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Optics Express

  • Editor: Andrew M. Weiner
  • Vol. 22, Iss. 16 — Aug. 11, 2014
  • pp: 19386–19400
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Disorder and broad-angle iridescence from Morpho-inspired structures

Bokwang Song, Seok Chan Eom, and Jung H. Shin  »View Author Affiliations


Optics Express, Vol. 22, Issue 16, pp. 19386-19400 (2014)
http://dx.doi.org/10.1364/OE.22.019386


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Abstract

The ordered, lamellae-structured ridges on the wing scales of Morpho butterflies give rise to their striking blue iridescence by multilayer interference and grating diffraction. At the same time, the random offsets among the ridges broaden the directional multilayer reflection peaks and the grating diffraction peaks that the color appears the same at various viewing angles, contrary to the very definition of iridescence. While the overall process is well understood, there has been little investigation into confirming the roles of each factor due to the difficulty of controllably reproducing such complex structures. Here we use a combination of self-assembly, selective etching, and directional deposition to fabricate Morpho-inspired structure with controlled random offsets. We find that while random offsets are necessary, it alone is not sufficient to produce the broad-angle reflection of Morpho butterflies. We identify diffraction as a critical factor for the bright, anisotropic broadening of the reflection peak of Morpho butterflies to a solid angle of 0.23 sr, and suggest random macroscopic surface curvature as a practical alternative, with an isotropic broad reflection peak whose solid angle can reach 0.11 sr at an incident angle of 60 o.

© 2014 Optical Society of America

1. Introduction

Many insects possess intricate structures in the wings and scales that cause diffraction, interference, scattering, and many combinations thereof [1

1. P. Vukusic and J. R. Sambles, “Photonic structures in biology,” Nature 424(6950), 852–855 (2003). [CrossRef] [PubMed]

3

3. L. P. Biró and J. P. Vigneron, “Photonic nanoarchitectures in butterflies and beetles: valuable sources for bioinspiration,” Laser Photon. Rev. 5(1), 27–51 (2011). [CrossRef]

]. They affect reflection [4

4. S. Kinoshita, S. Yoshioka, and J. Miyazaki, “Physics of structural colors,” Rep. Prog. Phys. 71(7), 076401 (2008). [CrossRef]

], polarization [5

5. V. Sharma, M. Crne, J. O. Park, and M. Srinivasarao, “Structural origin of circularly polarized iridescence in jeweled beetles,” Science 325(5939), 449–451 (2009). [CrossRef] [PubMed]

], and absorption [6

6. P. B. Clapham and M. C. Hutley, “Reduction of lens reflexion by moth eye principle,” Nature 244(5414), 281–282 (1973). [CrossRef]

] of the incident light, and are responsible for some of the most impressive optical phenomena in the natural world. Studying these phenomena has led to not only increased knowledge, but also possible breakthroughs in many diverse and critical applications such as displays [7

7. E. Iwase, K. Matsumoto, and I. Shimoyama, “The structural-color based on the mechanism butterfly wing coloring for wide viewing angle reflective display,” in Proceedings of 17th IEEE international conference on MEMS (Maastricht Exhibition and Convention Centre, Maastricht, 2004), pp. 105–108. [CrossRef]

], sensing [8

8. R. A. Potyrailo, H. Ghiradella, A. Vertiatchikh, K. Dovidenko, J. R. Cournoyer, and E. Olson, “Morpho butterfly wing scales demonstrate highly selective vapour response,” Nat. Photon. 1(2), 123–128 (2007). [CrossRef]

,9

9. A. D. Pris, Y. Utturkar, C. Surman, W. G. Morris, A. Vert, S. Zalyubovskiy, T. Deng, H. T. Ghiradella, and R. A. Potyrailo, “Towards high-speed imaging of infrared photons with bio-inspired nanoarchitectures,” Nat. Photon. 6(3), 195–200 (2012). [CrossRef]

], and energy conversions and solar cells [10

10. K. Forberich, G. Dennler, M. C. Scharber, K. Hingerl, T. Fromherz, and C. J. Brabec, “Performance improvement of organic solar cells with moth eye anti-reflection coating,” Thin Solid Films 516(20), 7167–7170 (2008). [CrossRef]

].

Recently, we have demonstrated that by spin-coating a close-packed monolayer of randomly sized silica microspheres, a substrate with random offsets can be generated and used to fabricate Morpho-inspired structural reflectors that show bright, angle-independent color [32

32. K. Chung, S. Yu, C. J. Heo, J. W. Shim, S. M. Yang, M. G. Han, H. S. Lee, Y. Jin, S. Y. Lee, N. Park, and J. H. Shin, “Flexible, angle-independent, structural color reflectors inspired by morpho butterfly wings,” Adv. Mater. 24(18), 2375–2379 (2012). [CrossRef] [PubMed]

]. This approach differed from other, recent reports on successfully introducing randomness for broad-angle iridescence [33

33. D. Ge, L. Yang, G. Wu, and S. Yang, “Spray coating of superhydrophobic and angle-independent coloured films,” Chem. Commun. 50(19), 2469–2472 (2014). [CrossRef] [PubMed]

] in that the color was controlled by multilayer reflection as in actual Morpho butterflies, thus enabling accurate color tuning across a wide range, and that a continuous distribution of disorder, both vertical and horizontal, was generated spontaneously in a large area without any lithography or etching [34

34. L. P. Biró, K. Kertész, E. Horváth, G. I. Márk, G. Molnár, Z. Vértesy, J.-F. Tsai, A. Kun, Zs. Bálint, and J. P. Vigneron, “Bioinspired artificial photonic nanoarchitecture using the elytron of the beetle Trigonophorus rothschildi varians as a ‘blueprint’,” J. R. Soc. Interface 7(47), 887–894 (2010). [CrossRef] [PubMed]

,35

35. I. Tamáska, Z. Vértesy, A. Deák, P. Petrik, K. Kertész, and L. P. Biró, “Optical properties of bioinspired disordered photonic nanoarchitectures,” Nanopages 8(2), 17–30 (2013). [CrossRef]

]. Unfortunately, the use of close-packed spheres creates identical horizontal and vertical offsets such that one cannot control the vertical offsets independently, and suppresses the effect of diffraction due to the continuous multilayer structure. In this paper, we use the silica microspheres as selective etch mask to fabricate a substrate with controlled vertical disorder in order to investigate its effect on the broadening of the reflection peaks. Based on quantitative comparison with actual Morpho butterflies and numerical simulations, we find that while vertical disorder is necessary to broaden the reflection peaks, it alone is not sufficient. In order to fully replicate the bright, broad-angle blue of Morpho butterflies, it is critical to include other effects such as diffraction that suppress the specular reflection and provide non-specular reflection. Surprisingly, we find that random macroscopic surface curvature, which is often overlooked in theoretical analysis, can be quite effective in generating such bright, broad-angle reflection.

2. Fabrication with disorder control

A monolayer of silica microspheres with diameters ranging from 250 nm to 440 nm (ethanolic silica suspension with 8 wt%) was spin-coated (3000 rpm) on a Si wafer, and then fixed to the Si substrate by a high temperature (1000 °C) annealing with oxygen gas. The microspheres were then used as etch-mask during CHF3/O2 plasma etching to transfer the texture of the randomly sized spheres onto the underlying Si substrate. By controlling the gas flow (CHF3: 30 sccm, O2: 0 sccm to 10 sccm) and operating pressure (15 mT to 40 mT), we could selectively etch either Si or SiO2, either to enhance or to diminish the original height difference among the silica microspheres. Afterward, a 300 nm thick layer of Cr was deposited to serve as the absorption layer for higher color purity [32

32. K. Chung, S. Yu, C. J. Heo, J. W. Shim, S. M. Yang, M. G. Han, H. S. Lee, Y. Jin, S. Y. Lee, N. Park, and J. H. Shin, “Flexible, angle-independent, structural color reflectors inspired by morpho butterfly wings,” Adv. Mater. 24(18), 2375–2379 (2012). [CrossRef] [PubMed]

], similar to melanin-containing scales in Morpho butterflies [28

28. S. Yoshioka and S. Kinoshita, “Structural or pigmentary? Origin of the distinctive white stripe on the blue wing of a Morpho butterfly,” Proc. Biol. Sci. 273(1583), 129–134 (2006). [CrossRef] [PubMed]

]. Finally, 8 pairs SiO2/TiO2 layers of 73 nm and 38 nm, respectively, were sputter-deposited. The deposition pressure was kept intentionally low at 0.3 mT to induce directional growth and preservation of the random texture of the substrate in the deposited multilayers. A schematic description of the fabrication process is shown in Fig. 1.
Fig. 1 A schematic description of the fabrication process.

Figure 2 shows the scanning-electron microscope (SEM) images of the original monolayer of silica microspheres and the etched Si substrates, and their vertical and horizontal offsets as measured by SEM and atomic force microscope (AFM).
Fig. 2 Structural analysis of disorder-controlled substrate. Cross-section SEM image (10 o-tilted) of (a) monolayer of randomly sized silica microspheres on the Si substrate (substrate s1), (b) etched Si substrate with SiO2/Si etching selectivity of 1 (substrate s2), (c) with etching selectivity 2 (substrate s3), and (d) with etching selectivity 3 (substrate s4). (e) Vertical height distribution of the substrates s1 - s4, as measured by SEM and AFM. The black arrows in inset indicate vertical height measured. (f) The horizontal distance distribution of the substrates s1 - s4 as measured by SEM and AFM. The black arrow in inset indicates horizontal distance measured. Scale bars, 1μm.
We see that using selective etching, the distribution of the vertical offsets can be controlled such that the standard deviation is reduced from 46 nm to 12 nm. On the other hand, the distribution of the horizontal offsets remains almost unchanged (Table 1), confirming that we are isolating the effect of the randomness in the vertical offsets.

Table 1. The statistical values of nanoscale offsets of the substrates in Fig. 2.

table-icon
View This Table

3. Optical analysis

3.1. Reflectance measurement methods

Angular and normal reflectance were measured for optical analysis. Angular reflectance was measured using a goniospectrophotometer consisting of two optical fibers [Fig. 3].
Fig. 3 A schematic view of measurement setup for angular reflectance.
The incident light from deuterium-halogen source (Avantes, AvaLight-DH-S-BAL) was guided and illuminated by an optical fiber, and collimated by lens. The diameter of beam spot on the samples was 5 mm. Reflected beam was coupled into the other optical fiber and measured by a spectrometer (Avantes, AvaSpec-2048). Al mirror was used for the reference. Measured data was calibrated by theoretical reflectance value of Al mirror. Normal reflectance was measured using a reflection probe separated into 2 connectors (Avantes, FCR-7UV200-2-ME). A light source was connected with one of the two connectors and illuminated through the probe end. Reflected beam was coupled into the probe end and measured by a spectrometer connected with the other connector. The same light source, spectrometer, and reference as angular reflectance measurements were used for normal reflectance measurements. In case of Morpho butterflies, the plane of incidence was adjusted to be parallel to the multilayered ridges. A schematic description of the measurement setup is shown in Fig. 3.

3.2. Results and analysis

Figure 4 shows the SEM and optical images of the Morpho butterflies and deposited multilayer films, normal reflectance spectra normalized to max value, and the corresponding colors.
Fig. 4 Images and normal reflectance. (a) Optical images of the wing of Morpho didius, the wing of Morpho rhetenor, a wrinkled multilayer film deposited on s1 unfixed to the Si substrate (defined as f0), a flat multilayer film deposited on s1 fixed to the Si substrate (defined as f1), flat multilayer films deposited on s2 - s4 (defined as f2 - f4) from left to right. (b) Cross-sectional SEM image of multilayered ridges on the scale of Morpho rhetenor butterfly. (c) Cross-sectional SEM image of the deposited multilayer films on microspheres. (d) Cross-sectional SEM image of the deposited multilayer films on the etched Si substrate f3. (e) Normal reflectance spectra, normalized to the max value, of the deposited multilayer films f0 - f4. Inset: Corresponding color coordinates on the 1931 CIE diagram. Scale bars, 1μm.
Note that the multilayer thin films deposited on both silica microspheres and etched Si substrates show the random undulations. However, both the continuous nature of the multilayers, as well as their smaller degree of undulations, are different from the discrete, 3D photonic-crystal like ridge structure of Morpho butterflies. Part of the reason for such differences in size is the higher refractive index of the deposited thin film. However, while the physics of reflection from such disordered multilayer structures are the same, these differences in structural details can lead to significant differences in their optical properties, as shall be discussed in detail below. The optical images were taken under ambient light conditions, and the reflectance spectra were measured using a conventional spectrometer under normal directional light conditions. For comparison, we also show the results from a wrinkled multilayer film formed by depositing on a monolayer of random-sized silica microspheres unfixed to the Si substrate, as discussed in [32

32. K. Chung, S. Yu, C. J. Heo, J. W. Shim, S. M. Yang, M. G. Han, H. S. Lee, Y. Jin, S. Y. Lee, N. Park, and J. H. Shin, “Flexible, angle-independent, structural color reflectors inspired by morpho butterfly wings,” Adv. Mater. 24(18), 2375–2379 (2012). [CrossRef] [PubMed]

], K. Chung et al., and from Morpho rhetenor and Morpho didius butterflies. We find that the normal reflectance spectra, and the corresponding color, of the deposited films are very similar to each other, regardless of the vertical disorder or flatness of the film, confirming that the periodicity of multilayers is the dominant factor in determining the color [36

36. K. Chung and J. H. Shin, “Range and stability of structural colors generated by Morpho-inspired color reflectors,” J. Opt. Soc. Am. A 30(5), 962–968 (2013). [CrossRef] [PubMed]

]. However, the optical images clearly show the difference in appearance. While the wrinkled film appears shiny and bright like Morpho butterflies, the flat films appear quite dark, becoming darker as vertical disorder is decreased.

The results of simulations are summarized in Fig. 10.
Fig. 10 Calculated far-field reflection intensities of (a) continuous multilayer structures deposited on a layer of uniformly sized microspheres of diameter 350 nm; (b) continuous multilayer structure with half of the random offsets of sample f1 in Fig. 4; (c) continuous multilayer with the same random offsets as sample f1 in Fig. 4. (d-f) Calculated far-field reflection intensities of structures designed by applying 300 nm gap spacing to the structures in (a)-(c). Schematic views of structure are on top. All calculation were performed under normal incident light. Insets: Plot with larger scale.
From Figs. 10(a)10(c), we confirm that introducing random vertical offsets to a continuous multilayer reduces the specular reflection peak, and introduces significant reflection at non-specular angles. However, as Figs. 10(d)10(f) show, diffraction provides much larger non-specular reflection intensity at greater angles than random vertical offset alone can. Without random offsets, only sharp diffraction peaks are observed. When combined with vertical offsets, however, strong reduction of the specular reflection intensity to less than 20% and continuous non-specular reflection from −30° to + 30° similar to that observed from Morpho butterflies can be achieved.

Figure 11 shows the effects of changing the multilayer pairs, gap spacing, and the incident angle.
Fig. 11 The effect of structural parameter. Calculated far-field reflection intensities of 300 nm gap-applied uniform (the structure in Fig. 10(d)) and random (the structure in Fig. 10(f)) structure with changing (a-b) the number of multilayer pairs under normal incident light; (c-d) the gap spacing between the neighboring elements under normal incident light; (e-f) the incident angle, at wavelength of 460 nm. (g-i) The dependence of total far-field reflection intensities upon each parameter . All calculations were performed at 460nm wavelength.
We find that, as expected, increasing the multilayer pair increases the reflected intensity, while increasing the gap spacing and the incidence angle reduces the reflected intensity. However, the reflected intensity from films with random disorder show much weaker dependence on such parameters than that from uniform films, consistent with the large body of reports on the importance of disorder for stable iridescence. Still, the fact that varying these parameters changes the reflected intensity indicates that a careful optimization of all such parameters in addition to the degree of disorder is necessary for practical applications.

5. Conclusion

In conclusion, we have investigated the effect of nanoscale disorder in Morpho-inspired structures. By directly controlling the vertical disorder in the multilayer structure, we show that while vertical disorder is an essential ingredient in broadening the reflection peaks, it is not sufficient. In case of Morpho butterflies, diffraction plays a critical role to fully generate the broad reflection; however, other methods to suppress specular reflection and generate broad reflections such as random surface curvature can work just as well, as we demonstrate by bright, broad-angle reflection of wrinkled Morpho-inspired thin films.

Acknowledgments

This work was supported in part by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIP) (Grant No. 2010-0029255, GRL: Grant No. K20815000003-11A0500-00310).

References and links

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P. Vukusic and J. R. Sambles, “Photonic structures in biology,” Nature 424(6950), 852–855 (2003). [CrossRef] [PubMed]

2.

M. Srinivasarao, “Nano-optics in the biological world: beetles, butterflies, birds, and moths,” Chem. Rev. 99(7), 1935–1962 (1999). [CrossRef] [PubMed]

3.

L. P. Biró and J. P. Vigneron, “Photonic nanoarchitectures in butterflies and beetles: valuable sources for bioinspiration,” Laser Photon. Rev. 5(1), 27–51 (2011). [CrossRef]

4.

S. Kinoshita, S. Yoshioka, and J. Miyazaki, “Physics of structural colors,” Rep. Prog. Phys. 71(7), 076401 (2008). [CrossRef]

5.

V. Sharma, M. Crne, J. O. Park, and M. Srinivasarao, “Structural origin of circularly polarized iridescence in jeweled beetles,” Science 325(5939), 449–451 (2009). [CrossRef] [PubMed]

6.

P. B. Clapham and M. C. Hutley, “Reduction of lens reflexion by moth eye principle,” Nature 244(5414), 281–282 (1973). [CrossRef]

7.

E. Iwase, K. Matsumoto, and I. Shimoyama, “The structural-color based on the mechanism butterfly wing coloring for wide viewing angle reflective display,” in Proceedings of 17th IEEE international conference on MEMS (Maastricht Exhibition and Convention Centre, Maastricht, 2004), pp. 105–108. [CrossRef]

8.

R. A. Potyrailo, H. Ghiradella, A. Vertiatchikh, K. Dovidenko, J. R. Cournoyer, and E. Olson, “Morpho butterfly wing scales demonstrate highly selective vapour response,” Nat. Photon. 1(2), 123–128 (2007). [CrossRef]

9.

A. D. Pris, Y. Utturkar, C. Surman, W. G. Morris, A. Vert, S. Zalyubovskiy, T. Deng, H. T. Ghiradella, and R. A. Potyrailo, “Towards high-speed imaging of infrared photons with bio-inspired nanoarchitectures,” Nat. Photon. 6(3), 195–200 (2012). [CrossRef]

10.

K. Forberich, G. Dennler, M. C. Scharber, K. Hingerl, T. Fromherz, and C. J. Brabec, “Performance improvement of organic solar cells with moth eye anti-reflection coating,” Thin Solid Films 516(20), 7167–7170 (2008). [CrossRef]

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S. M. Doucet and M. G. Meadows, “Iridescence: a functional perspective,” J. R. Soc. Interface 6(Suppl 2), S115–S132 (2009). [CrossRef] [PubMed]

12.

S. Berthier, Iridescences: The Physical Colors of Insects (Springer, 2007).

13.

C. W. Mason, “Structural colors in insects. I,” J. Phys. Chem. 30(3), 383–395 (1926). [CrossRef]

14.

C. W. Mason, “Structural colors in insects. II,” J. Phys. Chem. 31(3), 321–354 (1927). [CrossRef]

15.

C. W. Mason, “Structural colors in insects. III,” J. Phys. Chem. 31(12), 1856–1872 (1927). [CrossRef]

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S. Kinoshita and S. Yoshioka, “Structural colors in nature: the role of regularity and irregularity in the structure,” ChemPhysChem 6(8), 1442–1459 (2005). [CrossRef] [PubMed]

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Y. Takeoka, “Angle-independent structural coloured amorphous arrays,” J. Mater. Chem. 22(44), 23299 (2012). [CrossRef]

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S. Berthier, Photonique de Morphos (Springer, 2010).

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H. Ghiradella, “Light and color on the wing: structural colors in butterflies and moths,” Appl. Opt. 30(24), 3492–3500 (1991). [CrossRef] [PubMed]

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33.

D. Ge, L. Yang, G. Wu, and S. Yang, “Spray coating of superhydrophobic and angle-independent coloured films,” Chem. Commun. 50(19), 2469–2472 (2014). [CrossRef] [PubMed]

34.

L. P. Biró, K. Kertész, E. Horváth, G. I. Márk, G. Molnár, Z. Vértesy, J.-F. Tsai, A. Kun, Zs. Bálint, and J. P. Vigneron, “Bioinspired artificial photonic nanoarchitecture using the elytron of the beetle Trigonophorus rothschildi varians as a ‘blueprint’,” J. R. Soc. Interface 7(47), 887–894 (2010). [CrossRef] [PubMed]

35.

I. Tamáska, Z. Vértesy, A. Deák, P. Petrik, K. Kertész, and L. P. Biró, “Optical properties of bioinspired disordered photonic nanoarchitectures,” Nanopages 8(2), 17–30 (2013). [CrossRef]

36.

K. Chung and J. H. Shin, “Range and stability of structural colors generated by Morpho-inspired color reflectors,” J. Opt. Soc. Am. A 30(5), 962–968 (2013). [CrossRef] [PubMed]

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OCIS Codes
(330.0330) Vision, color, and visual optics : Vision, color, and visual optics
(050.1755) Diffraction and gratings : Computational electromagnetic methods
(350.4238) Other areas of optics : Nanophotonics and photonic crystals
(220.4241) Optical design and fabrication : Nanostructure fabrication
(310.6628) Thin films : Subwavelength structures, nanostructures

ToC Category:
Diffraction and Gratings

History
Original Manuscript: May 23, 2014
Revised Manuscript: July 21, 2014
Manuscript Accepted: July 25, 2014
Published: August 4, 2014

Virtual Issues
Vol. 9, Iss. 10 Virtual Journal for Biomedical Optics

Citation
Bokwang Song, Seok Chan Eom, and Jung H. Shin, "Disorder and broad-angle iridescence from Morpho-inspired structures," Opt. Express 22, 19386-19400 (2014)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-22-16-19386


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References

  1. P. Vukusic and J. R. Sambles, “Photonic structures in biology,” Nature424(6950), 852–855 (2003). [CrossRef] [PubMed]
  2. M. Srinivasarao, “Nano-optics in the biological world: beetles, butterflies, birds, and moths,” Chem. Rev.99(7), 1935–1962 (1999). [CrossRef] [PubMed]
  3. L. P. Biró and J. P. Vigneron, “Photonic nanoarchitectures in butterflies and beetles: valuable sources for bioinspiration,” Laser Photon. Rev.5(1), 27–51 (2011). [CrossRef]
  4. S. Kinoshita, S. Yoshioka, and J. Miyazaki, “Physics of structural colors,” Rep. Prog. Phys.71(7), 076401 (2008). [CrossRef]
  5. V. Sharma, M. Crne, J. O. Park, and M. Srinivasarao, “Structural origin of circularly polarized iridescence in jeweled beetles,” Science325(5939), 449–451 (2009). [CrossRef] [PubMed]
  6. P. B. Clapham and M. C. Hutley, “Reduction of lens reflexion by moth eye principle,” Nature244(5414), 281–282 (1973). [CrossRef]
  7. E. Iwase, K. Matsumoto, and I. Shimoyama, “The structural-color based on the mechanism butterfly wing coloring for wide viewing angle reflective display,” in Proceedings of 17th IEEE international conference on MEMS (Maastricht Exhibition and Convention Centre, Maastricht, 2004), pp. 105–108. [CrossRef]
  8. R. A. Potyrailo, H. Ghiradella, A. Vertiatchikh, K. Dovidenko, J. R. Cournoyer, and E. Olson, “Morpho butterfly wing scales demonstrate highly selective vapour response,” Nat. Photon.1(2), 123–128 (2007). [CrossRef]
  9. A. D. Pris, Y. Utturkar, C. Surman, W. G. Morris, A. Vert, S. Zalyubovskiy, T. Deng, H. T. Ghiradella, and R. A. Potyrailo, “Towards high-speed imaging of infrared photons with bio-inspired nanoarchitectures,” Nat. Photon.6(3), 195–200 (2012). [CrossRef]
  10. K. Forberich, G. Dennler, M. C. Scharber, K. Hingerl, T. Fromherz, and C. J. Brabec, “Performance improvement of organic solar cells with moth eye anti-reflection coating,” Thin Solid Films516(20), 7167–7170 (2008). [CrossRef]
  11. S. M. Doucet and M. G. Meadows, “Iridescence: a functional perspective,” J. R. Soc. Interface6(Suppl 2), S115–S132 (2009). [CrossRef] [PubMed]
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