Controlled Preparation of Highly Stretchable, Crack-Free Wrinkled Surfaces with Tunable Wetting and Optical Properties.

Constructing wrinkles by utilizing strain-driven surface instability in film-substrate systems is a general method to prepare micronano structures, which have a wide range of applications in smart surfaces and devices such as flexible electronics, reversible wetting, friction, and optics. However, cracks generated during the preparation and use process significantly affect the uniformity of wrinkled surfaces and degrade the functional properties of the film devices. The realization of crack-free wrinkles with high stretchability in hard film systems is still a great challenge. Here, we report on a facile technique for controllable preparation of large-area, highly stretchable, crack-free wrinkled surfaces by ultraviolet ozone (UVO) treatment of Ecoflex. The thickness dependence of the wrinkles and the in situ wrinkling process during mechanical loading are investigated. The wrinkles including striped, labyrinth-like, herringbone, and transitional structures are controllable by changing strain mode (uniaxial or biaxial), loading history (simultaneous or sequential), strain anisotropy, and gradient loading. The wrinkled surfaces obtained using UVO-treated Ecoflex have tunable wetting and optical properties and can maintain excellent mechanical stability under large strains. This study provides a facile method for the preparation of large-area, crack-free wrinkles, which is simple, fast, low-cost, and robust. The resulting wrinkled surfaces remain stable under high stretching, which is beneficial for many practical applications, especially in the cases of large strains.

Coexistence and Coevolution of Wrinkle and Ridge Patterns in the Film-Substrate System by Uniaxial Compression.

Homogeneous wrinkles and localized patterns are ubiquitous in nature and are useful for a wide range of practical applications. Although various strain-driven surface instability modes have been extensively investigated in the past decades, understanding the coexistence, coevolution, and interaction of wrinkles and localized patterns is still a great challenge. Here, we report on the formation and evolution of coexisting wrinkle and ridge patterns in metal films deposited on poly(dimethylsiloxane) (PDMS) substrates by uniaxial compression. It is found that the evolving surface patterns show unique features of morphological transition from stages I to III: namely, transition from localized ridges to coexisting wrinkles and ridges, and finally to sinusoidal-like structures, as the compression increases. Based on the compressive strain-driven surface instability theory and finite element numerical simulation, the morphological features, transition behaviors, and underlying mechanisms of such complex patterns are investigated in detail, and the changes of amplitude and wavelength versus the strain are consistent with our experiments. This work could promote a better understanding of the effect of strain localization and the interaction of multiple surface patterns in hard film-soft substrate systems.

High-performance flexible strain sensors based on silver film wrinkles modulated by liquid PDMS substrates.

Flexible strain sensors based on controllable surface microstructures in film-substrate systems can be extensively applied in high-tech fields such as human-machine interfaces, electronic skins, and soft robots. However, the rigid functional films are susceptible to structural destruction and interfacial failure under large strains or high loading speeds, limiting the stability and durability of the sensors. Here we report on a facile technique to prepare high-performance flexible strain sensors based on controllable wrinkles by depositing silver films on liquid polydimethylsiloxane (PDMS) substrates. The silver atoms can penetrate into the surface of liquid PDMS to form an interlocking layer during deposition, enhancing the interfacial adhesion greatly. After deposition, the liquid PDMS is spontaneously solidified to stabilize the film microstructures. The surface patterns are well modulated by changing film thickness, prepolymer-to-crosslinker ratio of liquid PDMS, and strain value. The flexible strain sensors based on the silver film/liquid PDMS system show high sensitivity (above 4000), wide sensing range (∼80%), quick response speed (∼80 ms), and good stability (above 6000 cycles), and have a broad application prospect in the fields of health monitoring and motion tracking.

Tunable Magnetic Domain Patterns in Thickness-Gradient Nickel Films on Flexible PDMS Substrates.

Flexible magnetoelectronic devices (based on magnetic films) have great application prospects in the fields of information storages, bionic robotics, and electronic skins. The intrinsic stress and external loading are very important to modulate the structures and properties of flexible magnetic films due to the magnetoelastic coupling effect. Here, we report on tunable magnetic domain patterns in thickness-gradient nickel (Ni) films deposited on flexible polydimethylsiloxane substrates. It is found that stripe magnetic domains spontaneously form in the Ni films and their sizes increase with the film thickness. The internal stress evolves from tensile to compressive states with decreasing film thickness, leading to the formation of cracks in thicker regions and wrinkles in thinner regions. Meanwhile, the orientations of stripe magnetic domains change from the gradient direction to the orthogonal direction. The structural features, evolution behaviors, and physical mechanisms of the cracks, wrinkles, and magnetic domains are analyzed based on the stress theory and magnetoelastic coupling. Periodic gradient Ni films with large-scale regulations of stripe magnetic domains are also realized by masking of copper grids. This study helps to better understand the magnetoelastic coupling effect in gradient flexible magnetic films and provides a technique to modulate anisotropic magnetic properties by designing specific film systems.

Rate-Dependent Pattern Evolution in Peeling Adhesive Tape Driven by Cohesive Failure.

In the case of low-rate peeling, an adhesive can undergo a large tensile deformation through the viscous flow and form the fingering pattern at the peeling interface, resulting in homogeneous stripes on the peeled surface. In the case of high-rate peeling, no larger viscous deformation occurs, and no surface patterns will be generated. However, it is still unclear how the surface pattern evolves when an adhesive is peeled from a relatively low rate to a high rate. Here, by peeling an adhesive tape at 180° over a wide range of rates, we find that the adhesive tape can undergo a steady peeling. As the peeling rate increases, it is observed that the surface pattern in the peeled adhesive tape tends to evolve from the initial striped pattern to a crescent pattern, then to a spotted pattern. Even in the case of the stick-slip peeling at a small angle, the patterned region also presents the same evolutionary trend. By exploiting a high-speed camera to track the deformation process of the adhesive, it is found that this evolution is actually driven by the cohesive failure of the peeling adhesive. We describe the failure process, revealing the formation mechanism of the crescent pattern. We also discuss the effect of the peeling rate on the interface instability morphology by combining the finite element simulations, elucidating how the surface pattern evolves with the peeling rate.

Controllable Buckle Delaminations in Polymer-Supported Periodic Gradient Films by Mechanical Compression.

Surface instabilities including wrinkles and buckle-delaminations are widespread in nature and can be found in a wide range of practical applications. Compared with the homogeneous wrinkle mode, the buckle-delaminations are spontaneously stress-localized, and their initiation positions and geometrical parameters are hardly precisely controlled by a simple method. Here, we report on the controllable buckle-delaminations in periodic thickness-gradient metal films on polydimethylsiloxane (PDMS) substrates by uniaxial mechanical compression. It is found that a periodic thickness-gradient film is spontaneously formed by masking a copper grid during deposition. The released mechanical strain tends to concentrate in thinner film regions, resulting in the restricted growth of buckle-delaminations. The geometrical features, evolutional behaviors, and underlying physical mechanisms of such buckle-delaminations are analyzed and discussed in detail based on the buckling model and finite element simulations. This work would provide a better understanding of the restricted buckle-delaminations in heterogeneous film-substrate systems and controllable fabrication of ordered structural arrays by copper grid masking and mechanical loading.

Recent progress on crack pattern formation in thin films.

Fascinating pattern formation by quasi-static crack growth in thin films has received increasing interest in both interdisciplinary science and engineering applications. The paper mainly reviews recent experimental and theoretical progress on the morphogenesis and propagation of various quasi-static crack patterns in thin films. Several key factors due to changes in loading types and substrate confinement for choosing crack paths toward different patterns are summarized. Moreover, the effect of crack propagation coupled to other competing or coexisting stress-relaxation processes in thin films, such as interface debonding/delamination and buckling instability, on the formation and transition of crack patterns is discussed. Discussions on the sources and changes in the driving force that determine crack pattern evolution may provide guidelines for the reliability and failure mechanism of thin film structures by cracking and for controllable fabrication of various crack patterns in thin films.

Tailoring Ordered Wrinkle Arrays for Tunable Surface Performances by Template-Modulated Gradient Films.

Complex wrinkled microstructures are ubiquitous in natural systems and living bodies. Although homogeneous wrinkles in film-substrate bilayers have been extensively investigated in the past 2 decades, tailoring heterogeneous wrinkles by a facile method is still a challenge. Here, we report on the controllable heterogeneous wrinkles in template-modulated thickness-gradient metal films sputter-deposited on polydimethylsiloxane substrates. It is found that the stress of the gradient film is strongly position-dependent and the wrinkles are always restricted in thinner film regions. The morphological characteristic and formation mechanism of the heterogeneous wrinkles are analyzed and discussed in detail based on the stress theory. Ordered wrinkle arrays are achieved by adjusting the deposition time, copper grid period, template shape, and lifting height. The surface performances (e.g., the friction property) are well controlled by the wrinkle arrays. This work could promote better understanding of the spontaneously heterogeneous wrinkles in template-modulated gradient films and controllable fabrication of various wrinkle arrays by independently tuning film deposition conditions and template parameters.

Non-Fluorinated Flexible Superhydrophobic Surface with Excellent Mechanical Durability and Self-Cleaning Performance.

Although plenty of superhydrophobic surfaces have been developed owing to their tremendous potential applications, it is still a great challenge for the superhydrophobic surfaces to possess environmental friendliness, biocompatibility, and mechanical durability simultaneously. Herein, a non-fluorinated flexible superhydrophobic surface was designed by constructing a film-substrate system with labyrinth-like wrinkles combining an intrinsically hydrophobic Zn film and a polydimethylsiloxane (PDMS) substrate. Excellent superhydrophobicity with a contact angle up to 168.5° and a slide angle as low as 0° has been achieved on the Zn/PDMS surface, which is attributed to the micro-/nano-textured structures of the labyrinth-like wrinkles, providing sufficient air pockets to form a stable Cassie-Baxter state. Furthermore, the Zn/PDMS surface retains excellent superhydrophobicity under stretching, bending, and twisting mechanical deformation up to 500 cycles due to the stability of the micro-/nano-textured structures of the labyrinth-like wrinkles protected by the fantastic self-healing ability of the micro-cracks. Additionally, the Zn/PDMS superhydrophobic surface possesses an outstanding self-cleaning performance for various contaminants. The present work provides a valuable routine to design non-fluorinated flexible superhydrophobic surfaces with superb mechanical durability and self-cleaning property as promising functional layers for flexible electronics, wearable devices, biomedical engineering, and so forth.

Ordered ring-shaped cracks induced by indentation in metal films on soft elastic substrates.

Ordered crack patterns contain plentiful physical mechanisms and are useful for technological applications such as lithography, template, and biomimicry. Here we report on ordered multiple ring-shaped cracks induced by indentation in metal films on soft elastic polydimethylsiloxane (PDMS) substrates. It is shown that the indentation triggers the deformation of PDMS substrate and generates a radial tensile stress in the film, leading to the formation of ring-shaped cracks with a nearly uniform spacing. The morphological characteristics and evolution behaviors of the multiple ring-shaped cracks are revealed by optical microscopy, atomic force microscopy, and scanning electron microscopy. Their formation mechanisms are discussed by theoretical analysis based on the fracture mechanics. The report in this work can promote better understanding of the indentation-induced stress anisotropy and mode competition in rigid-film-soft-substrate systems and provide a facile strategy to control the crack patterns by simple mechanical loading.

Hierarchical crack patterns of metal films sputter deposited on soft elastic substrates.

Controlled cracks are useful in a wide range of applications, including stretchable electronics, microfluidics, sensors, templates, biomimics, and surface engineering. Here we report on the spontaneous formation of hierarchical crack patterns in metal (nickel) films sputter deposited on soft elastic polydimethylsiloxane (PDMS) substrates. The experiment shows that the nickel film generates a high tensile stress during deposition, which is relieved by the formation of disordered crack networks (called primary cracks). Due to the strong interfacial adhesion and soft substrate, the cracks can penetrate into the PDMS substrate deeply. The width and depth of the primary cracks both increase with increasing film thickness, whereas the crack spacing is insensitive to the film thickness. The film pieces dividing by the primary cracks can fracture further when they are triggered by an external disturbance due to the residual tensile stress, resulting in the formation of fine crack networks (called secondary cracks). The width and spacing of the secondary cracks show different behaviors in comparison to the primary cracks. The morphological characteristics, growth behaviors, and formation mechanisms of the primary and secondary cracking modes have been discussed in detail. The report in this work could provide better understanding of two distinct cracking modes with different sizes and morphologies.

Hierarchical wrinkles and oscillatory cracks in metal films deposited on liquid stripes.

Fascinating crack and wrinkle patterns driven by stresses are ubiquitous in natural and artificial systems. It is of great interest to control the morphologies of stress-driven patterns by using facile techniques. Here we report on the spontaneous formation of hierarchical wrinkles and oscillatory cracks in metal films deposited on liquid (or soft polymer) stripes. It is found that the metal film is under a tensile stress during deposition owing to the thermal expansion of the liquid substrate. As the film thickness is beyond a critical value, oscillatory cracks with sawtoothlike shapes form on the liquid stripes. The ratio of crack oscillation period to amplitude is independent of the stripe width and film material, which can be well explained by the "brittle adhesive joints" model. After deposition, the metal film is under a compressive stress, which is relieved by formation of various wrinkle patterns. Hierarchical wrinkles with changing wavelengths form near the stripe edge while labyrinth or wavy wrinkles form at the center. Energy analysis was adopted to explain the formation and evolution of the wrinkle patterns. This study could promote better understanding of the formations of crack and wrinkle patterns in constrained film structures and controllable fabrication of stress-driven patterns by prefabricating liquid (or soft polymer) interlayer arrays.

Controlled Wrinkling Patterns in Periodic Thickness-Gradient Films on Polydimethylsiloxane Substrates.

Surface wrinkles in homogeneous and heterogeneous film-substrate systems have received intense attention in both science and engineering. Understanding the wrinkling phenomena of heterogeneous systems with continuously variable features is still a challenge. In this work, we propose an unconventional strategy to prepare periodic thickness-gradient metal films on polydimethylsiloxane (PDMS) substrates by masking of copper grids which are weaved by orthometric copper wires. It is found that a periodic thickness-gradient film spontaneously forms during the sputtering process because of the specific structures of the copper grids. Surface wrinkles are strongly modulated by the copper grid structures and are position-dependent within a period. A phase diagram has been established to correlate the wrinkle morphology with the mesh size and film thickness. The film surfaces at mesh centers are evolved from labyrinth wrinkling to herringbone wrinkling and then to stripe wrinkling and finally to wrinkling-free state when the mesh size decreases and/or the film thickness increases. The morphological characteristics, evolutional behaviors, and underlying mechanisms of such wrinkling are discussed in detail based on the stress theory and numerical simulation.

Harnessing fold-to-wrinkle transition and hierarchical wrinkling on soft material surfaces by regulating substrate stiffness and sputtering flux.

Strain-induced complex surface patterns such as wrinkles, folds and hierarchical structures are quite useful in a wide range of practical applications. Although various surface patterns have been extensively investigated, precisely controlling the coexistence and transition of multimodal structures is still a challenge. In this work, we report on a facile technique to harness fold-to-wrinkle transition and hierarchical wrinkling on soft material surfaces by regulating substrate stiffness and sputtering flux. It is found that as the substrate stiffness or sputtering flux increases, the surface patterns successively evolve from networked folds to isolated folds (coexistence of folds and wrinkles) and finally to labyrinth-like wrinkles. For larger sputtering flux, two distinct wrinkling patterns (i.e., G1 wrinkling due to surface instability during sputtering and G2 wrinkling due to thermal compression after deposition) can coexist on the sample surfaces, resulting in the spontaneous formation of hierarchical wrinkles. The report in this work could promote better understanding of the sputtering effect on the spontaneous pattern formation for soft materials and controllable fabrication of multiple complex patterns by simply regulating substrate stiffness and sputtering flux.

The shape of telephone cord blisters.

Formation of telephone cord blisters as a result of buckling delamination is widely observed in many compressed film-substrate systems. Here we report a universal morphological feature of such blisters characterized by their sequential sectional profiles exhibiting a butterfly shape using atomic force microscopy. Two kinds of buckle morphologies, light and heavy telephone cord blisters, are observed and differentiated by measurable geometrical parameters. Based on the Föppl-von Kármán plate theory, the observed three-dimensional features of the telephone cord blister are predicted by the proposed approximate analytical model and simulation. The latter further replicates growth and coalescence of the telephone cord into complex buckling delamination patterns observed in the experiment.

Controlled Formation of Surface Patterns in Metal Films Deposited on Elasticity-Gradient PDMS Substrates.

Controlled surface patterns are useful in a wide range of applications including flexible electronics, elastomeric optics, fluidic channels, surface engineering, measurement technique, biological templates, stamps, and sensors. In this work, we report on the controlled formation of surface patterns in metal films deposited on elasticity-gradient polydimethylsiloxane (PDMS) substrates. Because of the temperature gradient during the curing process, the PDMS substrate in each sample successively changes from a purely liquid state at one side to a purely elastic state at the opposite side. It is found that surface folds appear in the liquid or viscous PDMS region while wrinkles form in the elastic region. In the transition region from the liquid to elastic PDMS, a nested pattern (i.e., the coexisting of folds and wrinkles) can be observed. The folding wave is triggered by the intrinsic stress during the film deposition and its wavelength is independent of the film thickness. The wrinkling wave is induced by the thermal compression after deposition and its wavelength is proportional to the film thickness. The report in this work could promote better understanding of the effect of substrate elasticity on the surface patterns and fabrication of such patterns (folds and wrinkles) by tuning the substrate property.

Wrinkled stripes localized by cracks in metal films deposited on soft substrates.

Homogeneous global wrinkling patterns such as labyrinths, herringbones, ripples and straight stripes can be widely observed in natural and artificial systems, but localized wrinkling patterns (not including buckle-driven delaminations, folds, ridges and creases) are seldom observed in experiments. Here we report on the spontaneous formation of highly ordered wrinkled stripes localized by cracks in metal films deposited on soft substrates. The experiment shows that the metal film is under a large tensile stress during deposition, which is relieved by the formation of networked cracks. After deposition, a compressive stress is stored up in the film and it always focuses near the new formed cracks due to the plastic deformation of the film, resulting in the formation of localized wrinkled stripes composed of a large number of straight wrinkles perpendicular to the cracks. The morphological characteristic, formation mechanism and evolution behaviors of the localized wrinkled stripes have been described and discussed in detail.

Tunable formation of ordered wrinkles in metal films with controlled thickness gradients deposited on soft elastic substrates.

Controlled wrinkled surface is useful for a wide range of applications, including flexible electronics, smart adhesion, wettability, stamping, sensoring, coating, and measuring. In this work, thickness-gradient-guided spontaneous formation of ordered wrinkling patterns in metal films deposited on soft elastic substrates is revealed by atomic force microscopy, theoretic analysis, and simulation. It is observed that in the thicker film region, broad cracks form, and the film surface remains flat. In the thinner film region, the cracks attenuate along the direction of the thickness decrease, and various wrinkle patterns including branched stripes, herringbones, and labyrinths can coexist. The interplay between the residual compression and the thickness gradient leading to the formation of such wrinkling patterns is discussed based on a nonlinear wrinkling model. The simulated wrinkling patterns as well as the variation trends of the wrinkle wavelength and amplitude along the gradient direction are in good agreement with the experimental observations. The report in this work could promote better understanding and fabrication of such ordered wrinkling patterns by tunable thickness gradient.

Spontaneous formation of hierarchical wrinkles in Cr films deposited on silicone oil drops with constrained edges.

We report on the spontaneous formation of hierarchical wrinkling patterns in Cr films deposited on silicone oil drops with constrained edges. The appearance of the wrinkling patterns is strongly dependent on the film thickness and the size of the silicone oil drop. Because the Cr film at the drop edge is constrained due to the strong adhesion between the film and the glass surface, the wrinkle wavelength merely depends on the distance starting from the drop edge. When the distance increases, the wavelength increases quickly first, and then it slows down gradually in compliance with a simple power law. The evolution of the wrinkle amplitude is similar to that of the wavelength, but it is also closely related to the film thickness and the oil drop size. Based on the fact that the silicone oil is polymerized to form an elastic layer during deposition, the formation and evolution of the hierarchical wrinkling patterns have been analyzed in detail.