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1.
Phys Rev E ; 110(2-1): 024602, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-39294950

RESUMEN

In geometrically frustrated assemblies local intersubunit misfits propagate to intra-assembly strain gradients, giving rise to anomalous self-limiting assembly thermodynamics. Here we use theory and coarse-grained simulation to study a recently developed class of "curvamer" particles, flexible shell-like particles that exhibit self-limiting assembly due to the build up of curvature deformation in cohesive stacks. To address a generic, yet poorly understood aspect of frustrated assembly, we introduce a model of curvamer assembly that incorporates both intraparticle shape deformation as well as compliance of interparticle cohesive gaps, an effect we can attribute to a finite range of attraction between particles. We show that the ratio of intraparticle (bending elasticity) to interparticle stiffness not only controls the regimes of self-limitation but also the nature of frustration propagation through curvamer stacks. We find a transition from uniformly bound, curvature-focusing stacks at small size to gap opened, uniformly curved stacks at large size is controlled by a dimensionless measure of inter- versus intracurvamer stiffness. The finite range of interparticle attraction determines the range of cohesion in stacks that are self-limiting, a prediction which is in strong agreement with numerical studies of our coarse-grained colloidal model. These predictions provide critical guidance for experimental realizations of frustrated particle systems designed to exhibit self-limitation at especially large multiparticle scales.

2.
ACS Appl Mater Interfaces ; 16(26): 34079-34088, 2024 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-38889392

RESUMEN

Porous materials have attracted considerable attention due to their versatile applications, especially in water purification. Interconnected nanoporous structures are distinguished by their high degree of porosity and resistance to clogging, as well as their insensitivity to nanostructural orientation. Previous works on randomly linked copolymer systems have shown that they can effectively produce disordered cocontinuous nanostructures, which upon removal of one component yield interconnected nanoporous materials. However, the cocontinuous nanomaterials previously developed using polystyrene (PS) and poly(d,l-lactic acid) (PLA) strands, and the resulting interconnected nanoporous PS monoliths, were far too brittle to enable practical use as membranes. Here, we study the self-assembly of randomly linked copolymer networks prepared using blocks of the engineering polymer polysulfone (PSU). A wide cocontinuous regime (spanning 40 wt %) was found for randomly end-linked copolymer networks (RECNs) constructed from PSU and PLA strands, via a combination of mechanical testing, gravimetry, small-angle X-ray scattering, and scanning electron microscopy. The PSU/PLA cocontinuous nanomaterial with symmetric composition showed 2.4 times higher Young's modulus and ∼100 times greater toughness than the corresponding PS/PLA sample. The interconnected nanoporous PSU fabricated after etching of PLA even exhibited 1.6 times greater toughness than PS/PLA prior to PLA removal. To facilitate the production of thin films of cocontinuous nanomaterials, we applied solution-processable randomly linked linear PSU/PLA multiblock polymers onto ultrafiltration membranes. The interconnected nanoporous PSU thin film generated by etching PLA was found to effectively reject 50 nm diameter particles without significantly compromising permeability. This discovery presents a valuable addition to the existing techniques used to fabricate PSU membranes. In contrast to traditional methods, which are sensitive to processing conditions, produce a wide range of pore sizes, and offer limited adjustability of pore size, the current technique is anticipated to enable interconnected PSU membranes with more uniform and tailorable porosity.

3.
Soft Matter ; 20(8): 1689-1693, 2024 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-38323528

RESUMEN

We demonstrate a system for performing logical operations (OR, AND, and NOT gates) at the air-water interface based on Marangoni optical trapping and repulsion between photothermal particles. We identify a critical separation distance at which the trapped particle assemblies become unstable, providing insight into the potential for scaling to larger arrays of logic elements.

4.
ACS Appl Mater Interfaces ; 16(5): 6394-6402, 2024 Feb 07.
Artículo en Inglés | MEDLINE | ID: mdl-38266384

RESUMEN

Pressure-sensitive adhesives (PSAs) are widely employed in consumer goods, health care, and commercial industry. Anisotropic adhesion of PSAs is often desirable to enable high force capacity coupled with facile release and has typically been realized through the introduction of complex surface and/or bulk microstructures while also maintaining high surface conformability. Although effective, microstructure fabrication can add cost and complexity to adhesive fabrication. Here, we explore aligned liquid crystalline elastomers (LCEs) as directional adhesives. Aligned LCEs exhibit direction-dependent stiffness, dissipation, and nonlinear deformation under load. By varying the cross-link content, we study how the bulk mechanical properties of LCEs correlate to their peel strength and peel anisotropy. We demonstrate up to a 9-fold difference in peel force measured when the LCE is peeled parallel vs perpendicular to the alignment axis. Opportunities to spatially localize adhesion are presented in a monolithic LCE patterned with different director orientations.

5.
ACS Appl Mater Interfaces ; 15(42): 49633-49641, 2023 Oct 25.
Artículo en Inglés | MEDLINE | ID: mdl-37843430

RESUMEN

Cocontinuous polymeric nanostructures have drawn considerable attention due to their ability to combine distinct, percolation-dependent properties of two different polymer domains. Randomly end-linked copolymer networks (RECNs) have previously been shown to support the formation of disordered cocontinuous nanostructures across wide composition windows in a robust way. However, achieving highly efficient linking of telechelic polymers with excellent end-group fidelity often requires complex synthetic routes. As an alternative, we study here statistically cross-linked copolymer networks (SCCNs) composed of polystyrene and poly(2-vinylpyridine) (PS and P2VP) with cross-linkable allyl pendent groups that are conveniently synthesized by controlled radical copolymerization. Via selective extraction of P2VP, coupled with gravimetry, small-angle X-ray scattering, and electron microscopy, we find disordered cocontinuous phases across wide composition ranges (up to ≈ 35 wt %), approaching values previously determined for RECNs. Remarkably, even for samples that appear to exhibit full percolation, a substantial fraction of P2VP (≈ 20-30 wt %) cannot be removed, which we ascribe to short strands between nearby cross-linkers that are physically embedded within PS domains. The resulting PS porous monoliths with residual surface P2VP layers enable facile surface modification to resist protein adsorption and templating of porous gold nanostructures.

6.
Nat Mater ; 22(9): 1152-1159, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37500960

RESUMEN

Photomechanical crystals composed of three-dimensionally ordered and densely packed photochromes hold promise for high-performance photochemical actuators. However, bulk crystals with high structural ordering are severely limited in their flexibility, resulting in poor processibility and a tendency to fragment upon light exposure, while previous nano- or microcrystalline composites have lacked global alignment. Here we demonstrate a photon-fuelled macroscopic actuator consisting of diarylethene microcrystals in a polyethylene terephthalate host matrix. These microcrystals survive large deformations and show a high degree of three-dimensional ordering dictated by the anisotropic polyethylene terephthalate, which critically also has a similar stiffness. Overall, these ordered and compliant composites exhibit rapid response times, sustain a performance of over at least hundreds of cycles and generate work densities exceeding those of single crystals. Our composites represent the state-of-the-art for photochemical actuators and enable properties unattainable by single crystals, such as controllable, reversible and abrupt jumping (photosalient behaviour).

7.
ACS Appl Mater Interfaces ; 15(25): 30956-30963, 2023 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-37315182

RESUMEN

Electroadhesion is the modulation of adhesive forces through electrostatic interactions and has potential applications in a number of next-generation technologies. Recent efforts have focused on using electroadhesion in soft robotics, haptics, and biointerfaces that often involve compliant materials and nonplanar geometries. Current models for electroadhesion provide limited insight on other contributions that are known to influence adhesion performance, such as geometry and material properties. This study presents a fracture mechanics framework for understanding electroadhesion that incorporates geometric and electrostatic contributions for soft electroadhesives. We demonstrate the validity of this model with two material systems that exhibit disparate electroadhesive mechanisms, indicating that this formalism is applicable to a variety of electroadhesives. The results show the importance of material compliance and geometric confinement in enhancing electroadhesive performance and providing structure-property relationships for designing electroadhesive devices.

8.
Soft Matter ; 19(20): 3543-3550, 2023 May 24.
Artículo en Inglés | MEDLINE | ID: mdl-37170825

RESUMEN

In this work, we study the influence of surface tension on light-induced wrinkling of hydrogel disks containing patterned regions of photothermally-active gold nanoparticles at the air-water interface. The disks, which are initially radially stretched by the air-water surface tension, undergo wrinkling under illumination through a radially nonuniform photothermal deswelling. By tuning the surface tension of the surrounding air-water interface through variations in concentration of a poly(vinyl alcohol) surfactant, we observe a critical threshold for wrinkling, followed by a monotonic decrease in wrinkle number with decreasing surface tension. Finite element simulations performed to better understand this behavior reveal qualitatively similar trends as the experiments. The insights provided into elastocapillarity-mediated wrinkling may guide future efforts to control interfacial behaviour of reconfigurable and shape-morphing films.

9.
Angew Chem Int Ed Engl ; 62(1): e202214339, 2023 Jan 02.
Artículo en Inglés | MEDLINE | ID: mdl-36315038

RESUMEN

Aligned liquid crystal polymers are materials of interest for electronic, optic, biological and soft robotic applications. The manufacturing and processing of these materials have been widely explored with mechanical alignment establishing itself as a preferred method due to its ease of use and widespread applicability. However, the fundamental chemistry behind the required two-step polymerization for mechanical alignment has limitations in both fabrication and substrate compatibility. In this work we introduce a new protection-deprotection approach utilizing a two-stage Diels-Alder cyclopentadiene-maleimide step-growth polymerization to enable mild yet efficient, fast, controlled, reproducible and user-friendly polymerizations, broadening the scope of liquid crystal systems. Thorough characterization of the films by DSC, DMA, POM and WAXD show the successful synthesis of a uniaxially aligned liquid crystal network with thermomechanical actuation abilities.

10.
Phys Rev E ; 106(4-1): 044212, 2022 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-36397529

RESUMEN

Mechanical computing has seen resurgent interest recently owing to the potential to embed sensing and computation into new classes of programmable metamaterials. To realize this, however, one must push signals from one part of a device to another and do so in a way that can be reset robustly. We investigate the propagation of signals in a bistable mechanical cascade uphill in energy. By identifying a penetration length for perturbations, we show that signals can propagate uphill for finite distances and map out parameters for this to occur. Experiments on soft elastomers corroborate our results.

11.
Soft Matter ; 18(42): 8098-8105, 2022 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-36263510

RESUMEN

Soft materials interfaces can develop complex morphologies, such as cavities or finger-like features, during separation as a result of a mechanical instability. While the onset and growth of these instabilities have been investigated previously for interfaces between rigid and soft materials, no existing predictive model provides insight for controlling the separation morphology associated with these instabilities when both "sides" of the interface are soft. Here, we expand previous models to account for the geometry and materials properties of two soft materials that form an interface. The total compliance of the system, which depends nonlinearly on the thickness of each contacting soft material, plays a primary role in governing the morphology of the separating interface. We validate this model with experimental measurements using a series of soft elastomers with varying layer thicknesses and fixed materials properties, in order to emphasize the geometry alone can give rise to the observed differences in the interface separation process. This model also demonstrates that the degree of geometric asymmetry, or the ratio of the layer thicknesses that form an interface, influences the stress experienced in either layer, thus providing a rich means of controlling how unstable interface separations develop and propagate. This framework is a powerful tool to understand and control adhesion mechanisms in fields ranging from biology to soft robotics, and provides intuition for engineering a separation mode for a desired end result.

12.
Soft Matter ; 18(34): 6384-6391, 2022 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-35979602

RESUMEN

Self-folding origami, structures that are engineered flat to fold into targeted, three-dimensional shapes, have many potential engineering applications. Though significant effort in recent years has been devoted to designing fold patterns that can achieve a variety of target shapes, recent work has also made clear that many origami structures exhibit multiple folding pathways, with a proliferation of geometric folding pathways as the origami structure becomes complex. The competition between these pathways can lead to structures that are programmed for one shape, yet fold incorrectly. To disentangle the features that lead to misfolding, we introduce a model of self-folding origami that accounts for the finite stretching rigidity of the origami faces and allows the computation of energy landscapes that lead to misfolding. We find that, in addition to the geometrical features of the origami, the finite elasticity of the nearly-flat origami configurations regulates the proliferation of potential misfolded states through a series of saddle-node bifurcations. We apply our model to one of the most common origami motifs, the symmetric "bird's foot," a single vertex with four folds. We show that though even a small error in programmed fold angles induces metastability in rigid origami, elasticity allows one to tune resilience to misfolding. In a more complex design, the "Randlett flapping bird," which has thousands of potential competing states, we further show that the number of actual observed minima is strongly determined by the structure's elasticity. In general, we show that elastic origami with both stiffer folds and less bendable faces self-folds better.


Asunto(s)
Elasticidad
13.
Soft Matter ; 18(21): 4077-4089, 2022 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-35603603

RESUMEN

Formation of desired three-dimensional (3D) shapes from flat thin sheets with programmed non-uniform deformation profiles is an effective strategy to create functional 3D structures. Liquid crystal elastomers (LCEs) are of particular use in programmable shape morphing due to their ability to undergo large, reversible, and anisotropic deformation in response to a stimulus. Here we consider a rectangular monodomain LCE thin sheet divided into one high- and one low-temperature strip, which we dub a 'bistrip'. Upon activation, a discontinuously patterned, anisotropic in-plane stretch profile is generated, and induces buckling of the bistrip into a rolled shape with a transitional bottle neck. Based on the non-Euclidean plate theory, we derive an analytical model to quantitatively capture the formation of the rolled shapes from a flat bistrip with finite thickness by minimizing the total elastic energy involving both stretching and bending energies. Using this analytical model, we identify the critical thickness at which the transition from the unbuckled to buckled configuration occurs. We further study the influence of the anisotropy of the stretch profile on the rolled shapes by first converting prescribed metric tensors with different anisotropy to a unified metric tensor embedded in a bistrip of modified geometry, and then investigating the effect of each parameter in this unified metric tensor on the rolled shapes. Our analysis sheds light on designing shape morphing of LCE thin sheets, and provides quantitative predictions on the 3D shapes that programmed LCE sheets can form upon activation for various applications.

14.
J Am Chem Soc ; 144(12): 5226-5232, 2022 Mar 30.
Artículo en Inglés | MEDLINE | ID: mdl-35285620

RESUMEN

Two-photon polymerization (TPP) currently offers the highest resolution available in 3D printing (∼100 nm) but requires femtosecond laser pulses at very high peak intensity (∼1 TW/cm2). Here, we demonstrate 3D printing based on triplet-triplet-annihilation photopolymerization (TTAP), which achieves submicron resolution while using a continuous visible LED light source with comparatively low light intensity (∼10 W/cm2). TTAP enables submicrometer feature sizes with exposure times of ∼0.1 s/voxel without requiring a coherent or pulsed light source, opening the door to low-cost fabrication with submicron resolution. This approach enables 3D printing of a diverse array of designs with high resolution and is amenable to future parallelization efforts.

15.
Proc Natl Acad Sci U S A ; 119(4)2022 01 25.
Artículo en Inglés | MEDLINE | ID: mdl-35064088

RESUMEN

Sensing technology is under intense development to enable the Internet of everything and everyone in new and useful ways. Here we demonstrate a method of stretchable and self-powered temperature sensing. The basic sensing element consists of three layers: an electrolyte, a dielectric, and an electrode. The electrolyte/dielectric interface accumulates ions, and the dielectric/electrode interface accumulates electrons (in either excess or deficiency). The ions and electrons at the two interfaces are usually not charge-neutral, and this charge imbalance sets up an ionic cloud in the electrolyte. The design functions as a charged temperature-sensitive capacitor. When temperature changes, the ionic cloud changes thickness, and the electrode changes open-circuit voltage. We demonstrate high sensitivity (∼1 mV/K) and fast response (∼10 ms). Such temperature sensors can be made small, stable, and transparent. Depending on the arrangement of the electrolyte, dielectric, and electrode, we develop four designs for the temperature sensor. In addition, the temperature sensor has good linearity in the range of tens of Kelvin. We further show that the temperature sensors can be integrated into stretchable electronics and soft robots.

16.
Adv Mater ; 34(3): e2105758, 2022 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-34741359

RESUMEN

Demands for next-generation soft and responsive materials have sparked recent interest in the development of shape-changing particles and particle assemblies. Over the last two decades, a variety of mechanisms that drive shape change have been explored and integrated into particulate systems. Through a combination of top-down fabrication and bottom-up synthesis techniques, shape-morphing capabilities extend from the microscale to the nanoscale. Consequently, shape-morphing particles are rapidly emerging in a variety of contexts, including photonics, microfluidics, microrobotics, and biomedicine. Herein, the key mechanisms and materials that facilitate shape changes of microscale and nanoscale particles are discussed. Recent progress in the applications made possible by these particles is summarized, and perspectives on their promise and key open challenges in the field are discussed.

17.
Proc Natl Acad Sci U S A ; 118(18)2021 05 04.
Artículo en Inglés | MEDLINE | ID: mdl-33903243

RESUMEN

Cyclic actuation is critical for driving motion and transport in living systems, ranging from oscillatory motion of bacterial flagella to the rhythmic gait of terrestrial animals. These processes often rely on dynamic and responsive networks of oscillators-a regulatory control system that is challenging to replicate in synthetic active matter. Here, we describe a versatile platform of light-driven active particles with interaction geometries that can be reconfigured on demand, enabling the construction of oscillator and spinner networks. We employ optically induced Marangoni trapping of particles confined to an air-water interface and subjected to patterned illumination. Thermal interactions among multiple particles give rise to complex coupled oscillatory and rotational motions, thus opening frontiers in the design of reconfigurable, multiparticle networks exhibiting collective behavior.


Asunto(s)
Bacterias/efectos de la radiación , Fenómenos Fisiológicos Bacterianos/efectos de la radiación , Flagelos/fisiología , Movimiento (Física) , Flagelos/efectos de la radiación , Luz , Pinzas Ópticas , Agua/química
18.
ACS Polym Au ; 1(2): 100-106, 2021 Oct 13.
Artículo en Inglés | MEDLINE | ID: mdl-36855425

RESUMEN

Oppositely charged polymerized ionic liquids (PILs) were used to form complex coacervates in two different organic solvents, 2,2,2-trifluoroethanol (TFE) and hexafluoro-2-propanol (HFIP), and the corresponding phase diagrams were constructed using UV-vis, NMR, and turbidity experiments. While previous studies on complex coacervates have focused almost exclusively on aqueous environments, the use of PILs in the current work enabled studies in solvents with substantially lower dielectric constants (27.0 for TFE, 16.7 for HFIP). The critical salt concentration required to induce complete miscibility was roughly 2-fold larger in HFIP compared with TFE, and two different PIL complexes, solidlike precipitates and liquidlike coacervates, were found in both systems. This study provides insight into the effects of low-dielectric-constant solvents on complex coacervation, which has not been widely studied because of the limited solubility of conventional polyelectrolytes in these media.

19.
ACS Macro Lett ; 9(8): 1172-1177, 2020 Aug 18.
Artículo en Inglés | MEDLINE | ID: mdl-32864191

RESUMEN

Photoinduced shape morphing has implications in fields ranging from soft robotics to biomedical devices. Despite considerable effort in this area, it remains a challenge to design materials that can be both rapidly deployed and reconfigured into multiple different three-dimensional forms, particularly in aqueous environments. In this work, we present a simple method to program and rewrite spatial variations in swelling and, therefore, Gaussian curvature in thin sheets of hydrogels using photoswitchable supramolecular complexation of azobenzene pendent groups with dissolved α-cyclodextrin. We show that the extent of swelling can be programmed via the proportion of azobenzene isomers, with a 60% decrease in areal swelling from the all trans to the predominantly cis state near room temperature. The use of thin gel sheets provides fast response times in the range of a few tens of seconds, while the shape change is persistent in the absence of light thanks to the slow rate of thermal cis-trans isomerization. Finally, we demonstrate that a single gel sheet can be programmed with a first swelling pattern via spatially defined illumination with ultraviolet light, then erased with white light, and finally redeployed with a different swelling pattern.

20.
Adv Mater ; 32(25): e2000600, 2020 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-32419233

RESUMEN

Electroadhesion provides a simple route to rapidly and reversibly control adhesion using applied electric potentials, offering promise for a variety of applications including haptics and robotics. Current electroadhesives, however, suffer from key limitations associated with the use of high operating voltages (>kV) and corresponding failure due to dielectric breakdown. Here, a new type of electroadhesion based on heterojunctions between iono-elastomer of opposite polarity is demonstrated, which can be operated at potentials as low as ≈1 V. The large electric field developed across the molecular-scale ionic double layer (IDL) when the junction is placed under reverse bias allows for strong adhesion at low voltages. In contrast, under forward bias, the electric field across the IDL is destroyed, substantially lowering the adhesion in a reversible fashion. These ionoelastomer electroadhesives are highly efficient with respect to the force capacity per electrostatic capacitive energy and are robust to defects or damage that typically lead to catastrophic failure of conventional dielectric electroadhesives. The findings provide new fundamental insight into low-voltage electroadhesion and broaden its possible applications.

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