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Nonlinear elasticity and transition to macroscopic irreversibility in composite hydrogels. 复合水凝胶的非线性弹性和向宏观不可逆性的转变。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-19 DOI: 10.1039/d5sm00990a
Ippolyti Dellatolas, Thibaut Divoux, Emanuela Del Gado, Irmgard Bischofberger

Filler-hydrogel composites combine enhanced mechanical properties with functionalities conferred by the nanofillers. When the nanofillers interact attractively with the hydrogel matrix, even low nanofiller volume fractions can lead to a strong increase in the linear viscoelastic moduli. Here, we build on our understanding of the microscopic phenomena at play in these systems to explore their nonlinear response, using attractive nanofillers embedded in a gelatin matrix. We identify a critical deformation beyond which the material no longer recovers its macroscopic viscoelastic properties, marking the onset of macroscopic irreversibility. Increasing nanofiller volume fraction leads to nanofiller-induced stiffening of the polymer matrix, yet the overall viscoelastic response of the composites remains qualitatively similar to that of pure hydrogels: under increasing strain amplitude, their elastic and viscous moduli, G' and G″, exhibit a pronounced overshoot followed by a crossover associated with yielding. A transition occurs in the composite at the strain amplitude where G' reaches its maximum, characterized by a marked change in the stress relaxation dynamics. Beyond , the composites no longer recover their initial viscoelastic properties in repeated strain amplitude sweeps, indicating that the material has sustained macroscopically irreversible changes and a permanent loss of elasticity. We thus identify three distinct regimes in the strain-stiffening materials: nonlinear elasticity, macroscopic irreversibility, and yielding. We further suggest that the plasticity underpinning macroscopic irreversibility is due to the breaking of bonds that contribute most to the composite's strain stiffening response in the hydrogel matrix.

填料-水凝胶复合材料结合了纳米填料增强的机械性能和功能。当纳米填料与水凝胶基质相互作用时,即使纳米填料的体积分数很低,也会导致线性粘弹性模量的大幅增加。在这里,我们建立在我们对这些系统中起作用的微观现象的理解的基础上,利用嵌入在明胶基质中的有吸引力的纳米填料来探索它们的非线性响应。我们确定了一个临界变形,超过该变形,材料不再恢复其宏观粘弹性特性,标志着宏观不可逆性的开始。增加纳米填充剂体积分数会导致聚合物基体的变硬,但复合材料的整体粘弹性响应在性质上仍与纯水凝胶相似:在应变幅度增加的情况下,它们的弹性和粘性模量G'和G″表现出明显的超调,随后出现与屈服相关的交叉。复合材料在应变幅值G′达到最大值处发生转变,表现为应力松弛动力学的显著变化。此外,复合材料在反复的应变振幅扫描中不再恢复其初始的粘弹性特性,这表明材料已经发生了持续的宏观不可逆变化,并且永久性地失去了弹性。因此,我们在应变增强材料中确定了三种不同的机制:非线性弹性,宏观不可逆性和屈服。我们进一步提出,支撑宏观不可逆性的可塑性是由于在水凝胶基质中对复合材料应变硬化响应贡献最大的键的断裂。
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引用次数: 0
The effect of humidity, temperature, and drying duration on microparticle detachment force: insights into capillary-induced deformation at the particle-substrate interface. 湿度、温度和干燥时间对微粒脱离力的影响:微粒-衬底界面毛细管诱导变形的见解。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-19 DOI: 10.1039/d5sm01109d
Javad Sherafatpour, Anna Ipatova, Alexis Duchesne, H N Yoshikawa, Pascal Mariot, Christine Faille, Ichiro Ueno, Georg F Dietze, Farzam Zoueshtiagh

We experimentally investigate how drying history influences microparticle-substrate adhesion in hydrophilic systems. By systematically varying air temperature, relative humidity, and drying duration under controlled conditions, we quantify the detachment force of individual microparticles. Air temperature emerges as the dominant factor: higher temperatures and lower humidity enhance adhesion, while prolonged drying generally reduces it, except under combined high-temperature and low-humidity conditions, where strong adhesion persists. Complementary scanning electron microscopy (SEM) results reveal drying-time-dependent changes in the particle-substrate contact size, consistent with capillary-induced compression of the contact zone followed by partial relaxation. These findings indicate that transient capillary stresses during evaporation deform the particle-substrate interface and leave a lasting imprint on adhesion strength. Overall, the study shows how capillarity, drying dynamics, and contact mechanics couple to regulate adhesion in colloidal systems, offering new insights into particle-substrate interactions in soft matter contexts.

我们实验研究了干燥历史如何影响亲水系统中微粒与基质的粘附。通过在受控条件下系统地改变空气温度、相对湿度和干燥时间,我们量化了单个微粒的分离力。气温成为主导因素:较高的温度和较低的湿度会增强附着力,而长时间的干燥通常会降低附着力,但高温和低湿结合的条件下附着力会持续很强。互补扫描电镜(SEM)结果显示,颗粒-衬底接触尺寸随干燥时间的变化,与毛细管诱导的接触区压缩和部分松弛相一致。这些结果表明,蒸发过程中的瞬态毛细管应力使颗粒-衬底界面变形,并对粘附强度留下持久的印记。总的来说,该研究显示了毛细作用、干燥动力学和接触力学如何耦合来调节胶体系统中的粘附,为软物质环境下颗粒-基质相互作用提供了新的见解。
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引用次数: 0
Osmotic forces modify lipid membrane fluctuations. 渗透力改变脂膜波动。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-19 DOI: 10.1039/d5sm01094b
Amaresh Sahu

In hydrodynamic descriptions of lipid bilayers, the membrane is often approximated as being impermeable to the surrounding, solute-containing fluid. However, biological and in vitro lipid membranes are influenced by their permeability and the resultant osmotic forces-whose effects remain poorly understood. Here, we study the dynamics of a fluctuating, planar lipid membrane that is ideally selective: fluid can pass through it, while solutes cannot. We find that the canonical membrane relaxation mode, in which internal membrane forces are balanced by fluid drag, no longer exists over all wavenumbers. Rather, this mode only exists when it is slower than solute diffusion-corresponding to a finite range of wavenumbers. The well-known equipartition result, quantifying the size of membrane undulations due to thermal perturbations, is consequently limited in its validity to the aforementioned range. Moreover, this range shrinks as the membrane surface tension is increased, and above a critical tension, the membrane mode vanishes. Our findings are relevant when interpreting experimental measurements of membrane fluctuations, especially in vesicles at moderate to high tensions.

在脂质双分子层的流体动力学描述中,膜通常近似为对周围的含溶质流体不渗透。然而,生物和体外脂质膜受到其渗透性和由此产生的渗透力的影响,其作用仍然知之甚少。在这里,我们研究的动态波动,平面脂质膜是理想的选择性:流体可以通过它,而溶质不能。我们发现,在所有波数上,膜内力由流体阻力平衡的典型膜弛豫模式不再存在。相反,这种模式只有在它比溶质扩散慢的时候才存在——对应于有限范围的波数。众所周知的均分结果,量化了由于热扰动引起的膜波动的大小,因此其有效性限制在上述范围内。此外,这个范围随着膜表面张力的增加而缩小,超过临界张力,膜模消失。我们的发现在解释膜波动的实验测量时是相关的,特别是在中高张力的囊泡中。
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引用次数: 0
A hydrogel foam with a gradient pore structure for highly efficient solar-driven seawater desalination. 一种具有梯度孔结构的水凝胶泡沫,用于高效太阳能驱动的海水淡化。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-19 DOI: 10.1039/d6sm00022c
Tangsen He, Xin Li, Peng Kang, Ying Li, Haiyan Zhu, Gang Shi

Solar interface evaporation is a sustainable and clean water production approach. Polymer hydrogels, as some of the core materials of solar-driven interface evaporation systems, have received extensive attention. However, traditional hydrogel foams have randomly distributed open cells and closed cells, which make it difficult to simultaneously achieve rapid water transport and efficient steam escape, and show excellent thermal insulation performance. In this study, a polyvinyl alcohol/acetylene black hydrogel foam (PAPHF) evaporator with a gradient pore structure was developed through a simple and scalable "foaming-resting-crosslinking-freezing" strategy. The top layer of this evaporator has a large-sized open-cell structure, which enhances light absorption, water transport and steam escape, while the bottom layer of the evaporator has a small-sized closed-cell structure, which can effectively reduce heat conduction loss and improve surface heat localization ability. The optimized PAPHF evaporator achieved an evaporation rate of 3.13 kg m-2 h-1 and an energy conversion efficiency of 88.9% under 1 sun radiation (1 kW m-2), exceeding the performance of many of the reported evaporators of the same type. In addition, the PAPHF evaporator can effectively perform seawater desalination and wastewater purification. This study provides a new idea for the structural design of high-performance solar evaporators.

太阳界面蒸发是一种可持续的清洁水生产方法。高分子水凝胶作为太阳能驱动界面蒸发系统的核心材料,受到了广泛的关注。然而,传统的水凝胶泡沫具有随机分布的开孔和闭孔,难以同时实现快速的水分输送和高效的蒸汽逸出,并表现出优异的保温性能。本研究采用简单可扩展的“发泡-静置-交联-冷冻”策略,研制了具有梯度孔结构的聚乙烯醇/乙炔黑色水凝胶泡沫(PAPHF)蒸发器。该蒸发器顶层采用大尺寸开孔结构,增强了光吸收、水输运和蒸汽逸出,而蒸发器底层采用小尺寸闭孔结构,可有效减少热传导损失,提高表面热定位能力。优化后的PAPHF蒸发器在1次太阳辐射(1 kW m-2)下的蒸发速率为3.13 kg m-2 h-1,能量转换效率为88.9%,超过了许多已报道的同类型蒸发器的性能。此外,PAPHF蒸发器可以有效地进行海水淡化和废水净化。该研究为高性能太阳能蒸发器的结构设计提供了新的思路。
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引用次数: 0
Correction: Capillary assembly of metal-coated polymer microspheres for interconnection in electronic applications. 修正:用于电子应用互连的金属涂层聚合物微球的毛细管组装。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-19 DOI: 10.1039/d6sm90038k
Van Long Huynh, Knut E Aasmundtveit, Hoang-Vu Nguyen

Correction for 'Capillary assembly of metal-coated polymer microspheres for interconnection in electronic applications' by Van Long Huynh et al., Soft Matter, 2025, 21, 6641-6648. DOI: https://doi.org/10.1039/D5SM00446B.

“电子应用中用于互连的金属涂层聚合物微球毛细管组装”的修正,Van Long Huynh等人,软物质,2025,21,6641-6648。DOI: https://doi.org/10.1039/D5SM00446B。
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引用次数: 0
Elastic resistive force theory: development and applications to flexible intruders. 弹性阻力理论:在柔性入侵者中的发展与应用。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-18 DOI: 10.1039/d6sm00040a
Lale Yılmaz, Madison Douglas, J Taylor Perron, Ken Kamrin

Dry granular intrusion and extraction occur commonly for off-road vehicles, foundation work, and plant uprooting. Although many models exist to describe such scenarios, reduced-order models such as granular resistive force theory (RFT), offer a good balance between accuracy and computational cost. RFT efficiently approximates the resistive force experienced by an intruder moving through a granular medium as a function of the intruder's velocity direction, geometry, and material parameters. However, due to the explicitly velocity-dependent nature of its formulation, it fails at modeling static conditions, the force build-up that occurs before flow, and stagnant points on moving intruders. We propose elastic RFT to remedy these shortcomings. Elastic RFT intrinsically models both granular elasticity and flow adjacent to intruders by splitting intruder motion into separate parts corresponding to elastic and plastic granular deformation. This allows force to build up elastically before flow and lets the plastic part of motion maintain RFT flow rules. We present the details of the underlying kinematic and constitutive assumptions for elastic RFT. Moreover, we also propose a procedure to couple RFT or elastic RFT to deformable intruders, which we demonstrate in applications of elastic RFT to sample plant uprooting problems treating the roots as nonlinear inextensible beams. We highlight potential application areas for elastic RFT coupled to deformable objects, including simulation of deformable wheel locomotion.

干颗粒侵入和提取通常发生在越野车辆,基础工作和植物连根拔起。尽管存在许多模型来描述这种情况,但诸如颗粒阻力理论(RFT)之类的降阶模型在精度和计算成本之间提供了很好的平衡。RFT有效地将入侵者在颗粒介质中移动时所经历的阻力近似为入侵者的速度方向、几何形状和材料参数的函数。然而,由于其公式明显依赖于速度的性质,它无法模拟静态条件,在流动之前发生的力积累以及移动入侵者的停滞点。我们提出弹性RFT来弥补这些缺点。弹性RFT通过将侵入体运动分解为对应于弹性和塑性颗粒变形的独立部分,从本质上模拟了侵入体附近的颗粒弹性和流动。这允许力在流动之前形成弹性,并使运动的塑性部分保持RFT流动规则。我们提出了弹性RFT的基本运动学和本构假设的细节。此外,我们还提出了一种将RFT或弹性RFT耦合到变形入侵者的方法,并将弹性RFT应用于将根视为非线性不可扩展梁的植物连根问题。我们强调了弹性RFT与可变形物体耦合的潜在应用领域,包括可变形车轮运动的模拟。
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引用次数: 0
A solvent-topology perspective on hydrophobic aggregation. 疏水聚集的溶剂拓扑研究。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-18 DOI: 10.1039/d5sm01246e
Vicente Domínguez-Arca

Hydrophobic aggregation is often described in terms of effective attractive forces between apolar units. In aqueous and soft-matter environments, however, aggregation necessarily involves a collective reorganization of the solvent, whose connectivity and confinement properties may play a central role. Here we investigate a deliberately minimal lattice model in which hydrophobic (apolar) segments interact with the solvent only through a local restriction rule, without introducing explicit solute-solute attractions. Each lattice site is occupied either by solvent or by an apolar segment at a fixed composition. Solvent sites are classified as restricted when the local density of nearby apolar segments exceeds a prescribed threshold, and configurations are sampled with a Boltzmann-like weight that penalizes the total number of restricted-solvent sites. Within this framework, aggregation can only arise through the reorganization of solvent restriction fields. By decomposing the solvent into free and restricted subsets, we analyze their connectivity using standard percolation diagnostics alongside conventional measures of solute clustering. Baseline simulations reveal that while amphiphile aggregation evolves smoothly with concentration, the restricted-solvent subset can undergo a sharp, kernel-dependent connectivity crossover: for sufficiently isotropic interaction neighborhoods, restricted water becomes a system - spanning only over an intermediate range of solute fractions. Free solvent, by contrast, remains spanning across the explored parameter range. Notably, these solvent-topology signatures are significantly sharper and more structured than the corresponding solute-ordering metrics. A systematic extension to larger system sizes refines this picture. The onset of restricted-solvent spanning remains localized and kernel selective, while high-density behavior becomes smoother and more fluctuation dominated, consistent with finite-size effects. Importantly, the amount of restricted solvent grows monotonically and robustly with system size, whereas its global connectivity reorganizes nontrivially. Taken together, these results support a restrained interpretation of hydrophobic aggregation as a solvent-driven topological crossover rather than a sharp thermodynamic phase transition, highlighting solvent topology as a sensitive diagnostic even when solute ordering remains gradual.

疏水聚集通常用极性单元之间的有效引力来描述。然而,在水和软物质环境中,聚集必然涉及溶剂的集体重组,其连通性和约束性质可能起核心作用。在这里,我们研究了一个刻意最小的晶格模型,其中疏水(极性)段仅通过局部限制规则与溶剂相互作用,而不引入明确的溶质-溶质吸引。在固定的组合物中,每个晶格位置要么被溶剂占据,要么被极性段占据。当附近极性段的局部密度超过规定的阈值时,溶剂位点被分类为受限的,并且配置用玻尔兹曼样权重进行采样,该权重对受限溶剂位点的总数进行惩罚。在这个框架内,聚合只能通过溶剂限制场的重组而产生。通过将溶剂分解为自由和受限的子集,我们使用标准的渗透诊断和传统的溶质聚类测量来分析它们的连通性。基线模拟表明,虽然两亲体聚集随着浓度的变化而平稳发展,但限制溶剂子集可以经历一个尖锐的、依赖于核的连通性交叉:对于充分各向同性的相互作用邻域,限制水成为一个系统,仅跨越溶质分数的中间范围。相比之下,自由溶剂仍然跨越所探索的参数范围。值得注意的是,这些溶剂拓扑特征比相应的溶质排序指标更加清晰和结构化。系统扩展到更大的系统规模使这一图景更加完美。限制溶剂跨越的开始仍然是局部的和核选择性的,而高密度行为变得更平滑,更多的波动主导,与有限尺寸效应一致。重要的是,限制溶剂的数量随系统大小单调而稳健地增长,而其全局连通性则非平凡地重组。综上所述,这些结果支持了疏水聚集作为溶剂驱动的拓扑交叉而不是一个尖锐的热力学相变的克制解释,强调溶剂拓扑作为一个敏感的诊断,即使溶质顺序仍然是渐进的。
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引用次数: 0
Pre-yielding mechanical response near the jamming transition. 干扰过渡附近的预屈服力学响应。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-18 DOI: 10.1039/d5sm01183c
Hidemasa Bessho, Takeshi Kawasaki, Kunimasa Miyazaki

The mechanical and rheological properties of jammed packings of frictionless particles under shear strain remain not fully understood, even when the strain amplitude is very small and well below the yielding threshold. Systems above the jamming transition point φJ are known to display two anomalous mechanical behaviors with respect to the driving frequency ω (or time t) and the strain amplitude γ. In the linear-response regime (γ → 0), the complex modulus exhibits an algebraic scaling, G(ω) ∼ ω1/2 (or G(t) ∼ t-1/2 in the time representation). In contrast, in the quasi-static limit (ω → 0), the modulus shows the nonlinear behavior, G(γ) ∼ γ-1/2, a phenomenon referred to as softening. The ranges of ω and γ over which these algebraic scalings hold broaden as φJ is approached from above, whereas both G(ω) and G(γ) vanish for φ < φJ. In this study, we investigate the mechanical response in the regime where these two anomalies coexist in the vicinity of φJ. To this end, we perform numerical analyses using two rheological protocols: oscillatory shear and transient stress relaxation. Our results demonstrate that the mechanical responses are not simply described as a superposition of the two algebraic relaxations and instead exhibit rich nonlinear viscoelastic behavior both above and even below φJ.

无摩擦颗粒堵塞填料在剪切应变下的力学和流变特性仍未完全了解,即使应变幅度非常小且远低于屈服阈值。已知在干扰过渡点φJ以上的系统与驱动频率ω(或时间t)和应变幅值γ有关,表现出两种异常的力学行为。在线性响应区(γ→0),复模量呈现代数标度,G(ω) ~ ω1/2(或G(t) ~ t-1/2在时间表示中)。相反,在准静态极限(ω→0)下,模量表现出非线性行为,G(γ) ~ γ-1/2,这种现象被称为软化。当φ j从上面逼近时,这些代数标度的ω和γ范围变宽,而对于φ < φ j, G(ω)和G(γ)消失。在本研究中,我们研究了在φJ附近这两种异常共存的区域内的力学响应。为此,我们使用两种流变学协议进行数值分析:振荡剪切和瞬态应力松弛。我们的研究结果表明,力学响应不是简单地描述为两个代数松弛的叠加,而是在φJ以上甚至低于φJ时都表现出丰富的非线性粘弹性行为。
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引用次数: 0
Nonequilibrium phases of a biomolecular condensate facilitated by enzyme activity. 酶活性促进的生物分子凝聚物的非平衡相。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-18 DOI: 10.1039/d5sm01106j
Sebastian Coupe, Nikta Fakhri

Biomolecular condensates represent a frontier in cellular organization, existing as dynamic macromolecular structures driven out of equilibrium by active cellular processes. Here we explore active mechanisms of condensate regulation by examining the interplay between DEAD-box helicase activity and RNA base-pairing interactions within a reconstituted ribonucleoprotein condensate. We demonstrate that the ATP-dependent activity of a DEAD-box helicase-a key class of enzymes in condensate regulation-acts as a nonequilibrium driver of condensate properties through the continuous remodeling of RNA interactions. By combining the LAF-1 DEAD-box helicase with a designer RNA hairpin concatemer, we unveil a complex landscape of dynamic behaviors, including time-dependent alterations in RNA partitioning, evolving condensate morphologies, and shifting condensate dynamics. Importantly, we reveal an antagonistic relationship between RNA secondary structure and helicase activity which enables an initially homogeneous nonequilibrium state. By elucidating these nonequilibrium mechanisms, we gain a deeper understanding of cellular organization and expand the potential for active synthetic condensate systems.

生物分子凝聚体代表了细胞组织的前沿,作为动态的大分子结构存在,被活跃的细胞过程赶出平衡。本研究通过研究DEAD-box解旋酶活性与重组核糖核蛋白凝析物中RNA碱基配对相互作用之间的相互作用,探索凝析物调控的活性机制。我们证明了DEAD-box解旋酶的atp依赖性活性——在凝析物调节中的一类关键酶——通过RNA相互作用的持续重塑,作为凝析物性质的非平衡驱动因素。通过将af -1 DEAD-box解旋酶与设计RNA发夹串联器相结合,我们揭示了动态行为的复杂景观,包括RNA分配的时间依赖性改变,进化的凝聚形态和转移的凝聚动力学。重要的是,我们揭示了RNA二级结构和解旋酶活性之间的拮抗关系,这使得最初均匀的非平衡状态成为可能。通过阐明这些非平衡机制,我们对细胞组织有了更深入的了解,并扩大了活性合成凝析油系统的潜力。
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引用次数: 0
Nudging cell migration from within through microrod-induced morphological deformation. 通过微棒诱导的形态变形,推动细胞从内部迁移。
IF 2.8 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2026-03-17 DOI: 10.1039/d5sm01149c
Masayuki Hayakawa, Tatsuya Tanaka, Hiroaki Suzuki

Cell migration plays a central role in various biological processes, including development, wound healing, and cancer metastasis, and represents a fundamental form of self-organized motion at the cellular scale. These self-propelled cells can serve as microscale agents with potential applications in bioengineering and microsystem design. To realize such possibilities, it is essential to establish effective methods for controlling their migration. Conventional approaches, such as chemotactic, optogenetic, and substrate-based guidance, depend on external interventions that influence only a limited number of cells. Here, we present a proof-of-concept in Dictyostelium discoideum to bias cell migration by inducing deformation from within the cell. We demonstrate that glass microrods are internalized and that these internalized rods elongate the cells along their own axis. The elongated cells tend to migrate in the direction of their long axis, resulting in enhanced directional persistence. Unlike conventional methods requiring external deterministic cues or patterned environments, our approach enables cells to autonomously and persistently alter their migration behavior through internal morphological deformation. This study introduces a new framework for modulating cell migration and establishes a foundation for developing biohybrid systems that utilize living cells as self-propelled carriers.

细胞迁移在多种生物过程中起着核心作用,包括发育、伤口愈合和癌症转移,是细胞尺度上自组织运动的一种基本形式。这些自推进细胞在生物工程和微系统设计中具有潜在的应用前景。为了实现这种可能性,必须建立有效的方法来控制它们的迁移。传统的方法,如趋化、光遗传和基于底物的引导,依赖于仅影响有限数量细胞的外部干预。在这里,我们提出了一个概念证明,在盘状盘基骨柱通过诱导细胞内的变形来偏倚细胞迁移。我们证明了玻璃微棒是内化的,这些内化的棒沿着它们自己的轴延长细胞。细长的细胞倾向于向其长轴方向迁移,从而增强了定向持久性。与需要外部确定性线索或模式环境的传统方法不同,我们的方法使细胞能够通过内部形态变形自主和持续地改变其迁移行为。本研究提出了一个调节细胞迁移的新框架,并为开发利用活细胞作为自我推进载体的生物混合系统奠定了基础。
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引用次数: 0
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Soft Matter
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