Search for: All records

Synthetic replication of the precise mesoscale control found in natural systems poses substantial experimental challenges due to the need for manipulation across multiple length scales (from nano- to millimeter). 

Soft bioelectronic devices exhibit motion-adaptive properties for neural interfaces to investigate complex neural circuits. Here, we develop a fabrication approach through the control of metamorphic polymers’ amorphous-crystalline transition to miniaturize and integrate multiple components into hydrogel bioelectronics. We attain an about 80% diameter reduction in chemically cross-linked polyvinyl alcohol hydrogel fibers in a fully hydrated state. This strategy allows regulation of hydrogel properties, including refractive index (1.37-1.40 at 480 nm), light transmission (>96%), stretchability (139-169%), bending stiffness (4.6 ± 1.4 N/m), and elastic modulus (2.8-9.3 MPa). To exploit the applications, we apply step-index hydrogel optical probes in the mouse ventral tegmental area, coupled with fiber photometry recordings and social behavioral assays. Additionally, we fabricate carbon nanotubes-PVA hydrogel microelectrodes by incorporating conductive nanomaterials in hydrogel for spontaneous neural activities recording. We enable simultaneous optogenetic stimulation and electrophysiological recordings of light-triggered neural activities in Channelrhodopsin-2 transgenic mice. 

Abstract Filamentous bundles are ubiquitous in Nature, achieving highly adaptive functions and structural integrity from assembly of diverse mesoscale supramolecular elements. Engineering routes to synthetic, topologically integrated analogs demands precisely coordinated control of multiple filaments’ shapes and positions, a major challenge when performed without complex machinery or labor-intensive processing. Here, we demonstrate a photocreasing design that encodes local curvature and twist into mesoscale polymer filaments, enabling their programmed transformation into target 3-dimensional geometries. Importantly, patterned photocreasing of filament arrays drives autonomous spinning to form linked filament bundles that are highly entangled and structurally robust. In individual filaments, photocreases unlock paths to arbitrary, 3-dimensional curves in space. Collectively, photocrease-mediated bundling establishes a transformative paradigm enabling smart, self-assembled mesostructures that mimic performance-differentiating structures in Nature (e.g., tendon and muscle fiber) and the macro-engineered world (e.g., rope). 

Through a combined approach of experiment and simulation, this study quantifies the role of entanglements in determining the mechanical properties of glassy polymer blends. Uniaxial extension experiments on 100-nm films containing a bidisperse mixture of polystyrene enable quantitative comparison with molecular dynamics (MD) simulations of a coarse-grained model for polymer glasses, where the bidisperse blends allow us to systematically tune the entanglement density of both systems. In the MD simulations, we demonstrate that not all entanglements carry substantial load at large deformation, and our analysis allows the development of a model to describe the number of effective, load-bearing entanglements per chain as a function of blend ratio. The film strength measured experimentally and the simulated film toughness are quantitatively described by a model that only accounts for load-bearing entanglements. 

Abstract Cavitation has long been recognized as a crucial predictor, or precursor, to the ultimate failure of various materials, ranging from ductile metals to soft and biological materials. Traditionally, cavitation in solids is defined as an unstable expansion of a void or a defect within a material. The critical applied load needed to trigger this instability -- the critical pressure -- is a lengthscale independent material property and has been predicted by numerous theoretical studies for a breadth of constitutive models. While these studies usually assume that cavitation initiates from defects in the bulk of an otherwise homogeneous medium, an alternative and potentially more ubiquitous scenario can occur if the defects are found at interfaces between two distinct media within the body. Such interfaces are becoming increasingly common in modern materials with the use of multimaterial composites and layer-by-layer additive manufacturing methods. However, a criterion to determine the threshold for interfacial failure, in analogy to the bulk cavitation limit, has yet to be reported. In this work, we fill this gap. Our theoretical model captures a lengthscale independent limit for interfacial cavitation, and is shown to agree with our observations at two distinct lengthscales, via two different experimental systems. To further understand the competition between the two cavitation modes (bulk versus interface), we expand our investigation beyond the elastic response to understand the ensuing unstable propagation of delamination at the interface. A phase diagram summarizes these results, showing regimes in which interfacial failure becomes the dominant mechanism.