Flexible pressure sensors with a high sensitivity over a broad linear range can simplify wearable sensing systems without additional signal processing for the linear output, enabling device miniaturization and low power consumption. Here, we demonstrate a flexible ferroelectric sensor with ultrahigh pressure sensitivity and linear response over an exceptionally broad pressure range based on the material and structural design of ferroelectric composites with a multilayer interlocked microdome geometry. Due to the stress concentration between interlocked microdome arrays and increased contact area in the multilayer design, the flexible ferroelectric sensors could perceive static/dynamic pressure with high sensitivity (47.7 kPa, 1.3 Pa minimum detection). In addition, efficient stress distribution between stacked multilayers enables linear sensing over exceptionally broad pressure range (0.0013-353 kPa) with fast response time (20 ms) and high reliability over 5000 repetitive cycles even at an extremely high pressure of 272 kPa. Our sensor can be used to monitor diverse stimuli from a low to a high pressure range including weak gas flow, acoustic sound, wrist pulse pressure, respiration, and foot pressure with a single device.

We present detailed results about the structural, conformational, rheo-optical, and topological properties of an entangled of C 400 H 802 linear polyethylene (PE) melt over a wide range of shear rates (covering both the linear and the highly nonlinear viscoelastic regimes) from direct nonequilibrium molecular dynamics (NEMD) simulations of a large system containing 192 chains (corresponding to 79200 interacting atomistic units). We discuss results for (i) the probability distribution of the mean-square chain end-to-end distance and its radius of gyration, (ii) the conformation tensor, (iii) the material functions in steady shear (viscosity, normal stress differences, nonequilibrium shear compliance, hydrostatic pressure), (iv) the flow birefringence, (v) the orientation angle and order parameter, (vi) the interaction energies and their relative importance, (vii) the intermolecular pair distribution function, and (viii) the intrinsic molecular shape of the chains (represented by the isosurface plots in terms of their monomer number density), all as a function of flow strength. A detailed primitive path (PP) analysis has allowed us to examine how the flow field alters the statistical properties of the underlying topological network of the melt (probability distribution functions and mean values of PP contour length, of the number and size of entanglement strands, etc.). Our results reveal significant distortions of all these distributions due to applied flow. One of the most important results of our work is that as the shear rate is increased, the average value of the contour length goes through a maximum and the number of entanglements per chain exhibits a shear-thinning behavior which bears many similarities with the corresponding behavior of the shear viscosity. Overall, most of the computed rheological properties of the C 400 H 802 melt change in a nonlinear way with the applied shear rate due to the simultaneous effect of (a) chain orientation and stretching, (b) chain rotation and tumbling under shear, and (c) chain disentanglement.

The gradient stiffness between stiff epidermis and soft dermis with interlocked microridge structures in human skin induces effective stress transmission to underlying mechanoreceptors for enhanced tactile sensing. Inspired by skin structure and function, we fabricate hierarchical nanoporous and interlocked microridge structured polymers with gradient stiffness for spacer-free, ultrathin, and highly sensitive triboelectric sensors (TESs). The skin-inspired hierarchical polymers with gradient elastic modulus enhance the compressibility and contact areal differences due to effective transmission of the external stress from stiff to soft layers, resulting in highly sensitive TESs capable of detecting human vital signs and voice. In addition, the microridges in the interlocked polymers provide an effective variation of gap distance between interlocked layers without using the bulk spacer and thus facilitate the ultrathin and flexible design of TESs that could be worn on the body and detect a variety of pressing, bending, and twisting motions even in humid and underwater environments. Our TESs exhibit the highest power density (46.7 μW/cm), pressure (0.55 V/kPa), and bending (∼0.1 V/°) sensitivities ever reported on flexible TESs. The proposed design of hierarchical polymer architectures for the flexible and wearable TESs can find numerous applications in next-generation wearable electronics.

Atomistic configurations of model unentangled ring polyethylene (PE) melts ranging in chain length from C 24 up to C 400 have been subjected to detailed molecular dynamics (MD) simulations in the isothermal-isobaric statistical ensemble at temperature T = 450 K and P = 1 atm. Strictly monodisperse samples were employed in all cases. We present and discuss in detail simulation results for a variety of structural, thermodynamic, conformational and dynamic properties of these systems, and their variation with chain length. Among others, these include the mean chain radius of gyration, the pair correlation function, the intrinsic molecular shape, the local dynamics, the segmental mean square displacement (msd), the chain center-of-mass self-diffusion coefficient D G , the chain terminal relaxation time τ d , the characteristic spectrum of the Rouse relaxation times τ p , and the dynamic structure factor S(q,t). In all cases, the results are compared against the corresponding data from simulations with linear PE melts of the same chain length (the linear analogues) and the predictions of the Rouse theory for polymer rings which we derive here in its entirety. The Rouse theory is found to provide a satisfactory description of the simulation findings, especially for rings with chain length between C 50 and C 170 . An important finding of our work (from the observed dependence of D G , τ p , ζ, and η 0 on chain length N) is that PE ring melts follow approximately Rouse-like dynamics even when their chain length is as long as C 400 ; this is more than twice the characteristic crossover chain length (∼C 156 ) marking the passage from Rouse to reptation dynamics for the corresponding linear PE melts. In a second step, and by mapping the simulation data onto the Rouse model, we have managed to extract the friction coefficient ζ and the zero-shear rate viscosity η 0 of the simulated ring melts. Overall, and in agreement with previous theoretical and experimental studies, our simulation results support that the structure of ring polymers in the melt is more compact than that of their linear analogues due to their nonconcatenated configurations. Additional results for the intermolecular mer-mer and center-of-mass pair correlation functions confirm that the effective correlation hole effect is more pronounced in melts of rings than in melts of linear chains.

Articles you may be interested inTemperature dependent micro-rheology of a glass-forming polymer melt studied by molecular dynamics simulation J. Chem. Phys. 141, 124907 (2014) The topological state of entangled polymers has been analyzed recently in terms of primitive paths which allowed obtaining reliable predictions of the static ͑statistical͒ properties of the underlying entanglement network for a number of polymer melts. Through a systematic methodology that first maps atomistic molecular dynamics ͑MD͒ trajectories onto time trajectories of primitive chains and then documents primitive chain motion in terms of a curvilinear diffusion in a tubelike region around the coarse-grained chain contour, we are extending these static approaches here even further by computing the most fundamental function of the reptation theory, namely, the probability ͑s , t͒ that a segment s of the primitive chain remains inside the initial tube after time t, accounting directly for contour length fluctuations and constraint release. The effective diameter of the tube is independently evaluated by observing tube constraints either on atomistic displacements or on the displacement of primitive chain segments orthogonal to the initial primitive path. Having computed the tube diameter, the tube itself around each primitive path is constructed by visiting each entanglement strand along the primitive path one after the other and approximating it by the space of a small cylinder having the same axis as the entanglement strand itself and a diameter equal to the estimated effective tube diameter. Reptation of the primitive chain longitudinally inside the effective constraining tube as well as local transverse fluctuations of the chain driven mainly from constraint release and regeneration mechanisms are evident in the simulation results; the latter causes parts of the chains to venture outside their average tube surface for certain periods of time. The computed ͑s , t͒ curves account directly for both of these phenomena, as well as for contour length fluctuations, since all of them are automatically captured in the atomistic simulations. Linear viscoelastic properties such as the zero shear rate viscosity and the spectra of storage and loss moduli obtained on the basis of the obtained ͑s , t͒ curves for three different polymer melts ͑polyethylene, cis-1,4-polybutadiene, and trans-1,4-polybutadiene͒ are consistent with experimental rheological data and in qualitative agreement with the double reptation and dual constraint models. The new methodology is general and can be routinely applied to analyze primitive path dynamics and chain reptation in atomistic trajectories ͑accumulated through long MD simulations͒ of other model polymers or polymeric systems ͑e.g., bidisperse, branched, grafted, etc.͒; it is thus believed to be particularly useful in the future in evaluating proposed tube models and developing more accurate theories for entangled systems.

Biological tissues are multi-responsive and functional, and similar properties might be possible in synthetic systems by merging responsive polymers with hierarchical soft architectures. For example, mechanochromic polymers have applications in force-responsive colourimetric sensors and soft

Hierarchical and gradient structures in biological systems with special mechanical properties have inspired innovations in materials design for construction and mechanical applications. Analogous to the control of stress transfer in gradient mechanical structures, the control of electron transfer in gradient electrical structures should enable the development of high-performance electronics. This paper demonstrates a high performance electronic skin (e-skin) via the simultaneous control of tactile stress transfer to an active sensing area and the corresponding electrical current through the gradient structures. The flexible e-skin sensor has extraordinarily high piezoresistive sensitivity at low power and linearity over a broad pressure range based on the conductivity-gradient multilayer on the stiffness-gradient interlocked microdome geometry. While stiffness-gradient interlocked microdome structures allow the efficient transfer and localization of applied stress to the sensing area, the multilayered structure with gradient conductivity enables the efficient regulation of piezoresistance in response to applied pressure by gradual activation of current pathways from outer to inner layers, resulting in a pressure sensitivity of 3.8 × 10 5 kPa −1 with linear response over a wide range of up to 100 kPa. In addition, the sensor indicated a rapid response time of 0.016 ms, a low minimum detectable pressure level of 0.025 Pa, a low operating voltage (100 μV), and high durability during 8000 repetitive cycles of pressure application (80 kPa). The high performance of the e-skin sensor enables acoustic wave detection, differentiation of gas characterized by different densities, subtle tactile manipulation of objects, and real-time monitoring of pulse pressure waveform.

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