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Thank you for visiting nature. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser or turn off compatibility mode in Internet Explorer. In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript. Structural colors have drawn wide attention for their potential as a future printing technology for various applications, ranging from biomimetic tissues to adaptive camouflage materials.

However, an efficient approach to realize robust colors with a scalable fabrication technique is still lacking, hampering the realization of practical applications with this platform. Here, we develop a new approach based on large-scale network metamaterials that combine dealloyed subwavelength structures at the nanoscale with lossless, ultra-thin dielectric coatings.

By using theory and experiments, we show how subwavelength dielectric coatings control a mechanism of resonant light coupling with epsilon-near-zero regions generated in the metallic network, generating the formation of saturated structural colors that cover a wide portion of the spectrum. The network-like architecture of these nanomaterials allows for high mechanical resistance, which is quantified in a series of nano-scratch tests.

With such remarkable properties, these metastructures represent a robust design technology for real-world, large-scale commercial applications. Billions of years ago, green algae originated life, changing the face of the earth from gray to green and paving the way for the life forms we see today 1. Since then, living organisms have extensively used color for a variety of purposes, ranging from communication to self-defense, from reproduction to camouflage 2. The enormous variety of colors, such as the sapphire blue wings of the Morpho butterfly 3 , 4 and the thermochromic coloration of the chameleon 5 , has stimulated the interest of researchers dating back to seventeenth century, when Hooke theorized about the origin of color in the brilliant feathers of peacocks and ducks 6.

The engineering of structural colors from artificial photonic structures has attracted conspicuous interest in research due to the many applications that can potentially be opened by this technology 5 , 9 , 10 , 11 , 12 , 13 , 14 , 15 , 16 , Structural colors based on photonic crystals and metamaterials have been explored, showing very promising results, including the possibility to create colors at the diffraction limit A major challenge is overcoming the problems of limited scalability and lack of robustness, which affect the real-world applicability of photonic crystals and classical metamaterials.

It is therefore highly desirable to investigate new approaches that can transform these initial breakthroughs into real-world applications. In the following, we describe a new biomimetic material that overcomes the aforementioned challenges, introducing a new type of structural coloration that is highly scalable and extremely robust. This nanomaterial takes inspiration from subwavelength nanoscale networks identified in the feathers of Cotinga maynana , a South American bird The interaction of light waves with complex materials has already been reported to have a series of fascinating dynamics, ranging from energy harvesting to ultra-dark nanomaterials and beyond 7 , 11 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , Taking inspiration from the Cotinga maynana feathers as an example in nature of a network-based optical nanomaterial, we create complex nano-photonic structures that combine a cellular metallic network 28 , 29 with subwavelength coatings made by lossless dielectrics.

This material combination provides significant advantages for real-world applications: In this scenario, the component of the wavevector parallel to the interface is not conserved, resulting in a highly spatially dependent electromagnetic response. Taking advantage of such a complex light—matter interaction, we illustrate here how to create colors with remarkable properties.

The morphological analysis of the samples was studied via scanning electron microscopy assisted by focused ion beam etching FIB. The compositional analysis was performed by Rutherford backscattering spectrometry. Detailed information is given in the Supplementary Information. The electromagnetic reflectance of the coated samples was measured using a variable-angle spectroscopic ellipsometer from J. Woollam Co. The dielectric constant of the Al 2 O 3 coating deposited by ALD was determined using a Cauchy model by analyzing a nm-thick Al 2 O 3 coating deposited on a Si wafer.

Numerical simulations were carried out using our parallel code NANOCPP, which is a highly scalable up to hundreds of thousands CPU Maxwell equation solver, able to include dispersive materials with arbitrary dispersion curves To build a realistic model for our sample, we considered a metallic structure whose profile was extracted from the morphological analysis of the samples FIB shown in Figure 1a. The dispersion parameters of the various materials were taken from direct measurements.

Observation of structural colors in random metallic networks with subwavelength dielectric coatings. The photographs were taken under illumination from ceiling lights. The RGB color space is marked by the triangle area. The chromaticity is calculated directly from reflectance spectra obtained either experimentally circles markers or by FDTD simulations dashed line.

The edges of the tongue-shaped plane correspond to color values of maximal saturation. We selected dealloying to assemble a nanoscale metallic network with controllable features. This method, first proposed by Raney to synthesize metal catalysts 31 , utilizes the selective dissolution of the less noble constituent of an alloy during wet etching. In our experiments, nm-thick Pt. Characteristic geometrical features of the network can be altered by changing the etching time, the etchant concentration or the initial composition of the thin film 32 , 33 , 34 , 35 , We characterized the growth of the subwavelength Al 2 O 3 coatings by Rutherford backscattering spectroscopy and FIB-assisted scanning electron microscopy see Supplementary Information.

A three-dimensional image of the Pt. In a final series of experiments, we characterized the optical response of the network metamaterial for different thicknesses of the dielectric layer Al 2 O 3. These experiments unveiled a very interesting mechanism of structural coloration from the nanowire network, as shown in Figure 1b. By changing the coating thickness, we observed the formation of a multitude of colors spanning from yellow, orange and red to, finally, blue. The same physical effect with the optical response blue-shifted and smaller color range was observed for a Pt-Al network see Supplementary Information and Supplementary Fig.

Conversely, when the same coatings were deposited on a dense PtYAl metal thin film, no particular color was produced see Supplementary Information and Supplementary Fig. The colors observed in the metallic network were saturated and go even slightly beyond the red green blue gamut in the CIE chromaticity diagram Figure 1c. To illustrate that these colors were consistently observed by varying Al 2 O 3 layer thickness, we compared experimental results with theoretical predictions based on finite-difference time-domain FDTD simulations.

For the latter, we used a two-dimensional section of the FIB tomography of the sample illustrated in Figure 1a. Our FDTD simulations, shown in Figure 1c as a dotted line, reproduced the experimental results well, confirming the possibility of achieving such a large variety of colors by tuning the thickness of the Al 2 O 3 layer. Figure 1b shows experimental images of samples characterized by different thicknesses of Al 2 O 3.

Remarkably, despite the existence of the metallic nanoscale network below the Al 2 O 3 layer, the samples demonstrated a highly uniform color in all different configurations. A comparison with FDTD calculations is provided in Figure 1d , which illustrates the color palette that can be observed when the thickness of Al 2 O 3 increases. To emphasize that the structural coloration in these nanoplasmonic structures can be achieved by various deposition techniques, we also fabricated a structural colored graphic arts by using physical vapor deposition.

The bicolored graphic art combines a highly uniform structural color blue with a metallic white color dense film. The material choice for the coating layer is not limited to Al 2 O 3 a lossless dielectric. Dielectric coatings with and without losses could, in principle, be used to alter the plasmonic response and finally change the structural coloration. Another approach to altering the color impression, especially its saturation, is to change the number of trapping sites within the network metamaterial, for example, by reducing the metamaterial thickness.

Examples of different graphic arts designs with structural colors from metamaterial networks. Photograph and optical micrograph of a colored graphic art designed by combining a RF-sputtered Al 2 O 3 -coated network metamaterial and photolithography. The inset shows an optical micrograph illustrating a detail of the graphic art and the uniformity of the color. To quantify the mechanical robustness of these colors, we resort to nano-scratch resistance testing Figure 3a , which is an ideal technique to characterize the adhesion failure of coatings.

A detailed description of the experimental procedure we used is given in the Supplementary Information. Figure 3b reports optical micrographs of four representative nano-scratch tests. Figure 4 illustrates s -polarized reflectivity spectra at normal Figure 4a and oblique Figure 4b—4e incidence for different alumina coating thickness. Figure 4a demonstrates that the formation of colors originates from a large red shift of the reflectivity response of the nanomaterial, observed when the Al 2 O 3 layer changes thickness.

FDTD simulations quantitatively reproduce well the experimental results, confirming the principal role of the Al 2 O 3 coating layer in red-shifting the spectral response of the material. The mean angular dispersion of the reflectance minimum has been determined from the reflectance spectra obtained by ellipsometry. These experiments show that the structural colors observed in Figure 1 are non-iridescent, that is, robust against large changes of the incident angle.

Wear properties of the structural colors. A diamond stylus is used to scratch the film with progressively increasing load. The critical load characterizing the adhesion failure of the films is indicated by a pink arrow. Optical properties of the network metamaterials: The value of reflectance is indicated by the color bar. In this section, we analyze in more detail the mechanisms by which structural colors are created and observed in the metallic network of Figure 1.

When polychromatic light impinges on the structure of Figure 1a , the interaction between light and matter generates surface plasmon polaritons SPP 38 , which are surface waves localized at the metal-dielectric interface of the structure 7. In our samples Figure 5a , the motion of SPP develops along complex trajectories in space due to a strongly disordered metallic profile, Figure 5a , inset.

It is convenient to study this motion in a new curvilinear system, whose axes are parallel to the spatial trajectories of SPP. Figure 5a shows how these coordinates appear in the original space. When we change spatial coordinates in any electromagnetic system, Maxwell equations remain invariant if we introduce an inhomogeneous refractive index distribution that makes the two reference systems equivalent 39 , The two structures of Figure 5a and 5b are exactly equivalent: This is an exact result of Maxwell equations that contains no approximation.

This result also implies that when light impinges on the structure of Figure 5a , it happens to propagate in the medium of Figure 5b. The calculation of a conformal grid for the disordered surface of Figure 5a requires a new formulation of optical conformal mapping, which we recently developed, and allows for the generation of conformal grids for arbitrary structures with arbitrary-large numerical precision.

This approach is relatively involved, and it will be discussed in a future work. Generation of an equivalent ENZ material in the metallic nanowire network of Figure 1a. When light impinges on this structure, it excites the propagation of SPP waves, which move along the complex surface of the metal a , inset. The two systems of a and b are exactly the same for light propagation. The equivalent structure of b demonstrates a complex network of ENZ structures b , dark blue area , which are created by points of convex metallic curvature right inset.

As observed in the insets of Figure 5a and 5b dashed lines , ENZ regions are created in the points where the metallic surface is convex, whereas high dielectric permittivities originate in the points where the surface is concave. When waves propagate into an ENZ material, the phase velocity diverges, thus creating standing waves with infinite wavelengths 41 , 42 , We illustrated these dynamics by a series of FDTD simulations. Figure 6a presents a magnified version of Figure 4a , showing FDTD-calculated reflectivity spectra for different thicknesses of the Al 2 O 3 layer.

FDTD results corresponding to different combinations of alumina thicknesses and input wavelengths are summarized in Figure 6b—6j. When light impinges on the disordered metallic structure Figure 6b , some energy is scattered back, generating components along all directions in space, whereas the remainder is coupled into SPP waves. As illustrated in Figure 6c—6e , which show FDTD-calculated electromagnetic energy density distributions, SPP waves are completely localized in the proximity of different convex points of the surface, exactly where the ENZ regions are formed.

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Thank you for visiting nature. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser or turn off compatibility mode in Internet Explorer. In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript. Structural colors have drawn wide attention for their potential as a future printing technology for various applications, ranging from biomimetic tissues to adaptive camouflage materials. However, an efficient approach to realize robust colors with a scalable fabrication technique is still lacking, hampering the realization of practical applications with this platform. Here, we develop a new approach based on large-scale network metamaterials that combine dealloyed subwavelength structures at the nanoscale with lossless, ultra-thin dielectric coatings.

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