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Bio-Inspired Artificial Helical Chromatophore for Stealth Mode

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Bio-Inspired Artificial Helical Chromatophore for Stealth Mode Bio-inspired Artificial Helical Chromatophore for Stealth Mode Duck Weon Lee Department of Chemistry and Material Science, Aalto University, PO Box 16100, FI-00076 AALTO, Finland Abstract Stealth technology has been very usefully applied in the military fields and is now becoming more prominent as a strategic technology. In nature, the firefly squid can protect itself from enemies using camouflage as a stealth mode. On the other hand, it is able to send fluorescent signals to attract prey by switching into a bright mode. Despite the development of many existing biomimetic materials, there are significant constraints related to their color-changeable velocity and mobility. Herein, we have developed a bio-inspired artificial thermochromic material system, which can reversibly switch between stealth and bright modes and thus provide a means to adapting to one’s environment analogous to the strategy applied by firefly squids. Through vertical contraction, a helically coiled yarn artificial muscle, selectively coated by Rhodamine B and TiO2, can switch between fluorescent and stealth modes with a maximum speed of 0.31 cm/s. Upon external thermal impulse, artificial thermochromic muscle can spin up to 309° and achieve a negative strain of 84.6%. In addition, this research demonstrates thermochromic effects even in underwater aqueous conditions, showing applicability toward underwater robotics. With the cost-effectiveness of the demonstrated system, the developed artificial thermochromic muscles can be implemented into a variety of applications, such as colorimetric sensors and aqueous color-changeable soft robotics. Stealth technology, a type of camouflage, can be used as an antidetection technology to hide aircraft, submarines, satellites, and missiles from sonar, infrared, radar, and other detectors which take advantage of a power and direction of electromagnetic radiation1–3. Hence, depending on how to block the electromagnetic radiation by using a specific structure and material, a developing material can be as a unique stealth defender. Also, several conceptual cloaking devices have been actively studied because their specific structure and material properties creating own refractive properties diffusing light is able to cause the cloaking phenomenon under diverse environments4,5. Hence, this state-of-the-art technology has been developed with diverse types such as active camouflage, plasma stealth, and Howell devices5– 7. Among these technologies, active camouflage technology can be mixed into its surroundings using a specific painting and structure capable of changing luminosity, which has critical potential that camouflages objects from visual detection. This camouflage has existed and evolved in nature as a means of protecting one's life from enemies for a long time8–11. For example, cephalopods are able to alter their skin color in response to external environments, such as ambient temperature, pressure, and visible changes that trigger rapid adaptive camouflage12. In particular, the firefly squid is able to produce fluorescent light flashes used as warning signals against predators for other colleagues around or when approaching their prey in a sneaky way, and can then quickly return to stealth mode13. This camouflage is based on reversible structural changes in “chromatophores” containing an elastic pouch including diverse pigments and a set of radial muscles striped with diagonal lines with nerves and glia11,13,14. In other words, the radial muscles reversibly control the fluorescence, and thus the appearance of bright colorful spots on the pliant skin of firefly squids by expanding and retracting a pigment sac. Myofilaments in radially arranged muscles contract to stretch a thin disk of the pigment sac to cause a bright mode, and the apparent color can change without actual fluorophores undergoing chemical changes13,15,16. Analogous to the cephalopods’ skin, existing man-made fluorescent actuators can change their color in response to external physical forces, such as straining, pressing, and shearing16. Also, many bio-inspired applications, signaled by a color change, such as stretchable and wearable electrochromic devices17, electro-mechano-chemically responsive elastomers9,18 and color-changeable strain detectors and tactile sensors,8,15 have been demonstrated. Yun et al. also reported that color changes caused by external physical forces are able to serve as a visual indicator of the energy storage of a material system working as a supercapacitor19. Figure 1. Bright and stealth modes of the firefly squid and bio-inspired artificial chromatophore. a) A bright mode of the firefly squid with an expanded chromatophore by the contracted radial muscles (inset), b) A stealth mode of the firefly squid with a contracted chromatophore via stretched radial muscles (inset), c) The bright and d) stealth mode of optical images and specifications of the bio-inspired helical artificial chromatophore. However, in the above referred existing materials, physical forces must be directly applied to the material to induce a color change, thus indicating that the rate of the color change is directly related to how fast expanding or contracting mechanical deformation occurs. Also, some of them couldn’t be immediately and reversibly switched to a desired various level of color, consistently. Hence, the existing mechanochromic materials still leave an open gap between nature’s ability to produce rapidly adapting colors without direct physical contact9,10,20,21. Furthermore, although the velocity of the color change is a crucial factor as a method saving their lives in the nature, not many research studies have explained this function in detail22–24. In here, we developed a bio-inspired artificial chromatophore rapidly carrying out stealth mode from bright mode precisely and reversibly controlled by non-contact stimulus in air or aqueous conditions. To develop a useful artificial chromatophore, which is able to provide a gradual and extremely fast change in fluorescence emission, it employed a helical nylon artificial muscle with homochirality as a substrate for mimicking fluorescent effects in a chromatophore of the firefly squid in Figs. 1a and 1b. In particular, the choice of using homochiral nylon artificial muscle was motivated by the helical structure offering advantages of a hidden inner surface upon contraction of the coiled artificial muscle structure. When the artificial muscle unfolded, the inner and outer sides were exposed at the same time, but only the outer side was visible when closed25-28. Also, through the cylindrical-symmetry structure, the artificial pigment sacs on the inner surface of the helix were capable of absorption, reflection, and fluorescent emission against UV-Vis spectrum (300-800 nm) for all directions, when the system was in bright mode. Therefore, the helical structure overcame limitations of the direction in which the external stimulus was received for the conventional two-dimensional (2D) existing fluorescent actuator or mechanochromic materials15,29. Moreover, uniaxial string contraction in the helical structure through released shear force by thermal energy could substitute the anchoring mechanism of radial muscles. These muscles are responsible for areal expansion and retraction of the pigment sac enabling fluorescence emission in the firefly squid as shown in the inset of Figs. 1a and 1b25,26,30,31. Thus, it was possible to allow external control of expansion and contraction of the artificial chromatophores where thermal energy was used to regulate the exposed area of the pigment sac, defined as the adjacent area between the upper and bottom strings. Hence, the active strings in the helical structure can similarly act as rapid adaptive radial muscles of the cephalopod stimulated by motoneurons of its central brain, even though their travel direction is different from that of the radial muscles13,32. These remarkable capabilities can be applied into color tunable buoys, stretchable color self-cleanings, and stretchable fire-protective gears under harsh conditions such as marine and mining. Results Fluorescence in the artificial chromatophores was characterized on a muscle of a free length (1.0 cm), 200 μm thickness, 1300 μm outer diameter, 900 μm inner diameter, approximately 0.1 cm single chromatophore size including one dyed section and two strings, 17.4° bias angle (αc), and 0.0025 g/cm of a pure nylon precursor fiber as demonstrated in Figs. 1c and 1d. For the overall fluorescence effect of the helical artificial chromatophore, nylon was selectively dyed by Rhodamine B. This was followed by selectively coating titanium dioxide (TiO2) nanoparticles (NPs), dissolved in an aqueous solution of polyvinyl alcohol (PVA), on a highly twisted yarn. In particular, to make an analogy to the natural world, Rhodamine B was employed as an equivalent to the firefly squid’s pigment sac. Rhodamine B coated on nylon was generally excited over the 320-580 nm wavelength of the UV-Vis spectrum 15,33–35. As a typical acid dye method, nylon yarn was dyed by charging the interaction of Rhodamine B with + positive charges of -NH3 derived from the fibrous -NH2 functional group through ionic interactions. TiO2 in PVA was coated on the outer side of the nylon artificial muscle by spray- coating (Gocheer airbrush kit, U.S.) to scatter, reflect, and absorb UV rays through its high refractive index (nD: 2.488, Rutile: Anatase = 85:15, size: 20 nm, Nanoshel Co., U.S.) 36–39. TiO2 mainly plays the role of UV blocking layer
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