An official website of the United States government
Abstract Most elastomers undergo strain‐induced crystallization (SIC) under tension; as individual chains are held rigidly in a fixed position by an applied strain, their alignment along the strain field results in a shift from strain‐hardening (SH) to SIC. A similar degree of stretching is associated with the tension necessary to accelerate mechanically coupled, covalent chemical responses of mechanophores in overstretched chains, raising the possibility of an interplay between the macroscopic response of SIC and the molecular response of mechanophore activation. Here, thiol‐yne‐derived stereoelastomers doped covalently with a dipropiolate‐derivatized spiropyran (SP) mechanophore (0.25–0.38 mol%) are reported. The material properties of SP‐containing films are consistent with undoped controls, indicating that the SP is a reporter of the mechanical state of the polymer. Uniaxial tensile tests reveal correlations between mechanochromism and SIC, which are strain‐rate‐dependent. When mechanochromic films are stretched slowly to the point of mechanophore activation, the covalently tethered mechanophore remains trapped in a force‐activated state, even after the applied stress is removed. Mechanophore reversion kinetics correlate with the applied strain rate, resulting in highly tunable decoloration rates. Because these polymers are not covalently crosslinked, they are recyclable by melt‐pressing into new films, increasing their potential range of strain‐sensing, morphology‐sensing, and shape‐memory applications.
more »
« less
Directed force propagation in semiflexible networks
We consider the propagation of tension along specific filaments of a semiflexible filament network in response to the application of a point force using a combination of numerical simulations and analytic theory. We find the distribution of force within the network is highly heterogeneous, with a small number of fibers supporting a significant fraction of the applied load over distances of multiple mesh sizes surrounding the point of force application. We suggest that these structures may be thought of as tensile force chains, whose structure we explore via simulation. We develop self-consistent calculations of the point-force response function and introduce a transfer matrix approach to explore the decay of tension (into bending) energy and the branching of tensile force chains in the network.
more »
« less
- Award ID(s):
- 1709785
- PAR ID:
- 10220926
- Date Published:
- Journal Name:
- Soft Matter
- ISSN:
- 1744-683X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
null (Ed.)Dynamic networks contain crosslinks that re-associate after disconnecting, imparting them with viscoelastic properties. While continuum approaches have been developed to analyze their mechanical response, these approaches can only describe their evolution in an average sense, omitting local, stochastic mechanisms that are critical to damage initiation or strain localization. To address these limitations, we introduce a discrete numerical model that mesoscopically coarse-grains the individual constituents of a dynamic network to predict its mechanical and topological evolution. Each constituent consists of a set of flexible chains that are permanently cross-linked at one end and contain reversible binding sites at their free ends. We incorporate nonlinear force–extension of individual chains via a Langevin model, slip-bond dissociation through Eyring's model, and spatiotemporally-dependent bond attachment based on scaling theory. Applying incompressible, uniaxial tension to representative volume elements at a range of constant strain rates and network connectivities, we then compare the mechanical response of these networks to that predicted by the transient network theory. Ultimately, we find that the idealized continuum approach remains suitable for networks with high chain concentrations when deformed at low strain rates, yet the mesoscale model proves necessary for the exploration of localized stochastic events, such as variability of the bond kinetics, or the nucleation of micro-cavities that likely conceive damage and fracture.more » « less
-
Abstract Despite plenty of static and dynamic mechanical measurements and modeling for bulk polydimethylsiloxane (PDMS) specimens, a notable gap exists in comprehensively understanding the dynamic mechanics under large cycle, low strain conditions, especially for microscale samples. This study integrates tensile testing and nanoindentation techniques to compare dynamic mechanical response for bulk PDMS samples and μ‐pillars. The results from cyclic tensile testing, which involved up to 10,000 cycles at a strain range of 10%–20%, indicate a stabilization of energy dissipation rate after the initial 25 cycles. This attributes to stress relaxation and strain hardening, validating by rapid dual‐phase exponential decay in maximum stress, coupled with an incremental increase in elastic modulus. In comparison to tensile testing, μ‐pillars exhibited a 0.82% reduction in stiffness, stabilizing ~600th cycle. Concurrently, there was an approximately twofold increase in approaching distance during the initial 120 cycles, and an approximately fourfold increase in dissipated energy over the first 80 cycles, before reaching a plateau. This lagging hysteresis effect attributes to the distribution of the resultant force, including top tension, bottom compression, and base tilt. Overall, this study illuminates temporal mechanical deformations in PDMS under two application scenarios, enhancing our understanding of PDMS mechanical behavior.more » « less
-
Cells are physically contacting with each other. Direct and precise quantification of forces at cell–cell junctions is still challenging. Herein, we have developed a DNA-based ratiometric fluorescent probe, termed DNAMeter, to quantify intercellular tensile forces. These lipid-modified DNAMeters can spontaneously anchor onto live cell membranes. The DNAMeter consists of two self-assembled DNA hairpins of different force tolerance. Once the intercellular tension exceeds the force tolerance to unfold a DNA hairpin, a specific fluorescence signal will be activated, which enables the real-time imaging and quantification of tensile forces. Using E-cadherin-modified DNAMeter as an example, we have demonstrated an approach to quantify, at the molecular level, the magnitude and distribution of E-cadherin tension among epithelial cells. Compatible with readily accessible fluorescence microscopes, these easy-to-use DNA tension probes can be broadly used to quantify mechanotransduction in collective cell behaviors.more » « less
-
Variation in muscular tension has important expressive impacts on agent motion; however, it is difficult to tune simulations to achieve particular effects. With a focus on gesture animation, we introduce mass trackers, a lightweight approach that employs proportional derivative control to track point masses that define the position of each wrist. The restriction to point masses allows the derivation of response functions that support straightforward tuning of system behavior. Using the point mass as an end-effector for an inverse kinematics rig allows easy control of both loose and high tension arm motion. Examples illustrate the expressive variation that can be achieved with this tension modulation. Two perceptual studies confirm that these changes impact the overall level of tension perceived in the motion of a gesturing character and further explore the parameter space. Practical guidelines on tuning are discussed.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/d0sm01177k
