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Local electroneutrality breakdown for electrolytes within varying-section nanopores 不同截面纳米孔内电解质的局部电中和击穿。
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-02-19 DOI: 10.1140/epje/s10189-024-00408-9
Paolo Malgaretti, Ignacio Pagonabarraga, Jens Harting

We determine the local charge dynamics of a (z-z) electrolyte embedded in a varying-section channel. By means of an expansion based on the length scale separation between the axial and transverse direction of the channel, we derive closed formulas for the local excess charge for both, dielectric and conducting walls, in 2D (planar geometry) as well as in 3D (cylindrical geometry). Our results show that, even at equilibrium, the local charge electroneutrality is broken whenever the section of the channel is not homogeneous for both dielectric and conducting walls as well as for 2D and 3D channels. Interestingly, even within our expansion, the local excess charge in the fluid can be comparable to the net charge on the walls. We critically discuss the onset of such local electroneutrality breakdown in particular with respect to the correction that it induces on the effective free energy profile experienced by tracer ions.

我们确定了[公式:见正文]电解质嵌入变截面通道的局部电荷动态。通过基于通道轴向和横向之间长度尺度分离的扩展,我们得出了介电壁和导电壁局部过剩电荷在二维(平面几何)和三维(圆柱几何)中的封闭公式。我们的结果表明,即使在平衡状态下,只要通道截面不均匀,介电壁和导电壁以及二维和三维通道的局部电荷电中性都会被打破。有趣的是,即使在我们的扩展中,流体中的局部过剩电荷也可能与壁上的净电荷相当。我们认真讨论了这种局部电中性崩溃的发生,特别是它对示踪离子所经历的有效自由能曲线的修正。
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引用次数: 0
From isolated polyelectrolytes to star-like assemblies: the role of sequence heterogeneity on the statistical structure of the intrinsically disordered neurofilament-low tail domain 从孤立的多电解质到星状集合体:序列异质性对内在无序神经丝低尾结构统计结构的作用。
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-02-15 DOI: 10.1140/epje/s10189-024-00409-8
Mathar Kravikass, Gil Koren, Omar A. Saleh, Roy Beck

Intrinsically disordered proteins (IDPs) are a subset of proteins that lack stable secondary structure. Given their polymeric nature, previous mean-field approximations have been used to describe the statistical structure of IDPs. However, the amino-acid sequence heterogeneity and complex intermolecular interaction network have significantly impeded the ability to get proper approximations. One such case is the intrinsically disordered tail domain of neurofilament low (NFLt), which comprises a 50 residue-long uncharged domain followed by a 96 residue-long negatively charged domain. Here, we measure two NFLt variants to identify the impact of the NFLt two main subdomains on its complex interactions and statistical structure. Using synchrotron small-angle x-ray scattering, we find that the uncharged domain of the NFLt induces attractive interactions that cause it to self-assemble into star-like polymer brushes. On the other hand, when the uncharged domain is truncated, the remaining charged N-terminal domains remain isolated in solution with typical polyelectrolyte characteristics. We further discuss how competing long- and short-ranged interactions within the polymer brushes dominate their ensemble structure and, in turn, their implications on previously observed phenomena in NFL native and diseased states.

Visual schematic of the SAXS measurement results of the Neurofilament-low tail domain IDP (NFLt). NFLts assemble into star-like brushes through their hydrophobic N-terminal domains (marked in blue). In increasing salinity, brush height (h) is initially increased following a decrease while gaining additional tails to their assembly. Isolating the charged sub-domain of the NFLt (marked in red) results in isolated polyelectrolytes

本征无序蛋白(IDPs)是缺乏稳定二级结构的蛋白质子集。鉴于其聚合性质,以往的均场近似方法被用来描述 IDPs 的统计结构。然而,氨基酸序列的异质性和复杂的分子间相互作用网络极大地阻碍了获得适当近似值的能力。神经丝蛋白(neurofilament low,NFLt)的内在无序尾部结构域就是这样一种情况,它由一个 50 个残基长的不带电结构域和一个 96 个残基长的带负电结构域组成。在这里,我们测量了两个 NFLt 变体,以确定 NFLt 的两个主要子域对其复杂相互作用和统计结构的影响。利用同步加速器小角 X 射线散射,我们发现 NFLt 的不带电结构域会诱导吸引性相互作用,使其自组装成星状聚合物刷。另一方面,当非带电结构域被截断时,剩余的带电 N 端结构域在溶液中保持孤立,具有典型的聚电解质特征。我们进一步讨论了聚合物刷中相互竞争的长程和短程相互作用是如何主导它们的集合结构的,并反过来讨论了它们对之前观察到的 NFL 本态和病态现象的影响。
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引用次数: 0
Dynamic structure factor of undulating vesicles: finite-size and spherical geometry effects with application to neutron spin echo experiments 起伏囊泡的动态结构因子:有限尺寸和球形几何效应在中子自旋回波实验中的应用。
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-02-14 DOI: 10.1140/epje/s10189-023-00400-9
Rony Granek, Ingo Hoffmann, Elizabeth G. Kelley, Michihiro Nagao, Petia M. Vlahovska, Anton Zilman

We consider the dynamic structure factor (DSF) of quasi-spherical vesicles and present a generalization of an expression that was originally formulated by Zilman and Granek (ZG) for scattering from isotropically oriented quasi-flat membrane plaquettes. The expression is obtained in the form of a multi-dimensional integral over the undulating membrane surface. The new expression reduces to the original stretched exponential form in the limit of sufficiently large vesicles, i.e., in the micron range or larger. For much smaller unilamellar vesicles, deviations from the asymptotic, stretched exponential equation are noticeable even if one assumes that the Seifert-Langer leaflet density mode is completely relaxed and membrane viscosity is neglected. To avoid the need for an exhaustive numerical integration while fitting to neutron spin echo (NSE) data, we provide a useful approximation for polydisperse systems that tests well against the numerical integration of the complete expression. To validate the new expression, we performed NSE experiments on variable-size vesicles made of a POPC/POPS lipid mixture and demonstrate an advantage over the original stretched exponential form or other manipulations of the original ZG expression that have been deployed over the years to fit the NSE data. In particular, values of the membrane bending rigidity extracted from the NSE data using the new approximations were insensitive to the vesicle radii and scattering wavenumber and compared very well with expected values of the effective bending modulus ((tilde{kappa })) calculated from results in the literature. Moreover, the generalized scattering theory presented here for an undulating quasi-spherical shell can be easily extended to other models for the membrane undulation dynamics beyond the Helfrich Hamiltonian and thereby provides the foundation for the study of the nanoscale dynamics in more complex and biologically relevant model membrane systems.

我们考虑了准球形囊泡的动态结构因子(DSF),并对齐尔曼和格兰尼克(ZG)最初提出的等向定向准扁平膜块散射表达式进行了概括。该表达式以起伏膜表面的多维积分形式获得。在足够大的囊泡范围内,即微米或更大的范围内,新的表达式还原为原始的拉伸指数形式。对于小得多的单淀粉囊泡,即使假定塞弗特-朗格小叶密度模式完全松弛并忽略膜粘度,也会明显偏离渐近拉伸指数方程。为了避免在拟合中子自旋回波(NSE)数据时进行详尽的数值积分,我们为多分散系统提供了一个有用的近似值,它能很好地检验完整表达式的数值积分。为了验证新表达式的有效性,我们对由 POPC/POPS 脂质混合物制成的可变大小囊泡进行了 NSE 实验,结果表明新表达式比多年来用于拟合 NSE 数据的原始拉伸指数形式或对原始 ZG 表达式的其他处理方法更具优势。特别是,使用新近似值从 NSE 数据中提取的膜弯曲刚度值对囊泡半径和散射波长不敏感,与根据文献结果计算出的有效弯曲模量预期值([公式:见正文])相比,效果非常好。此外,这里提出的针对起伏准球形壳的广义散射理论可以很容易地扩展到赫尔弗里希哈密顿以外的其他膜起伏动力学模型,从而为研究更复杂和生物相关模型膜系统的纳米尺度动力学奠定了基础。
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引用次数: 0
Collective motion of chiral particles in complex noise environments 手性粒子在复杂噪声环境中的集体运动
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-02-06 DOI: 10.1140/epje/s10189-023-00403-6
Jun Huang, Zhi-Gang Shao

Collective motion of chiral particles in complex noise environments is investigated based on the Vicsek model. In the model, we added chirality, along with complex noise, affecting particles clustering motion. Particles can only avoid noise interference in a specific channel, and this consideration is more realistic due to the complexity of the environment. Via simulations, we find that the channel proportion, p, critically influences chiral particle synchronization. Specifically, we observe a disorder-order transition at critical (p_textrm{c}), only when (p>p_textrm{c}), the system can achieve global synchronization. Combined with our definition of spatial distribution parameter and observation of the model, the reason is that particles begin to escape from the noise region under the influence of complex noise. In addition, the value of (p_textrm{c}) increases linearly with velocity, while it decreases monotonically with the increase in chirality and interaction radius. Interestingly, an appropriate noise amplitude minimizes (p_textrm{c}). Our findings may inspire novel strategies to manipulate self-propelled particles of distinct chirality to achieve desired spatial migration and global synchronization.

基于 Vicsek 模型,研究了手性粒子在复杂噪声环境中的集群运动。在该模型中,我们加入了手性以及影响粒子集群运动的复杂噪声。粒子只能在特定通道中避免噪声干扰,由于环境的复杂性,这种考虑更为现实。通过模拟,我们发现通道比例 p 对手性粒子的同步性有重要影响。具体来说,我们观察到在临界[公式:见正文]处出现了无序阶跃,只有当[公式:见正文]时,系统才能实现全局同步。结合我们对空间分布参数的定义和对模型的观察,原因在于粒子在复杂噪声的影响下开始逃离噪声区。此外,[公式:见正文]的值随速度线性增加,而随手性和相互作用半径的增加单调减少。有趣的是,适当的噪声振幅能使[公式:见正文]最小化。我们的发现可能会启发我们采用新的策略来操纵具有不同手性的自推进粒子,以实现所需的空间迁移和全局同步。
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引用次数: 0
Macroscopic dynamics of the ferroelectric smectic (A_F) phase with (C_{infty v} ) symmetry 具有 $$C_{infty v} $$ 对称性的铁电 Smectic $$A_F$ 相的宏观动力学
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-02-02 DOI: 10.1140/epje/s10189-024-00406-x
Helmut R. Brand, Harald Pleiner

We present the macroscopic dynamics of ferroelectric smectic A, smectic (A_F), liquid crystals reported recently experimentally by three groups. In this fluid and orthogonal smectic phase, the macroscopic polarization, ({textbf{P}}), is parallel to the layer normal thus giving rise to (C_{infty v}) overall symmetry for this phase in the spatially homogeneous limit. A combination of linear irreversible thermodynamics and symmetry arguments is used to derive the resulting dynamic equations applicable at sufficiently low frequencies and sufficiently long wavelengths. Compared to non-polar smectic A phases, we find a static cross-coupling between compression of the layering and bending of the layers, which does not lead to elastic forces, but to elastic stresses. In addition, it turns out that a reversible cross-coupling between flow and the magnitude of the polarization modifies the velocities of both, first and second sound. At the same time, the relaxation of the polarization gives rise to dissipative effects for second sound at the same order of the wavevector as for the sound velocity. We also analyze reversible cross-coupling terms between elongational flow and electric fields as well as temperature and concentration gradients, which lend themselves to experimental detection. Apparently this type of terms has never been considered before for smectic phases. The question how the linear ({{textbf{P}} cdot textbf{E}}) coupling in the energy alters the macroscopic response behavior when compared to usual non-polar smectic A phases is also addressed.

AbstractWe present the macroscopic dynamics of ferroelectric smectic A, smectic (A_F),smectic liquid crystals reported recently experally by three groups.在这种流体和正交的共晶相中,宏观极化(({textbf{P}})与层法线平行,因此在空间均匀极限中,该相具有(C_{infty v})整体对称性。线性不可逆热力学和对称性论证相结合,得出了适用于足够低频率和足够长波长的动态方程。与非极性 Smectic A 相相比,我们发现分层压缩和层弯曲之间存在静态交叉耦合,这不会导致弹性力,但会导致弹性应力。此外,流动与极化大小之间的可逆交叉耦合改变了第一和第二声的速度。与此同时,极化的松弛会对第二声产生耗散效应,其波矢阶与声速的波矢阶相同。我们还分析了伸长流与电场以及温度和浓度梯度之间的可逆交叉耦合项,这些项都可以通过实验检测到。显然,这种类型的项以前从未被考虑过。与通常的非极性脂相相比,能量中的线({{textbf{P}} cdot textbf{E}} )耦合如何改变宏观响应行为的问题也得到了探讨。
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引用次数: 0
Optimal escapes in active matter 活性物质中的最佳逃逸
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-01-28 DOI: 10.1140/epje/s10189-023-00402-7
Luca Angelani

The out-of-equilibrium character of active particles, responsible for accumulation at boundaries in confining domains, determines not-trivial effects when considering escape processes. Non-monotonous behavior of exit times with respect to tumbling rate (inverse of mean persistent time) appears, as a consequence of the competing processes of exploring the bulk and accumulate at boundaries. By using both 1D analytical results and 2D numerical simulations of run-and-tumble particles with different behaviours at boundaries, we scrutinize this very general phenomenon of active matter, evidencing the role of accumulation at walls for the existence of optimal tumbling rates for fast escapes.

在考虑逃逸过程时,活动粒子的非平衡特性决定了其在约束域中边界处的积累会产生非同小可的影响。出口时间与翻滚速率(平均持续时间的倒数)的非单调行为出现了,这是在体外探索和在边界积累的竞争过程的结果。通过使用一维分析结果和二维数值模拟在边界上具有不同行为的运行和翻滚粒子,我们仔细研究了这一非常普遍的活动物质现象,证明了在壁面上的积累对于快速逃逸的最佳翻滚速率的存在所起的作用。
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引用次数: 0
Vesicle condensation induced by synapsin: condensate size, geometry, and vesicle shape deformations 突触素诱导的囊泡凝聚:凝聚物的大小、几何形状和囊泡形状变形。
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-01-25 DOI: 10.1140/epje/s10189-023-00404-5
Jette Alfken, Charlotte Neuhaus, András Major, Alyona Taskina, Christian Hoffmann, Marcelo Ganzella, Arsen Petrovic, David Zwicker, Rubén Fernández-Busnadiego, Reinhard Jahn, Dragomir Milovanovic, Tim Salditt

We study the formation of vesicle condensates induced by the protein synapsin, as a cell-free model system mimicking vesicle pool formation in the synapse. The system can be considered as an example of liquid–liquid phase separation (LLPS) in biomolecular fluids, where one phase is a complex fluid itself consisting of vesicles and a protein network. We address the pertinent question why the LLPS is self-limiting and stops at a certain size, i.e., why macroscopic phase separation is prevented. Using fluorescence light microscopy, we observe different morphologies of the condensates (aggregates) depending on the protein-to-lipid ratio. Cryogenic electron microscopy then allows us to resolve individual vesicle positions and shapes in a condensate and notably the size and geometry of adhesion zones between vesicles. We hypothesize that the membrane tension induced by already formed adhesion zones then in turn limits the capability of vesicles to bind additional vesicles, resulting in a finite condensate size. In a simple numerical toy model we show that this effect can be accounted for by redistribution of effective binding particles on the vesicle surface, accounting for the synapsin-induced adhesion zone.

我们研究了蛋白突触素诱导的囊泡凝聚物的形成,这是一种模拟突触中囊泡池形成的无细胞模型系统。该系统可视为生物分子流体中液-液相分离(LLPS)的一个实例,其中一相本身就是由囊泡和蛋白质网络组成的复杂流体。我们要解决的相关问题是,为什么液-液相分离具有自限性并在一定大小时停止,即为什么宏观相分离会被阻止。利用荧光显微镜,我们观察到凝结物(聚合体)的不同形态取决于蛋白质与脂质的比例。通过低温电子显微镜,我们可以分辨凝集物中单个囊泡的位置和形状,尤其是囊泡之间粘附区的大小和几何形状。我们假设,已经形成的粘附区所引起的膜张力反过来又限制了囊泡结合其他囊泡的能力,从而导致凝结物的大小有限。在一个简单的数值玩具模型中,我们发现这种效应可以通过囊泡表面有效结合粒子的重新分布来解释,从而解释突触素诱导的粘附区。
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引用次数: 0
Detachment forces during parallel-plate gap separation mediated by a simple yield-stress fluid 由简单屈服应力流体介导的平行板间隙分离过程中的脱离力。
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-01-23 DOI: 10.1140/epje/s10189-023-00397-1
Vítor Hugo de Oliveira Pereira, Wilson Barros Jr.

In this work we have monitored the multiple stages of the normal traction force response of a yield-stress fluid confined between two circular parallel plates that are separated at constant velocity. At narrow initial gaps, the air–fluid interface suffers from the Saffman–Taylor instability, confirmed by visual inspection of fingering patterns imprinted on the fluid. At larger initial gaps, the fluid preserves the initially imposed circular symmetry of the confining plates, indicating the absence of instability. Due to the system characteristics and experimental environment, the multiple traction force contributions occurred in cascade, permitting us to isolate the adhesion responses associated with viscosity, capillarity, and yield stress. Employing a standard Herschel–Bulkley model, we assessed the scaling of the traction force in multiple regimes—specifically, evaluating the dependencies of the fingering to yield-stress transitions.

在这项研究中,我们对封闭在以恒定速度分开的两块圆形平行板之间的屈服应力流体的法向牵引力响应的多个阶段进行了监测。在初始间隙较小的情况下,空气-流体界面会出现萨夫曼-泰勒不稳定性,通过目测流体上的指印图案可以证实这一点。在初始间隙较大时,流体保持了最初施加的约束板圆形对称性,表明不存在不稳定性。由于系统特性和实验环境的原因,多重牵引力的作用是级联发生的,这使我们能够分离出与粘度、毛细管性和屈服应力相关的粘附反应。采用标准的赫歇尔-布克雷模型,我们评估了牵引力在多种状态下的缩放比例,特别是评估了指法到屈服应力转换的依赖关系。
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引用次数: 0
Scaling regimes for wormlike chains confined to cylindrical surfaces under tension 局限于圆柱表面的蠕虫链在张力作用下的缩放机制。
IF 1.8 4区 物理与天体物理 Q4 CHEMISTRY, PHYSICAL Pub Date : 2024-01-22 DOI: 10.1140/epje/s10189-023-00384-6
Greg Morrison, D. Thirumalai

We compute the free energy of confinement (mathcal{{F}}) for a wormlike chain (WLC), with persistence length (l_p), that is confined to the surface of a cylinder of radius R under an external tension f using a mean field variational approach. For long chains, we analytically determine the behavior of the chain in a variety of regimes, which are demarcated by the interplay of (l_p), the Odijk deflection length ((l_d=(R^2l_p)^{1/3})), and the Pincus length ((l_f = {k_BT}/{f}), with (k_BT) being the thermal energy). The theory accurately reproduces the Odijk scaling for strongly confined chains at (f=0), with (mathcal{{F}}sim Ll_p^{-1/3}R^{-2/3}). For moderate values of f, the Odijk scaling is discernible only when ({l_p}gg R) for strongly confined chains. Confinement does not significantly alter the scaling of the mean extension for sufficiently high tension. The theory is used to estimate unwrapping forces for DNA from nucleosomes.

我们利用均值场变分法计算了蠕虫链(WLC)的约束自由能[计算公式:见正文],蠕虫链的持续长度为[计算公式:见正文],在外部张力 f 的作用下,蠕虫链被约束在半径为 R 的圆柱体表面。对于长链,我们分析确定了链在各种状态下的行为,这些状态由[公式:见正文]、奥迪克偏转长度([公式:见正文])和平卡斯长度([公式:见正文],[公式:见正文]为热能)的相互作用来划分。该理论准确地再现了强约束链在[公式:见正文]与[公式:见正文]之间的 Odijk 缩放。对于中等值的 f,只有当强封闭链的[式:见正文]时,才能看到 Odijk 缩放。在张力足够大的情况下,密闭并不会明显改变平均延伸率的比例。该理论用于估算核糖体中 DNA 的解缠力。
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引用次数: 0
Correction: Convective mixing in porous media: a review of Darcy, pore-scale and Hele-Shaw studies 更正:多孔介质中的对流混合:达西、孔隙尺度和赫勒-肖研究综述。
IF 1.8 4区 物理与天体物理 Q3 Chemistry Pub Date : 2024-01-11 DOI: 10.1140/epje/s10189-023-00401-8
Marco De Paoli
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引用次数: 0
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The European Physical Journal E
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