization be reached in ‘white paint’?
When waves scatter multiple times in 3D random media, a disorder driven phase transition from diffusion to localization may occur (Anderson 1958 Phys. Rev. 109 1492-505; Abrahams et al 1979 Phys. Rev. Lett. 42 673-6). The question of classical localization: a theory of white paint? Anderson suggested the possibility to observe light localization in TiO2 samples (Anderson 1985 Phil. Mag. B 52 505-9). We recently claimed the observation of localization effects measuring photon time of flight (ToF) distributions (Störzer et al 2006 Phys. Rev. Lett. 96 063904) and evaluating transmission profiles (TPs) (Sperling>et al 2013 Nat. Photonics 7 48-52) in such TiO2 samples. Here we present a careful study of the long time tail of ToF distributions and the long time behavior of the TP width for very thin samples and different turbidities that questions the localization interpretation. We further show new data that allow an alternative consistent explanation of these previous data by a fluorescence process. An adapted diffusion model including an appropriate exponential fluorescence decay accounts for the shape of the ToF distributions and the TP width. These observations question whether the strong localization regime can be reached with visible light scattering in polydisperse TiO2 samples, since the disorder parameter can hardly be increased any further in such a 'white pain't material.
Coarsening dynamics of three-dimensional levitated foams : From wet to dry
We study diamagnetically levitated foams with widely different liquid fractions. Due to the levitation, drainage is effectively suppressed and the dynamics is driven by the coarsening of the foam bubbles. For dry foams, the bubble size is found to increases as the square root of foam age, as expected from a generalized von Neumann law. At higher liquid content the behavior changes to that of Ostwald ripening where the bubbles grow with the 1/3 power of the age. Using Diffusing Wave Spectroscopy we study the local dynamics in the different regimes and find diffusive behavior for dry foams and kinetic behavior for wet foams.