Stability analysis of a liquid crystal elastomer self-oscillator under a linear temperature field

Self-oscillating systems abound in the natural world and offer substantial potential for applications in controllers,micro-motors,medical equipments,and so on.Currently,numerical methods have been widely utilized for obtaining the characteristics of self-oscillation including amplitude and frequency.However,numerical methods are burdened by intricate computations and limited precision,hindering comprehensive investigations into self-oscillating systems.In this paper,the stability of a liquid crystal elastomer fiber self-oscillating system under a linear temperature field is studied,and analytical solutions for the amplitude and frequency are determined.Initially,we establish the governing equations of self-oscillation,elucidate two motion regimes,and reveal the underlying mechanism.Subsequently,we conduct a stability analysis and employ a multi-scale method to obtain the analytical solutions for the amplitude and frequency.The results show agreement between the multi-scale and numerical methods.This research contributes to the examination of diverse self-oscillating systems and advances the theoretical analysis of self-oscillating systems rooted in active materials.

A minimal model for the auxetic response of liquid crystal elastomers

We develop a minimal phenomenological model to describe the auxetic response recently observed in liquid crystal elastomers, and further determine by theoretical calculation the critical condition required for the auxetic response to occur.

Dynamic diselenide bond-enabled liquid crystal elastomer-based two-way shape memory aerogels with weldability and closedloop recyclability

Two-way shape memory polymeric aerogels(2W-SMPAs),with the ability to undergo reversible shape deformation in response to external stimuli,have extensive application in diverse fields such as actuators,sensors,robotics,and other relevant domains.In this study,we introduce a novel approach for fabricating a 2W-SMPA material based on liquid crystal elastomers(LCEs)incorporating dynamic diselenide bonds.The aerogel exhibits liquid crystal phases,excellent compressibility and shape stability,and the mesogens are uniaxial-oriented along the stretching direction.By capitalizing on the dynamic diselenide bonds,the LCEbased aerogel demonstrated remarkable reprogrammability,weldability,and recyclability through thermal reorganization.The shape-programmed aerogel sample exhibits reversible shrinking deformation during the heating and cooling cycles,ultimately achieving a maximum shrinkage ratio of 26.1%.Moreover,the LCE-based aerogel's porous structure and monodomain orientation effectively enable the adsorption of the photothermal dye DR1 and facilitated the reversible photothermal-induced shape deformation when exposed to 520 nm light irradiation.These findings reveal the potential application of this innovative LCE-based aerogel material,enabled by dynamic diselenide bonds,in various areas including control devices,soft actuators,and other diverse fields.

Regulating Actuations and Shapes of Liquid Crystal Elastomers through Combining Dynamic Covalent Bonds with Cooling-Rate-Mediated Control

Realizing multiple locked shapes in pre-oriented liquid crystal elastomers(LCEs)is highly desired for diversifying deformations and enhancing multi-functionality.However,conventional LCEs only deform between two shapes for each actuation cycle upon liquid crystal-isotropic phase transitions induced by external stimuli.Here,we propose to regulate the actuation modes and the locked shapes of a pre-orientated epoxy LCE by combining dynamic covalent bonds with cooling-rate-mediated control.The actuation modes can be adjusted on demand by exchange reactions of dynamic covalent bonds.Derived from the established actuation modes,such as elongation,bending,and spiraling,the epoxy LCE displays varied locked shapes at room temperature under different cooling rates.Various mediums are utilized to control the cooling rate,including water,silicone oil,and copper plates.This approach provides a novel way for regulating the actuation modes and locked shapes of cuttingedge intelligent devices.

Light-triggered fluorochromic cholesteric liquid crystal elastomer with hydrogen-bonded fluorescent switch: dualmodal-switchable circularly polarized luminescence

Solid materials with dynamically tunable circularly polarized luminescence(CPL) feature higher security levels and devicefriendly characteristics, showing great superiority in the field of information technology and anti-counterfeiting. To address the limited photoisomerization of fluorescent photoswitch in CPL-active solid materials, here a cholesteric liquid crystal elastomer(CLCE) containing a hydrogen-bonded(H-bonded) polymerizable fluorescent switch AHBA-PSD is prepared. Owing to the good flexibility and low glass-transition temperature of CLCE, AHBA-PSD shows a fast and fully reversible photocyclization/cycloreversion with fluorochromic behavior in CLCE. Further, by controlling the spectral overlapping area between the emission and reflection bands, the CLCE exhibits a strong CPL with a g_(lum) value of up to 0.76 accompanied by a reversible phototunable CPL signal. Meanwhile, the H-bond helps to stabilize the mechanical property, and the force-induced switching-off of CPL signal could be achieved due to the destroyed helical structures by external force. Finally, an automatically-recognized identification card with abundant chiroptical information is demonstrated.

An ultrahigh fatigue resistant liquid crystal elastomer-based material enabled by liquid metal

The low crosslink density characteristic of liquid crystal elastomer(LCE)materials causes poor fatigue resistance performance,which has seriously plagued their prospects in industrial applications.Here we report that the introduction of 5 wt%liquid metal nanodroplets(average diameter:ca.195 nm)into the LCE network can dramatically reinforce the corresponding composite’s mechanical properties,in particular ultrahigh fatigue resistance,capable of bearing unprecedented 10,000 tensile cycles within a large range of strain amplitude up to 70%and 2000 times of continuous actuating deformations.Furthermore,this liquid metal-incorporated LCE composite material exhibits large actuation stroke(maximum actuation strain:55%),high actuation stress(blocking stress:1.13 MPa),fully reversible thermal/photo-actuation functions,and self-healing ability at moderate temperatures,which qualifies the composite material for high-load actuators.

Liquid crystal elastomer composites for soft actuators

Liquid crystal elastomers are active materials that combine the anisotropic properties of liquid crystals with the elasticity of polymer networks.The LCEs exhibit remarkable reversible contraction and elongation capabilities in response to external stimuli,rendering them highly promising for diverse applications,such as soft robotics,haptic devices,shape morphing structures,etc,However,the predominant reliance on heating as the driving stimulus for LCEs has limited their practical applications.This drawback can be effectively addressed by incorporating fllers,which can generate heat under various stimuli.The recent progress in LCE composites has significantly expanded the application potential of LCEs.In this minireview,we present the design strategies for soft actuators with LCE composites,followed by a detailed exploration of photothermal and electrothermal LCE.composites as prominent examples.Furthermore,we provide an outlook on the challenges and opportunities in the feld of LCE composites.

Large-Size Honeycomb-Shaped and Iris-Like Liquid Crystal Elastomer Actuators

Nature is providing inspiration for researchers to mimic its functions or existing structures,which could remarkably promote the development of new materials.Here,a large-size honeycomb-shaped liquid crystal elastomer(LCE)actuator with LC orientation along the height of the honeycomb shape is built by combining magnetic field alignment and soft lithography technology.This homeotropic alignment allowed the height contraction of honeycomb and pore size expansion of hexagons in a reversible manner upon temperature variation.Therefore,this LCE actuator can be used as a structure for temperature-gated separation of particles.Another example is an iris-like LCE actuator,which has the capability of adjusting its aperture size with a temperature variation.Our approach provides a simple way to design customizable sophisticated LCE actuators for various potential applications.

BIAXIAL LOADING OF NEO-CLASSICAL LIQUID CRYSTAL ELASTOMERS:CONSTITUTIVE RELATIONS AND SOFT BEHAVIOR

The thermo-order-mechanical behaviors of liquid crystal elastomers （LCEs） under biaxial loading are studied in this paper. Inverse method for nonlinear elastic problems is utilized by imposing biaxial stretching to thin rectangular samples. Neo-classical elastic energy is used together with the Landau-de Gennes nematic free energy. Under plane stress assumptions, the constitutive equations are derived. Due to the possible reorientations of the liquid crystal molecules induced by the imposed biaxial loading, the in-plane nonlinear stress-strain relations can have different expressions depending on which loading axis will have the largest effective principal strain. And the free energy is a multi-well non-convex potential function. As shown by some typical loading paths, the LCE samples will exhibit an anisotropic nonlinear elastic behavior, as long as the loading has not induced a reorientation of the liquid crystal molecules. When this did occur, jumps of stresses could take place for dead loadings due to the losing of stability.

Carbon fiber reinforced liquid crystalline elastomer composites:a dual exploration in strength augmentation and transformation flexibility through 4D printing

Liquid Crystal Elastomers(LCEs)are renowned for their reversible deformation capabilities.Yet,enhancing their mechanical strength while retaining such flexibility has posed a considerable challenge.To overcome this,we utilized 4D printing to develop an innovative composite of LCE with carbon fiber fabric(LCEC).This approach has notably increased the tensile strength of LCE by eightfold,all the while maintaining its exceptional capacity for reversible deforma-tion.By adjusting the alignment angle between carbon fiber and the LCE printing direction from 0°to 90°,the LCEC demonstrates an array of new deformation patterns,including bending,twisting,wrapping,and S-shaped transformations,which are distinct from pure LCE materials.Our study unveils that LCE composites exhibit deformation processes markedly different from their pure material counterparts,with the ability of pure LCE to sustain tensile strains exceeding 1900%.These findings,previously undocumented and unexplored,represent a substantial contribution to the field of smart materials.Employing finite element analysis,we explored the carbon fiber and LcE matrix dynamics,revealing bending mechanics in LCECs.This combined experimental and simulation approach yields crucial insights for crafting durable,high-strength LCECs with diverse deformational properties,advancing smart material technology.

Ionic Elastomers for Electric Actuators and Sensors

In the past decades,ion conductive polymers and elastomers have drawn worldwide attention for their advanced functions in batteries,electroactive soft robotics,and sensors.Stretchable ionic elastomers with dispersed soft ionic moieties such as ionic liquids have gained remarkable attention as soft sensors,in applications such as the wearable devices that are often called electric skins.A considerable amount of research has been done on ionic-elastomer-based strain,pressure,and shear sensors;however,to the best of our knowledge,this research has not yet been reviewed.In this review,we summarize the materials and performance properties of engineered ionic elastomer actuators and sensors.First,we review three classes of ionic elastomer actuators—namely,ionic polymer metal composites,ionic conducting polymers,and ionic polymer/carbon nanocomposites—and provide perspectives for future actuators,such as adaptive four-dimensional(4D)printed systems and ionic liquid crystal elastomers(iLCEs).Next,we review the state of the art of ionic elastomeric strain and pressure sensors.We also discuss future wearable strain sensors for biomechanical applications and sports performance tracking.Finally,we present the preliminary results of iLCE sensors based on flexoelectric signals and their amplification by integrating them with organic electrochemical transistors.

Photo Responsive Silver Nanoparticles Incorporated Liquid Crystalline Elastomer Nanocomposites Based on Surface Plasmon Resonance

We reported a nano-Ag/liquid crystalline elastomer（LCE） nanocomposite by incorporating silver nanopar- ticles into a monodomain polysiloxane-based LCE matrix via a novel experimental protocol. The photo-thermo- mechanical actuation of the LCE matrix was realized via the surface plasmon resonance of silver nanoparticles while converting light into heat. The photoresponsive properties of nano-Ag/LCE nanocomposites were investigated with varying ilhunination intensities and silver nanoparticle doping concentrations（0.04% to 0.2%, mass fraction）. The nano-Ag/LCE nanocomposites show sensitive deformation under irradiation due to their excellent photothermal con- version efficiency, and this photostimulated muscle-like actuation is fully reversible via the on-off behavior of light. Incorporating silver nanoparticles into the LCE matrix also improves the mechanical properties and enhances the load-actuation capability of the material.

Thiol-acrylate Catalyst Enabled Post-Synthesis Fabrication of Liquid Crystal Actuators

Synthesizing orientated liquid crystal elastomers(LCEs)via the two-stage thiol-acrylate Michael addition and photopolymerization(TAMAP)reaction is extensively used.However,excess acrylates,initiators,and strong stimuli are inevitably involved in the second stage crosslinking.Herein,we simplify the strategy through taking advantage of a volatile alkaline(originally added to catalyze the thiol-acrylate addition in the first crosslinking stage).Without excess functional groups,the residual catalyst after annealing is still enough to trigger reactions of dynamic covalent bonds at a relatively mild temperature(80℃)to program the alignment of LCEs.The reversible reaction switches off by itself after this process since the catalyst gradually but totally evaporates upon heating.The obtained soft actuators exhibit robust actuation during repeated deformation(over 1000 times).Many shape-morphing modes can be achieved by rationally designing orientation patterns.This strategy not only facilitates the practical synthesis of LCE actuators,but also balances the intrinsic conflict between stability and reprogrammability of exchangeable LCEs.Moreover,the method of applying volatile catalysts has the potential to be extended to other dynamic covalent bonds(DCBs)applied to crosslinked polymer systems.

Intelligent Surfaces Thermally Switchable between the Highly Rough and Entirely Smooth States

Reversible switching from a highly rough surface to another entirely smooth surface under external stimuli is crucial for intelligent materials applied in the fields of an ti-foggi ng,self-clea ning,oil-water separati on and biotech no logy.In this work,a thermal-responsive liquid crystal elastomer(LCE)surface covered with oriented micropillars is prepared via a facile two-step crosslinking method coupled with an extrusion molding program.The reversible change of topological structures of the LCE surface along with temperature is investigated by metallographic microscope,atomic force microscopy and optical con tact angle measuring system.At room temperature,the LCE sample is filled with plenty of micropillars with an average len gth of 8.76 pm,resulting in a super-hydrophobic surface with a water con tact angle(WCA)of 135°.When the temperature is in creased to above the cleari ng point,all the micropillars disappear,the LCE surface becomes entirely flat and presents a hydrophilic state with a WCA of 64°.The roughness-related wetting property of this microstructured LCE surface possesses good recyclability in several heating/cooling cycles.This work realizes a truly reversible transformation from a highly rough surface to an entirely smooth surface,and might promote the potential applications of this dynamic-responsive LCE surface in smart sensors and biomimetic control devices.

Multi-functional stimuli-responsive biomimetic flower assembled from CLCE and MOF-based pedals

Simulating the structures and behaviors of living organisms are of great significance to develop novel multi-functional intelligent devices. However, the development of biomimetic devices with complex deformable structures and synergistic properties is still on the way. Herein, we propose a simple and effective approach to create the multi-functional stimuli-responsive biomimetic devices with independently pre-programmable colorful visual patterns, complex geometries and morphable modes. The metal organic framework(MOF)-based composite film acts as a rigidity actuation substrate to support and mechanically guide the spatial configuration of the soft chiral nematic liquid crystal elastomer(CLCE) sheet. We can directly program the structural color of the CLCE sheet by adjusting the thickness distribution without tedious chemical modification. By using this coordination strategy, we fabricate an artificial flower, which exhibits a synergistic effect of both shape transformation and color change like paeonia ‘Coral Sunset’at different flowering stages, and can even perform different flowering behaviors by bending, twisting and curling petals. The assembled bionic flower is innovatively demonstrated to respond to local stimuli of humidity, heat or ultraviolet irradiation. Therefore, the spatial assembly of CLCE combined with functional MOF materials has a wide range of potential application in multi-functional integrated artificial systems.

Flexible and elastic thermal regulator for multimode intelligent temperature control

As nonlinear thermal devices,thermal regulators can intelligently respond to temperature and control heat flow through changes in heat transfer capacities,which allows them to reduce energy consumption without external intervention.However,current thermal regulators generally based on high-quality crystallinestructure transitions are intrinsically rigid,which may cause structural damage and functional failure under mechanical strain;moreover,they are difficult to integrate into emerging soft electronic platforms.In this study,we develop a flexible,elastic thermal regulator based on the reversible thermally induced deformation of a liquid crystal elastomer/liquid metal(LCE/LM)composite foam.By adjusting the crosslinking densities,the LCE foam exhibits a high actuation strain of 121%with flexibility below the nematic–isotropic phase transition temperature(TNI)and hyperelasticity above TNI.The incorporation of LMresults in a high thermal resistance switching ratio of 3.8 over a wide working temperature window of 60◦C with good cycling stability.This feature originates from the synergistic effect of fragmentation and recombination of the internal LM network and lengthening and shortening of the bond line thickness.Furthermore,we fabricate a“grid window”utilizing photic-thermal integrated thermal control,achieving a superior heat supply of 13.7℃ at a light intensity of 180mW/cm^(2)and a thermal protection of 43.4℃at 1200 mW/cm^(2).The proposed method meets the mechanical softness requirements of thermal regulatormaterials with multimode intelligent temperature control.

Optically controlled elastic microcavities

Whispering gallery mode(WGM)resonators made from dielectrics like glass or polymers have outstanding optical properties like huge cavity quality(Q)factors which can be achieved on scales compatible with on-chip integration.However,tunability of these resonances is typically difficult to achieve or not suitable for robust device applications.We report here on the fabrication of polymeric micro-goblet WGM resonators with an optically controlled and stable reversible tunability over a large spectral range.This tunability is achieved by integration of photo-responsive liquid crystalline elastomers(LCEs)into micro-goblet cavities.The optical response of the elastomer allows reshaping the goblet by employing low pump power,leading to a fully reversible tuning of the modes.The structure can be realistically implemented in on-chip devices,combining the ultra-high Q factors,typical of WGM resonators,with reliable,optical tunability.This result serves as an example of how light can control light,by invoking a physical reshaping of the structure.This way of optical tuning creates interesting possibilities for all-optical control in circuits,enabling interaction between signal and control beams and the realization of self-tuning cavities.