Atomic insights into thickness-dependent deformation mechanism and mechanical properties of Ag/PMMA ultra-thin nanofilms.

In this work, the nanoindentations on bilayer composite nanofilms composed of metal Ag and polymer PMMA were simulated using molecular dynamics. The effects of the thickness of Ag and PMMA on the elastic moduli of the composite films were analyzed from Hertz contact theory, dislocation evolution and atomic migration. The results show that the maximum penetration depth that the Hertz model could well describe is about 6 Å, and this limiting value is almost independent on the film thickness. The deformation mode of the Ag films gradually changes from bending mode to indentation mode with an increase in Ag thickness, which improves the elastic modulus of the composite films. The rule of mixtures could give a theoretical prediction about the elastic modulus of the composite film close to the nanoindentation, and Hertz theory could also be used as long as the thickness of Ag films exceeded a certain value. The introduction of a PMMA layer impedes the development of dislocation in the Ag layer and improves the elastic limit of the composite films. This work provides an important basis for experimentally measuring the overall elastic modulus of metal/polymer composite film based on nanoindentation or extracting the elastic modulus of metal film from the overall indentation response of the composite film.

Surface Polymerization and Controlled Pyrolysis: Tailorable Synthesis of Bumpy Hollow Carbon Spheres for Energy Storage.

Architectural design of hollow carbon spheres (HCSs) plays a vital role in improving their performance and expanding applications. The tailorable synthesis of bumpy or asymmetric HCSs with a refined structure remains a challenge. Herein, bumpy HCSs (BHCSs) and bumpy concave HCSs (BCHCSs) have been engineered. The synthesis involves the formation of a core/shell precursor via the surface polymerization of pyrrole monomers on polystyrene nanoparticles, followed by the controlled pyrolysis process under different conditions. In comparison with HCSs, the concave hollow structure can reduce the excessive interior cavity and maintain prevalent merits of hollow structures; the bumpy shell can improve the surface area and number of active sites, thus improving the kinetics as energy storage devices. As a result, among BCHCSs, BHCSs, and HCSs, BCHCSs exhibit optimal electrochemical performance. The lithium-ion hybrid capacitors employing BCHCSs as an anode can deliver an energy density of 0.2182 kW h kg-1 at a power density of 0.2235 kW kg-1. Overall, this study provides an innovative design and strategy for constructing unique carbon nano-architectures for energy storage.

Earthworm-Inspired Ultradurable Superhydrophobic Fabrics from Adaptive Wrinkled Skin.

Wrapped by periodically wrinkled skin, soft earthworm shows excellent robustness against sticky soil. Mimicking this deformation adaptability, here, we report an ultradurable superhydrophobic fabric by exploiting the formation of adaptive, soft wrinkled poly(dimethylsiloxane) (PDMS) skins. Uniform wrinkles are created on woven fabric fibers due to the surface instability of PDMS coating with a cross-linking gradient induced by Ar plasma treatment. Both the surface topography of wrinkles and the viscoelasticity of the underlying compliant layer to release stress endow the treated superhydrophobic fabrics with extraordinary durability, withstanding 800 standard laundries or 1000 rubbing cycles under 44.8 kPa. Additionally, superhydrophobic fabrics are self-healable after heating or plasma treatment. This insight of engineering soft skins with periodic submicron surface topography and gradient modulus provides a pathway for the design of ultradurable, multifunctional wearables.

Buckled Amorphous Hollow Carbon Spheres: Facile Fabrication, Buckling Process, and Applications as Electrode Materials for Supercapacitors.

Buckled hollow carbon nanospheres (BHCSs) integrate several attractive properties desired for a variety of potential applications. However, the development of a feasible and simple method for preparing BHCS nanoparticles remains a great challenge. Herein, we present a facile strategy for fabricating monodisperse BHCSs via the compression of intact hollow carbon nanospheres (HCSs) with improved mechanical strength. The essence of our strategy lies in the successful preparation of robust HCSs that can sustain large mechanical deformation during compression, based on the introduction of polyvinylpyrrolidone in the synthesis of HCS templates. Both experiments and finite element analyses are conducted to probe the deformation mechanism of buckling, suggesting that the residual stress introduced by pyrolysis of precursors plays a predominant role in the buckling process. Furthermore, the use of BHCSs as high-performance supercapacitors is demonstrated. Our work provides important insights into the engineering of robust amorphous carbon nanomaterials by the template method and mechanical modulation and provides an innovative synthetic strategy for fabricating asymmetric hollow spheres with potential for a diversity of applications.

Highly efficient fog harvesting on superhydrophobic microfibers through droplet oscillation and sweeping.

Water droplet transport on fibers is of great importance for achieving high water collection efficiency from fog. Here, we exploit a new droplet sliding mechanism to accelerate the droplet coalescence and collection for highly efficient fog harvesting by coating hydrophilic microfibers with superhydrophobic layers of assembled carbon nanoparticles. We find that during the initial water collection, unlike the pinned droplets having axisymmetric barrel shapes wrapped around uncoated microfibers, the hanging droplets on coated microfibers with non-wrapping clamshell shapes are highly mobile due to their lower contact hysteresis adhesion; these are observed to oscillate, coalesce, and sweep the growing droplets along the horizontally placed microfibers. The driving force for droplet transport is mainly ascribed to the coalescence energy release and fog flow. After introducing small gravity force by tilting coated microfibers with a small angle of 5°, we find that it can effectively drive the oscillating mobile droplets for directional transport by rapidly sweeping the droplets with a much higher frequency. Finally, the water collection rate from fog on uncoated microfibers over a prolonged duration is found to be improved over 2 times after superhydrophobic coating, and it is further enhanced over 5 times after a small tilting angle of 5°.

Switchable Adhesion Actuator for Amphibious Climbing Soft Robot.

Climbing soft robots are of tremendous interest in both science and engineering due to their potential applications in intelligent surveillance, inspection, maintenance, and detection under environments away from the ground. The challenge lies in the design of a fast, robust, switchable adhesion actuator to easily attach and detach the vertical surfaces. Here, we propose a new design of pneumatic-actuated bioinspired soft adhesion actuator working both on ground and under water. It is composed of extremely soft bilayer structures with an embedded spiral pneumatic channel resting on top of a base layer with a cavity. Rather than the traditional way of directly pumping air out of the cavity for suction in hard polymer-based adhesion actuator, we inflate air into the top spiral channel to deform into a stable 3D dome shape for achieving negative pressure in the cavity. The characterization of the maximum shear adhesion force of the proposed soft adhesion actuator shows strong and rapid reversible adhesion on multiple types of smooth and semi-smooth surfaces. Based on the switchable adhesion actuator, we design and fabricate a novel load-carrying amphibious climbing soft robot (ACSR) by combining with a soft bending actuator. We demonstrate that it can operate on a wide range of foreign horizontal and vertical surfaces including dry, wet, slippery, smooth, and semi-smooth ones on ground and also under water with certain load-carrying capability. We show that the vertical climbing speed can reach about 286 mm/min (1.6 body length/min) while carrying over 200 g object (over 5 times the weight of ACSR itself) during climbing on ground and under water. This research could largely push the boundaries of soft robot capabilities and multifunctionality in window cleaning and underwater inspection under harsh environment.

Small degree of anisotropic wetting on self-similar hierarchical wrinkled surfaces.

We studied the wetting behavior of multiscale self-similar hierarchical wrinkled surfaces. The hierarchical surface was fabricated on poly(dimethylsiloxane) (PDMS) substrates by manipulating the sequential strain release and combined plasma/ultraviolet ozone (UVO) treatment. The generated structured surface shows an independently controlled dual-scale roughness with level-1 small-wavelength wrinkles (wavelength of 700-1500 nm and amplitude of 50-500 nm) resting on level-2 large-wavelength wrinkles (wavelength of 15-35 µm and amplitude of 3.5-5 µm), as well as accompanying orthogonal cracks. By tuning the aspect ratio of hierarchical wrinkles, the degree of wetting anisotropy in hierarchical wrinkled surfaces, defined as the contact angle difference between the parallel and perpendicular directions to the wrinkle grooves, is found to change between 3° and 9°. Through both experimental characterization (confocal fluorescence imaging) and theoretical analyses, we showed that the wetting state in the hierarchical wrinkled surface is in the Wenzel wetting state. We found that the measured apparent contact angle is larger than the theoretically predicted Wenzel contact angle, which is found to be attributed to the three-phase contact line pinning effect of both wrinkles and cracks that generates energetic barriers during the contact line motion. This is evidenced by the observed sudden drop of over 20° in the static contact angles along both perpendicular and parallel directions after slight vibration perturbation. Finally, we concluded that the observed small degree of wetting anisotropy in the hierarchical wrinkled surfaces mainly arises from the competition between orthogonal wrinkles and cracks in the contact line pinning.

Spontaneous Periodic Delamination of Thin Films To Form Crack-Free Metal and Silicon Ribbons with High Stretchability.

Design of electronic materials with high stretchability is of great importance for realizing soft and conformal electronics. One strategy of realizing stretchable metals and semiconductors is to exploit the buckling of materials bonded to elastomers. However, the level of stretchability is often limited by the cracking and fragmentation of the materials that occurs when constrained buckling occurs while bonded to the substrate. Here, we exploit a failure mechanism, spontaneous buckling-driven periodic delamination, to achieve high stretchability in metal and silicon films that are deposited on prestrained elastomer substrates. We find that both globally periodic buckle-delaminated pattern and ordered cracking patterns over large areas are observed in the spontaneously buckle-delaminated thin films. The geometry of periodic delaminated buckles and cracking periodicity can be predicted by theoretical models. By patterning the films into ribbons with widths smaller than the predicted cracking periodicity, we demonstrate the design of crack-free and spontaneous delaminated ribbons on highly prestrained elastomer substrates, which provides a high stretchability of about 120% and 400% in Si and Au ribbons, respectively. We find that the high stretchability is mainly attributed to the largely relaxed strain in the ribbons via spontaneous buckling-driven delamination, as made evident by the small maximum tensile strain in both ribbons, which is measured to be over 100 times smaller than that of the substrate prestrain.

Cuts Guided Deterministic Buckling in Arrays of Soft Parallel Plates for Multifunctionality.

Harnessing buckling instability in soft materials offers an effective strategy to achieve multifunctionality. Despite great efforts in controlling the wrinkling behaviors of film-based systems and buckling of periodic structures, the benefits of classical plate buckling in soft materials remain largely unexplored. The challenge lies in the intrinsic indeterminate characteristics of buckling, leading to geometric frustration and random orientations. Here, we report the controllable global order in constrained buckling of arrays of parallel plates made of hydrogels and elastomers on rigid substrates. By introducing patterned cuts on the plates, the randomly phase-shifted buckling in the array of parallel plates transits to a prescribed and ordered buckling with controllable phases. The design principle for cut-directed deterministic buckling in plates is validated by both mechanics model and finite element simulation. By controlling the contacts and interactions between the buckled parallel plates, we demonstrate on-demand reconfigurable electrical and optical pathways, and the potential application in design of mechanical logic gates. By varying the local stimulus within the plates, we demonstrate that microscopic pathways can be written, visualized, erased, and rewritten macroscopically into a completely new one for potential applications such as soft reconfigurable circuits and logic devices.

Self-similar Hierarchical Wrinkles as a Potential Multifunctional Smart Window with Simultaneously Tunable Transparency, Structural Color, and Droplet Transport.

Smart window has immense potential for energy savings in architectural and vehicular applications, while most studies focus on the tunability of a single property of optical transmittance. Here we explore harnessing dynamically tunable hierarchical wrinkles for design of a potential multifunctional smart window with combined structural color and water droplet transport control. The self-similar hierarchical wrinkles with both nanoscale and microscale features are generated on a prestrained poly(dimethylsiloxane) elastomer through sequential strain release and multistep oxygen plasma treatment. We show that the hierarchically wrinkled elastomer displays both opaqueness and iridescent structural color. We find that restretching/releasing the elastomer leads to the reversible and repeatable switch from opaqueness to transparency, arising from the flattening of large wrinkles (micrometer scale), while a nonvanishing structural color occurs due to the nondisappearing small wrinkles (nanoscale). The unique features of combined reversible large wrinkles and irreversible small wrinkles during hierarchical wrinkling are well reproduced by corresponding finite element simulation. The criteria for generating self-similar hierarchical wrinkles is revealed through a simplified theoretical model and validated by experiments. In addition to its tunable optical property, we further show its ability in control of water droplet transport on demand through mechanical stretching and release. We find that an initially pinned water droplet on the tilted hierarchically wrinkled surface starts to slide when the surface is stretched, and becomes pinned again upon strain release. Such a process is reversible and repeatable. The hierarchically wrinkled surface could find broad potential applications not only in multifunctional smart windows with additional features of aesthetics and water collection, but in microfluidics, design of slippery surfaces, and directional water transportation.

Programmable Kiri-Kirigami Metamaterials.

Programmable kirigami metamaterials with controllable local tilting orientations on demand through prescribed notches are constructed through a new approach of kiri-kirgami, and their actuation of pore opening via both mechanical stretching and temperature, along with their potential application as skins for energy-saving buildings, is discussed.

Design of Hierarchically Cut Hinges for Highly Stretchable and Reconfigurable Metamaterials with Enhanced Strength.

Applying hierarchical cuts to thin sheets of elastomer generates super-stretchable and reconfigurable metamaterials, exhibiting highly nonlinear stress-strain behaviors and tunable phononic bandgaps. The cut concept fails on brittle thin sheets due to severe stress concentration in the rotating hinges. By engineering the local hinge shapes and global hierarchical structure, cut-based reconfigurable metamaterials with largely enhanced strength are realized.