Snap-through of graphene nanowrinkles under out-of-plane compression.

Nanowrinkles (i.e. the buckled nanoribbons) are widely observed in nano-devices assembled by two-dimensional (2D) materials. The existence of nanowrinkles significantly affects the physical (such as mechanical, electrical and thermal) properties of 2D materials, and thus further, impedes the applications of those devices. In this paper, we take the nanowrinkle formed in a monolayer graphene as a model system to study its deformation behaviours, especially the configuration evolution and the snap-through buckling instabilities, when subjected to the out-of-plane compression. By performing molecular dynamics simulation, the graphene nanowrinkles with or without self-adhesion (which are notated as 'clipped' state or 'bump' state, respectively) are obtained depending on the geometric size and the applied axial compressive pre-strain. The elastica theory is employed to quantify the shape of 'bump' nanowrinkles, as well as the critical condition of the transition between 'clipped' and 'bump' states. By applying out-of-plane compression to the generated graphene nanowrinkle, it flips to an opposite configuration via snap-through buckling. We identify four different buckling modes according to the configuration evolution. An unified phase diagram is constructed to describe those buckling modes. For the cases with negligible van der Waals interaction getting involved in the snap-buckling process, i.e. without self-adhesion, the force-displacement curves for nanowrinkles with same axial pre-strain but different sizes can be scaled to collapse. Moreover, the critical buckling loads can also be scaled and predicted by the extended elastica theory. Otherwise, for the cases with self-adhesion, which corresponds to the greater axial pre-strain, the van der Waals interaction makes the scaling collapse break down. It is expected that the analysis about the snap-through buckling of graphene nanowrinkles reported in this work will advance the understanding of the mechanical behaviours of wrinkled 2D materials and promote the design of functional nanodevices, such as nanomechanical resonators and capacitors.

Stretchable Superhydrophobicity from Monolithic, Three-Dimensional Hierarchical Wrinkles.

We report the design of three-dimensional (3D) hierarchical wrinkle substrates that can maintain their superhydrophobicity even after being repeatedly stretched. Monolithic poly(dimethysiloxane) with multiscale features showed wetting properties characteristic of static superhydrophobicity with water contact angles (>160°) and very low contact angle hysteresis (<5°). To examine how superhydrophobicity was maintained as the substrate was stretched, we investigated the dynamic wetting behavior of bouncing and splashing upon droplet impact with the surface. On hierarchical wrinkles consisting of three different length scales, superhydrophobic bouncing was observed. The substrate remained superhydrophobic up to 100% stretching with no structural defects after 1000 cycles of stretching and releasing. Stretchable superhydrophobicity was possible because of the monolithic nature of the hierarchical wrinkles as well as partial preservation of nanoscale structures under stretching.

Controlled Three-Dimensional Hierarchical Structuring by Memory-Based, Sequential Wrinkling.

This paper describes how a memory-based, sequential wrinkling process can transform flat polystyrene sheets into multiscale, three-dimensional hierarchical textures. Multiple cycles of plasma-mediated skin growth followed by directional strain relief of the substrate resulted in hierarchical architectures with characteristic generational (G) features. Independent control over wrinkle wavelength and wrinkle orientation for each G was achieved by tuning plasma treatment time and strain-relief direction for each cycle. Lotus-type superhydrophobicity was demonstrated on three-dimensional G1-G2-G3 hierarchical wrinkles as well as tunable superhydrophilicity on these same substrates after oxygen plasma. This materials system provides a general approach for nanomanufacturing based on bottom-up sequential wrinkling that will benefit a diverse range of applications and especially those that require large area (>cm(2)), multiscale, three-dimensional patterns.

Controlling the orientation of nanowrinkles and nanofolds by patterning strain in a thin skin layer on a polymer substrate.

We describe herein how to control the orientation of polymer nanowrinkles and nanofolds with large amplitudes. Nanowrinkles were created by chemically treating thermoplastic polystyrene sheets to form a thin skin layer and then heating the substrate to relieve strain. By manipulating the strain globally and locally in the skin layer, we could tune whether wrinkles or folds formed, as well as the distances over which these structures could be produced. This unique materials system provided access to high strain regimes, which enabled mechanisms behind the spontaneous formation of complex structures to be explored.

Enhanced Room Temperature Ferromagnetism in Highly Strained 2D Semiconductor Cr2Ge2Te6.

Emergent magnetism in van der Waals materials offers exciting opportunities in fabricating atomically thin spintronic devices. One pertinent obstacle has been the low transition temperatures (Tc) inherent to these materials, precluding room temperature applications. Here, we show that large structural gradients found in highly strained nanoscale wrinkles in Cr2Ge2Te6 (CGT) lead to significant increases of Tc. Magnetic force microscopy was utilized in characterizing multiple strained CGT nanostructures leading to experimental evidence of elevated Tc, depending on the strain percentage estimated from finite element analysis. Our findings are further supported by ab initio and DFT studies of the strained material, which indicates that strain directly augments the ferromagnetic coupling between Cr atoms in CGT, influenced by superexchange interaction; this provides strong insight into the mechanism of the enhanced magnetism and Tc.

Area-Specific, Hierarchical Nanowrinkling of Two-Dimensional Materials.

This paper describes an approach to generate hierarchical wrinkles in two-dimensional (2D) electronic materials with spatial control over adjacent wavelengths. A rigid fluoropolymer mold was used to pattern a sacrificial polymer skin layer on monolayer graphene, molybdenum disulfide, and hexagonal boron nitride on prestrained thermoplastic sheets. Strain relief and removal of the polymer layer resulted in 2D-material wrinkles whose wavelengths scaled linearly with the local skin thickness. A second generation of wrinkles could be created on top of the first generation by applying a subsequent cycle of polymer skin coating, strain relief, and polymer removal. This area-specific hierarchical wrinkling is general and will facilitate the engineering of the local properties of various 2D materials and their heterostructures.

Multifunctional Polymer Memory via Bi-Interfacial Topography for Pressure Perception Recognition.

Emerging memory devices, that can provide programmable information recording with tunable resistive switching under external stimuli, hold great potential for applications in data storage, logic circuits, and artificial synapses. Realization of multifunctional manipulation within individual memory devices is particularly important in the More-than-Moore era, yet remains a challenge. Here, both rewritable and nonerasable memory are demonstrated in a single stimuli-responsive polymer diode, based on a nanohole-nanowrinkle bi-interfacial structure. Such synergic nanostructure is constructed from interfacing a nanowrinkled bottom graphene electrode and top polymer matrix with nanoholes; and it can be easily prepared by spin coating, which is a low-cost and high-yield production method. Furthermore, the resulting device, with ternary and low-power operation under varied external stimuli, can enable both reversible and irreversible biomimetic pressure recognition memories using a device-to-system framework. This work offers both a general guideline to fabricate multifunctional memory devices via interfacial nanostructure engineering and a smart information storage basis for future artificial intelligence.

A Combinational Effect of "Bulk" and "Surface" Shape-Memory Transitions on the Regulation of Cell Alignment.

A novel shape-memory cell culture platform has been designed that is capable of simultaneously tuning surface topography and dimensionality to manipulate cell alignment. By crosslinking poly(ε-caprolactone) (PCL) macromonomers of precisely designed nanoarchitectures, a shape-memory PCL with switching temperature near body temperature is successfully prepared. The temporary strain-fixed PCLs are prepared by processing through heating, stretching, and cooling about the switching temperature. Temporary nanowrinkles are also formed spontaneously during the strain-fixing process with magnitudes that are dependent on the applied strain. The surface features completely transform from wrinkled to smooth upon shape-memory activation over a narrow temperature range. Shape-memory activation also triggers dimensional deformation in an initial fixed strain-dependent manner. A dynamic cell-orienting study demonstrates that surface topographical changes play a dominant role in cell alignment for samples with lower fixed strain, while dimensional changes play a dominant role in cell alignment for samples with higher fixed strain. The proposed shape-memory cell culture platform will become a powerful tool to investigate the effects of spatiotemporally presented mechanostructural stimuli on cell fate.