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Force-facilitated rare thermally activated bond rupture enables stress relaxation and hysteresis in hydrogel elastomers 力促进的罕见热激活键断裂使水凝胶弹性体的应力松弛和滞后
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-08 DOI: 10.1016/j.eml.2026.102443
Chih-Jung Lin , Heng-Kwong Tsao , Yu-Jane Sheng
Hydrogel elastomers display stress relaxation, hysteresis, and the Mullins effect even in highly crosslinked networks where chain mobility is strongly suppressed, yet their microscopic origin remains elusive. Although bond rupture has been recognized as a possible contributor, its temporal and spatial occurrence under applied force has not been clearly elucidated. Dissipative particle dynamics simulations with bond-rupture capability reproduce the macroscopic responses, attributed to rare rupture events in tensile strands. Rupture does not result from direct mechanical fracture but from thermal fluctuations that surpass a stress-lowered energy barrier, initiating network reconfiguration that relaxes stress and produces hysteresis. Microscopic variations in mean bond length quantitatively mirror macroscopic stress evolution, ruling out viscoelastic dissipation as the primary mechanism. Our results establish thermally activated bond rupture as the unifying microscopic origin of stress relaxation and hysteresis in hydrogel elastomers, linking microscopic bond dynamics to macroscopic stress responses under cyclic deformations.
水凝胶弹性体即使在链迁移率受到强烈抑制的高度交联网络中也表现出应力松弛、滞后和穆林斯效应,但其微观起源仍然难以捉摸。虽然粘结断裂已被认为是一个可能的因素,但其在施加力作用下的时间和空间发生情况尚未清楚阐明。耗散粒子动力学模拟与键断裂能力再现宏观响应,归因于罕见的断裂事件在拉伸股。破裂不是由直接的机械断裂引起的,而是由超过应力降低的能量势垒的热波动引起的,从而引发网络重构,从而松弛应力并产生滞后。平均键长的微观变化定量地反映了宏观应力演化,排除了粘弹性耗散作为主要机制的可能性。我们的研究结果表明,热激活键断裂是水凝胶弹性体中应力松弛和滞后的统一微观起源,将微观键动力学与循环变形下的宏观应力响应联系起来。
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引用次数: 0
Fatigue threshold of dual-crosslinking hydrogels 双交联水凝胶的疲劳阈值
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2025-12-30 DOI: 10.1016/j.eml.2025.102439
Yijian Zheng, Yang Gao, Tongqing Lu
The fatigue threshold of covalent hydrogels follows the Lake-Thomas model, equating to the energy needed to break covalent bonds between crosslinks at the crack tip. Dynamic bonds are widely introduced as secondary crosslinks to toughen hydrogels. Previous studies have reported that dynamic bonds contribute to the fatigue threshold in some tough hydrogels but not in others, making their contribution unclear. In this work, we prepare dual-crosslinking hydrogels (PAV-M2+) by introducing ligands along covalent polymer chains, enabling dynamic coordination with various M2+ ions to tune the relaxation time. In such hydrogels, we propose that covalent bonds contribute to the fatigue threshold via the Lake-Thomas model, while dynamic bonds contribute based on the competition between relaxation time and the crack-tip strain rate. When the strain rate greatly exceeds the inverse of the relaxation time, dynamic bonds cannot re-associate and contribute little to fatigue threshold. Conversely, when the strain rate is much lower than the inverse of relaxation time, they re-associate reversibly and enhance the threshold. The fatigue threshold of PAV-Ni hydrogels (relaxation time ∼ 300 ms) is 10.5 J/m2 at a strain rate of 1 s−1 (consistent with the Lake-Thomas prediction, 9.4 J/m2), and increases to 17.7 J/m2 at 0.1 s−1. The fatigue threshold of PAV-Zn hydrogels (relaxation time ∼ 0.3 ms) is 39.8 J/m2 at 1 s−1 and 41.4 J/m2 at 0.1 s−1, due to the recovery of dynamic bonds during loading cycles. Based on these results, we propose a modified Lake-Thomas model that incorporates the contribution of dynamic bonds to fatigue threshold, capturing the competition between relaxation time and strain rate.
共价水凝胶的疲劳阈值遵循Lake-Thomas模型,等于断裂裂纹尖端交联共价键所需的能量。动态键作为二级交联被广泛引入以增强水凝胶。先前的研究已经报道了动态键对某些坚韧水凝胶的疲劳阈值有贡献,但对其他水凝胶没有贡献,这使得它们的贡献尚不清楚。在这项工作中,我们通过在共价聚合物链上引入配体来制备双交联水凝胶(PAV-M2+),使其能够与各种M2+离子动态配位来调节弛豫时间。在这种水凝胶中,我们提出共价键通过Lake-Thomas模型贡献疲劳阈值,而动态键基于松弛时间和裂纹尖端应变率之间的竞争贡献疲劳阈值。当应变速率大大超过松弛时间的倒数时,动态键不能重新结合,对疲劳阈值的贡献很小。相反,当应变速率远低于松弛时间的倒数时,它们会可逆地重新关联并提高阈值。当应变速率为1 s−1时,PAV-Ni水凝胶的疲劳阈值(松弛时间~ 300 ms)为10.5 J/m2(与Lake-Thomas预测一致,为9.4 J/m2),当应变速率为0.1 s−1时,疲劳阈值增加到17.7 J/m2。由于加载过程中动态键的恢复,PAV-Zn水凝胶的疲劳阈值(松弛时间~ 0.3 ms)在1 s−1时为39.8 J/m2,在0.1 s−1时为41.4 J/m2。基于这些结果,我们提出了一个改进的Lake-Thomas模型,该模型包含了动态键对疲劳阈值的贡献,捕捉了松弛时间和应变速率之间的竞争。
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引用次数: 0
Front Cover CO1 封面CO1
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-03-02 DOI: 10.1016/S2352-4316(26)00024-6
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引用次数: 0
A rediscovery of stiff pentmodes. A comment on “High bulk modulus pentamodes: the three-dimensional metal water'' 硬五模态的再发现。对“高体积模量五模体:三维金属水”的评析
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-10 DOI: 10.1016/j.eml.2026.102444
Graeme W. Milton
We bring attention to the fact that the claim of Brambilla et.al. [1] of discovering a novel design for pentamode materials is incorrect. Back in 2016 Briane Harutyunyan and myself [2] designed a class of stiff pentamodes, that include the high bulk modulus pentamodes of Brambilla et.al. Our design generalized to three-dimensions, and to full anisotropy, the main aspects of a two-dimensional construction of Sigmund [3]. It is emphasized that the in depth analysis of Brambilla et.al. goes well beyond our brief treatment.
我们提请注意这样一个事实,即Brambilla等人的主张。发现五模材料新设计的想法是不正确的。早在2016年,Briane Harutyunyan和我自己就设计了一类刚性五模体,其中包括Brambilla等人的高体积模量五模体。我们的设计推广到三维和全各向异性,Sigmund[3]的二维结构的主要方面。强调对Brambilla等人的深入分析。远远超出了我们简短的讨论。
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引用次数: 0
Stabilizing the buckling instabilities of soft cylindrical shell grippers 软圆柱壳夹持器屈曲失稳的稳定研究
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-02 DOI: 10.1016/j.eml.2025.102437
Wenjie Li , Yu Herng Tan , Zhong Wang , Xuguang Dong , Huichan Zhao
Soft cylindrical shell grippers consist of a rigid outer shell and a soft inner layer that inflates inward under internal pressure. This inflatable ring actuator mechanism enables the gripper to conform to and stably grasp objects, offering unique advantages in handling irregular shapes and compliant materials, and making these grippers promising candidates for soft robotic manipulation. However, upon inflation, their soft inner walls often undergo a sequence of buckling instabilities—from wrinkling to creasing and more complex post-buckling behaviors. Due to the stochastic nature of these buckling instabilities, the resulting deformation patterns—such as the number, positions, and deflections of creases—vary unpredictably, leading to inconsistencies in gripper performance. This study investigates the factors governing the buckling instabilities of soft cylindrical shell grippers and proposes strategies for their stabilization. Through theoretical analysis and finite element (FE) simulations, we establish the relationship between geometric parameters and the predicted buckling instabilities. To control the instability morphology, we introduce evenly distributed geometric imperfections and implement a material training process to mitigate non-uniform deformation by leveraging the Mullins effect. We demonstrate that these combined strategies significantly improve grasping performance, including increased contact area, enhanced self-centering, and improved repeatability. Finally, we validate the gripper’s effectiveness in real-world scenarios through on-arm pick-and-place experiments. This work provides a framework for designing soft cylindrical shell grippers with greater reliability, while maintaining simplicity in fabrication.
软圆柱壳夹持器由坚硬的外壳和在内部压力下向内膨胀的软内层组成。这种充气环致动机构使夹持器符合并稳定地抓取物体,在处理不规则形状和柔性材料方面具有独特的优势,并使这些夹持器成为软机器人操作的有希望的候选者。然而,膨胀后,它们柔软的内壁往往经历一系列的屈曲不稳定——从起皱到折痕以及更复杂的后屈曲行为。由于这些屈曲不稳定性的随机性,所产生的变形模式(如折痕的数量、位置和挠度)不可预测地变化,导致夹持器性能不一致。本文研究了软壳夹持器屈曲失稳的影响因素,并提出了其稳定策略。通过理论分析和有限元模拟,建立了几何参数与预测屈曲失稳之间的关系。为了控制不稳定形态,我们引入均匀分布的几何缺陷,并实施材料训练过程,以利用穆林斯效应来减轻不均匀变形。我们证明了这些组合策略显着提高抓取性能,包括增加接触面积,增强自定心和提高可重复性。最后,我们通过手臂拾取和放置实验验证了抓手在现实场景中的有效性。这项工作为设计具有更高可靠性的软圆柱壳夹持器提供了框架,同时保持了制造的简单性。
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引用次数: 0
Anomalous thermomechanical actuation of liquid crystal elastomer balloons 液晶弹性体气球的异常热机械驱动
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-14 DOI: 10.1016/j.eml.2026.102448
Zumrat Usmanova, Ruobing Bai
Elastomeric balloons are widely studied in various soft actuation systems owing to their simplicity and versatility. Recently, balloons made of liquid crystal elastomers (LCEs) stand out with their unconventional, thermal-responsive inflation behaviors due to the intrinsic coupling between directionally ordered liquid crystal mesogens and stretchable polymer networks, offering an attractive way for fast, large, reversible, and stimuli-responsive actuation. However, this thermomechanical coupling, together with their resultant actuation and instability in LCE balloons, remains poorly understood. Here we show the anomalous thermomechanical actuation of a spherical LCE balloon by solving a boundary-value problem based on the well-established quasi-convex elastic energy for polydomain LCE. We modify the elastic energy to ensure its consistency with the classical model by Bladon, Warner, and Terentjev based on freely jointed chains. We predict the thermally modulated pressure-volume response of the LCE balloon, where the peak pressure for snap-through instability depends non-monotonically on temperature. This nonmonotonic dependence originates from the competing temperature-dependent effects of the mesogen order and the network elasticity, which also govern the modulus of the LCE in the nematic phase. Finally, by extending the free energy to a Gent-like model, we quantify the detailed temperature-dependent snap-through behavior, compare multiple performance metrics of spherical and cylindrical balloons, and analyze an envisioned thermally modulated fluid pump across a wide range of operating temperatures.
弹性体气球由于其简单和通用性,在各种软驱动系统中得到了广泛的研究。最近,由液晶弹性体(LCEs)制成的气球因其非常规的热响应膨胀行为而脱颖而出,这是由于定向有序液晶介元与可拉伸聚合物网络之间的内在耦合,为快速、大型、可逆和刺激响应驱动提供了一种有吸引力的方法。然而,这种热-机械耦合,以及它们在LCE气球中的致动性和不稳定性,仍然知之甚少。本文基于已建立的多域LCE准凸弹性能,通过求解边值问题,展示了球形LCE气球的反常热力驱动。我们修改了弹性能,使其与Bladon、Warner和Terentjev基于自由关节链的经典模型保持一致。我们预测了LCE气球的热调制压力-体积响应,其中瞬时穿过不稳定性的峰值压力非单调地依赖于温度。这种非单调依赖源于中介质序和网络弹性的温度依赖效应,这也决定了LCE在向列相的模量。最后,通过将自由能扩展到类似根特的模型,我们量化了详细的温度相关的snap-through行为,比较了球形和圆柱形气球的多个性能指标,并分析了在广泛的工作温度范围内设想的热调制流体泵。
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引用次数: 0
Effects of electrolyte infiltration on the cracking of active materials in lithium-ion batteries 电解液浸润对锂离子电池活性物质开裂的影响
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-21 DOI: 10.1016/j.eml.2026.102452
Yisen Peng , Feng Hao
The cracking of electrode active materials causes capacity fade that is one of the bottlenecks in high-performance battery design. Electrolyte infiltrates surface cracks, increasing electrochemically active area and offering fast pathways for lithium-ion insertion/extraction, while interior cracks hinder lithium-ion diffusion within active materials. However, the theoretical model is still lacking to differentiate electrolyte infiltration into surface crack and interior crack. Herein, a chemo-mechanical phase field model coupling the modified smoothed boundary method (SBM) is established to investigate the effect of electrolyte infiltration on chemo-mechanical responses. Within a unified framework, the proposed model captures the coupled processes of electrolyte infiltration and crack growth by distinguishing between interior and surface cracks and tracking the electrolyte-active material interface. It is found that surface cracks infiltrated by electrolyte enhance the accumulation of lithium ions and stress concentration at the crack tip, which further accelerates fracture propagation. The freshly exposed crack surfaces in turn enable more electrochemical reaction sites and improve rate capability, although the cracks destroy the mechanical integrity of active materials. The voltage jump could be induced by coalescence of surface and interior cracks, accompanying by electrolyte penetration. The proposed model provides insights into the complex interaction of electrolyte infiltration, lithium-ion diffusion, stress evolution, and fracture propagation.
电极活性材料的开裂引起的容量衰减是高性能电池设计的瓶颈之一。电解质渗入表面裂纹,增加了电化学活性面积,为锂离子的插入/提取提供了快速途径,而内部裂纹阻碍了锂离子在活性材料中的扩散。然而,目前还缺乏区分电解液渗入表面裂纹和渗入内部裂纹的理论模型。为此,建立了一种耦合改进光滑边界法(SBM)的化学-力学相场模型,研究了电解质浸润对化学-力学响应的影响。在统一的框架内,该模型通过区分内部和表面裂纹以及跟踪电解质-活性材料界面来捕获电解质渗透和裂纹扩展的耦合过程。研究发现,电解液对表面裂纹的渗透增强了裂纹尖端锂离子的积累和应力集中,进一步加速了裂纹的扩展。尽管裂纹破坏了活性材料的机械完整性,但新暴露的裂纹表面反过来又能产生更多的电化学反应位点并提高反应速率。电压跳变是由表面裂纹和内部裂纹合并引起的,同时伴随着电解液的渗透。该模型提供了电解质渗透、锂离子扩散、应力演化和断裂扩展的复杂相互作用的见解。
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引用次数: 0
Revealing surface tension in elastic membranes via indentation 通过压痕揭示弹性膜的表面张力
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-04 DOI: 10.1016/j.eml.2026.102455
Wanying Zheng , Zhida Gao , Chuanli Yu , Jun Yin , Zhaohe Dai
When an elastic membrane is deformed, the external work is stored not only as volume-related elastic strain energy but also as area-related surface energies, since the total membrane area changes. The latter contribution is challenging to quantify experimentally, especially for ultrathin membranes. Here, we demonstrate that such surface effects can be revealed through indentation by comparing tests performed at gas and liquid interfaces. Specifically, using monolayer graphene indented across N2–graphene and water–graphene interfaces, we show that graphene indented against water appears significantly softer—a signature of interfacial energetics favoring the water–graphene configuration. A membrane theory incorporating both elasticity and surface forces quantitatively reproduces the measured force–displacement curves, enabling the extraction of the interfacial tension difference and, in turn, membrane’s wettability. These results establish indentation as a probe of solid–liquid surface tension at the membrane limit and highlight that surface effects – often regarded as negligible in 2D materials – must be carefully accounted for in applications ranging from straintronics to nanofluidics.
当弹性膜发生变形时,由于总膜面积的变化,外功不仅以与体积相关的弹性应变能的形式存储,而且以与面积相关的表面能的形式存储。后者的贡献是具有挑战性的量化实验,特别是对超薄膜。在这里,我们证明了这种表面效应可以通过压痕通过比较在气体和液体界面进行的测试来揭示。具体来说,通过在n2 -石墨烯和水-石墨烯界面上使用单层石墨烯,我们发现石墨烯在水的作用下表现得明显更柔软——这是有利于水-石墨烯结构的界面能量学特征。结合弹性和表面力的膜理论定量地再现了测量的力-位移曲线,从而可以提取界面张力差,进而提取膜的润湿性。这些结果确立了压痕作为膜极限下固液表面张力的探针,并强调了表面效应——在二维材料中通常被认为可以忽略不计——必须在从应变电子学到纳米流体的应用中仔细考虑。
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引用次数: 0
Multistable mechanical metamaterials with compatible sensitive actuation and high stability 具有兼容敏感驱动和高稳定性的多稳态机械超材料
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-15 DOI: 10.1016/j.eml.2026.102450
Xiangyu Guo , Yuanming Xu , Nan Zhu , Hang Xu
Multistable mechanical metamaterials (MMMs) program shape reconfigurations through snap-through transitions between multiple stable states in response to environmental stimuli, such as changes in mechanical load, temperature, or magnetic field. One major unresolved challenge is the trade-off resulting from the inherent coupling between the critical actuation load and the multistability. MMMs that require high actuation loads to snap through exhibit strong mechanical stability but are difficult to trigger and cannot respond to small-amplitude environmental stimuli. In contrast, those that can snap through under low loads become highly susceptible to disturbances and may fail to maintain multistability. This study introduces a tri-beam bistable building block to decouple critical actuation load and structural multistability. The constructed MMMs are capable of programming strain energy barriers into their layouts to achieve multistability under arbitrary actuation loads, even low to near-zero. The mechanical properties and deformation mechanisms of MMMs are investigated via a combination of numerical simulation, analytical modeling, and experimental validation. The proposed heterogeneous discrete assembly strategy integrates rigid and flexible components into MMM unit cells, enabling support-free additive manufacturing of reconfigurable one-directional, planar, and spatial MMMs with near-isotropic mechanical behavior. The developed MMMs exhibit post-manufacturing re-programmable deformation, high compactability, and multi-directional stability.
多稳态机械超材料(MMMs)通过响应环境刺激(如机械负荷、温度或磁场的变化)在多个稳定状态之间的瞬时转换来编程形状重新配置。一个尚未解决的主要挑战是临界驱动负载和多稳定性之间固有耦合的权衡。需要高驱动负载才能通过的mm具有很强的机械稳定性,但难以触发,并且不能响应小幅度的环境刺激。相比之下,那些可以在低负载下快速通过的电路变得非常容易受到干扰,并且可能无法保持多稳定性。本研究引入了一种三梁双稳构件来解耦临界驱动载荷和结构的多重稳定性。所构建的mm能够在其布局中编程应变能屏障,以实现任意驱动载荷下的多稳定性,甚至低至接近零。通过数值模拟、分析建模和实验验证相结合的方法研究了mm材料的力学性能和变形机理。提出的异构离散装配策略将刚性和柔性组件集成到MMM单元格中,使具有近各向同性力学行为的可重构单向、平面和空间mm的无支撑增材制造成为可能。开发的mm具有制造后可重新编程变形,高紧凑性和多向稳定性。
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引用次数: 0
Conditional diffusion modeling for constructing geometrical connectivity in multiscale metamaterial system 构造多尺度超材料系统几何连通性的条件扩散建模
IF 4.5 3区 工程技术 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-10 DOI: 10.1016/j.eml.2026.102446
Hao Wu , Chen Yu , Chuang Liu , HengAn Wu
Designing multiscale metamaterial systems necessitates the creation of microstructures with compatible boundaries to achieve desired elastic properties induced by topological optimization. However, fulfilling these multiple target requirements remains a significant challenge when designing microstructures with compatible boundaries. To address these issues, we propose a data-driven framework leveraging a conditional diffusion model for the inverse design of microstructures with specific elastic properties and geometrical boundary constraints. Utilizing a large dataset of microstructures generated via topological optimization, our generative model accurately produces diverse geometrical designs for target elastic properties, providing a broad design space for boundary compatibility. The model's accuracy in designing microstructures surpasses that of previous studies. We comprehensively study the relationships between elastic properties and varying ranges of geometrical boundary shapes. Moreover, by incorporating boundary constraints during generation, the proposed BoundaryDiff method ensures mechanical consistency from microscale units to macroscale assemblies. Numerical experiments show that stitched structures generated by our model maintain homogenized elastic properties in close agreement with theoretical predictions, effectively addressing incompatibilities between adjacent microstructures. A numerical case demonstrates the feasibility of our approach in designing multiscale metamaterial systems. This study bridges the gap between microstructure design and topological optimization, holding significant promise for designing functional multiscale metamaterial systems.
设计多尺度超材料系统需要创建具有兼容边界的微结构,以实现由拓扑优化引起的所需弹性性能。然而,在设计具有兼容边界的微结构时,满足这些多目标需求仍然是一个重大挑战。为了解决这些问题,我们提出了一个数据驱动的框架,利用条件扩散模型来逆设计具有特定弹性特性和几何边界约束的微结构。利用通过拓扑优化生成的大型微结构数据集,我们的生成模型精确地生成目标弹性特性的各种几何设计,为边界兼容性提供了广阔的设计空间。该模型在微观结构设计方面的精度超过了以往的研究。我们全面研究了弹性特性与几何边界形状变化范围之间的关系。此外,通过在生成过程中引入边界约束,所提出的BoundaryDiff方法确保了从微观单元到宏观尺度组件的力学一致性。数值实验表明,该模型生成的缝合结构保持了均匀的弹性特性,与理论预测非常吻合,有效地解决了相邻微观结构之间的不相容问题。数值算例验证了该方法在设计多尺度超材料系统中的可行性。该研究弥合了微观结构设计和拓扑优化之间的差距,为设计功能多尺度超材料系统带来了重大希望。
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引用次数: 0
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Extreme Mechanics Letters
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