受驱无序胶体动力学

利用Langevin分子动力学，本数值研究点钉扎中心随机分布的二维胶体动力学．随着钉扎中心强度的提高，我们发现了从弹性脱钉到塑性脱钉的渡越，并伴随临界钉扎力在渡越区的明显提高，类似于超导体中的峰值效应．另外，我们首次发现：当塑性流动发生时，高速运动胶体粒子感受到的平均钉扎力在从玻璃态到液态的转变过程中会出现峰值效应，并伴随有速度-驱动力曲线的交叠．     

Key role of receptor density in colloid/cell specific interaction: a quantitative biomimetic study on giant vesicles

This paper presents an experimental study of the adsorption of colloids on model membranes mediated by specific ligand-receptor interactions. The colloids consist of lipid multilamellar liposomes (spherulites) functionalized with the B-subunit of Shiga Toxin (STxB), while the membranes are lipid Giant Unilamellar Vesicles (GUV) containing STxB lipid receptor, Globotriaosylceramide (Gb3). Through confocal microscopy and flow cytometry, we show the specificity of the adsorption. Moreover, we show that flow cytometry can be used to efficiently quantify the kinetics of colloid adsorption on GUVs with very good statistics. By varying the bulk colloid concentration and receptor density in the membrane, we point out the existence of an optimum Gb3 density for adsorption. We propose that this optimum corresponds to a transition between reversible colloid adsorption at low Gb3 density and irreversible adsorption, and likely spherulite fusion, at high density. We compare our results both to STxB-colloids adhering on living cells and to free STxB proteins interacting with GUVs containing Gb3. This biomimetic system could be used for a quantitative evaluation of the early stage of virus infection or drug delivery.     

A classical density functional approach to depletion interaction of Lennard-Jones binary mixtures

In this article, we apply classical density functional theory to investigate the characteristics of depletion interaction in Lennard-Jones (LJ) binary fluid mixtures. First, to confirm the validity of our adopted density functional formalism, we calculate the radial distribution functions using a theoretical approach and compare them with results obtained by molecular dynamics simulation. Then, this approach is applied to two colloids immersed in LJ solvent systems. We investigate the variation of depletion interaction with respect to the distance of two colloids in LJ binary systems. We find that depletion interaction may be attractive or repulsive, mostly depending on the bulk density of the solvent and the temperature of the binary system. For high bulk densities, the repulsive barrier of depletion force is remarkable when the total excluded volume of colloids touches each other and reaches a maximum. The height of the repulsive barrier is related to the parameters of the LJ potential and bulk density. Moreover, the depletion force may exhibit attractive wells if the bulk density of the solvent is low. The attractive well tends to appear when the surface–surface distance of colloids is half of the size of the polymer and deepens with temperature lowering in a fixed bulk density. In contrast with the hard-sphere system, no oscillation of depletion potential around zero is observed.     

结晶紫的表面增强共振拉曼光谱和银胶浓度的关系

常用的银胶一般浓度较低且不稳定,这就限制了它在表面增强共振拉曼谱(SERRS)中的应用,本文旨在探讨一种容易制备,浓度高而且特别稳定的银胶在增强结晶紫(CV)SERRS讯号方面的应用,对一定浓度的CV,我们发现只有配合适当浓度的银胶才能获得最强的SERRS的信号,这个现象是由于稳定剂(PVP)在银颗粒表面的作用造成的。     

Nonequilibrium forces between dragged ultrasoft colloids

The dynamical deformation of ultrasoft colloids as well as their dynamic frictional forces are numerically investigated, when one colloid is dragged past another at constant velocity. Hydrodynamic interactions are captured by a particle-based mesoscopic simulation method. At vanishing relative velocity, the equilibrium repulsive force-distance curve is obtained. At large drag velocities, in contrast, we find an apparent attractive force for departing colloids along the dragging direction. The deformation, in the close encounter of colloids, and the energy dissipation are examined as a function of the drag velocity and their separation.     

Colloids on free-standing smectic films

We study the structure of a free-standing smectic-A film around a micron-size polystyrene colloid adsorbed onto the film. We find that a colloid or a cluster of colloids is surrounded by an optically distinct and radially decorated meniscus ending with a sharp edge. The observed strong and finite-range attraction between the adsorbed colloids is driven by the fusion of menisci. We interpret the structure of the smectic meniscus in terms of a model dominated by the surface free energy and we argue that the characteristic appearance of the meniscus is due to layer undulations.     

Microscopics of complexation between long DNA molecules and positively charged colloids

Extensive atomic force and electron microscopy reveal a new, generic DNA-colloid complex with a fixed number of DNA bases per colloid. The fiber shaped complex is stable in the presence of excess colloids in the solution. As more DNA is added to the solution and the ratio between colloids and DNA approaches the fiber's stoichiometry, the system undergoes a sharp coagulation transition. The system is restabilized at even higher DNA concentrations through localization of small colloid clusters on extensive DNA networks.     

Solvent effects on the linear and nonlinear optical response of silver nanoparticles

Linear and nonlinear (NL) optical properties of silver colloids stabilized with poly(N-vinylpyrrolidone) (PVP) in water, acetone, methanol, and ethylene glycol were studied. Images obtained by transmission electron microscopy reveal narrow size distributions of silver nanoparticles (NPs) with diameters centered at ≈ 6.3 nm (aqueous colloid) and in the 4.3–4.9 nm range for the other colloids. The behavior of the surface plasmon resonance band associated with the NPs was monitored through the linear absorption spectrum, and its dependence on the linear refraction index and the electric dipole moment (EDM) of the solvent molecules was analyzed. The phenomenological parameter, A, obtained from the linear absorption spectra, includes contributions due to the surface effects and the solvent. The third order susceptibility of the colloid was measured using the Z-scan technique at 532 nm, and the NL optical susceptibility of the NPs was determined using the Maxwell–Garnett model. The results indicate that the NL response of the colloids is largely influenced by the molecules adsorbed on the NPs surfaces and the EDM of the solvent molecules. PACS  42.65.-k; 42.65.An; 73.20.Mf; 78.67.-n; 78.67.Bf; 82.70.Dd     

Characterization of laser-ablated and chemically reduced silver colloids in aqueous solution by UV/VIS spectroscopy and STM/SEM microscopy

Silver colloids in aqueous solution were studied by different scanning microscopy techniques and UV/VIS spectroscopy. The silver colloids were produced either by chemical reduction or by nanosecond laser ablation from a solid silver foil in water. Variation of laser power and ablation time leads to solutions of metal clusters of different sizes in water. We characterized the electronic absorption of the clusters by UV/VIS spectroscopy. STM (scanning tunneling microscope) imaging of the metal colloids shows atomic resolution of rod- or tenon-like silver clusters up to 10-nm length formed by laser ablation. Our scanning electron microscope measurements, however, show that much larger silver colloids up to 5-μm length are also formed, which are not visible in the STM due to their roughness. We correlate them with the long-wavelength tail of the multimodal UV/VIS spectrum. The silver colloids obtained by chemical reduction are generally larger and their electronic spectra are red-shifted compared to the laser-ablated clusters. Irradiation of the colloid solution with nanosecond laser pulses of appropriate fluence at 532 nm and 355 nm initially reduced the colloid size. Longer irradiation at 355 nm, however, leads to the formation of larger colloids again. There seems to be a critical lower particle size, where silver clusters in aqueous solution become unstable and start to coagulate. Received: 24 June 2002 / Revised version: 25 July 2002 / Published online: 25 October 2002 RID="*" ID="*"This work is part of the thesis of H. M?ltgen RID="**" ID="**"Corresponding author. Fax: +49-211/811-5195, E-mail: kleinermanns@uni-duesseldorf.de     

Influence of surface affinity of planar walls on effective interaction between the wall and colloids

Using density functional theory, we investigate the effective interaction between a big colloid immersed in a sea of small colloids and a wall which has different affinity to the small colloids. Steele 10-4-3 potential is introduced to mimic both short-range repulsive and long-range attractive interactions between the wall and the small colloids. It is found that the surface affinity of the wall has a significant influence on the effective interaction. In the short-range repulsive case, the repulsion greatly enhances the big colloid-wall effective attraction, which sensitively depends on the concentration of small colloids, and is not sensitive to the repulsive strength. In the long-range attractive case, both the concentration of small colloids and the attractive strength have great effect on the effective interaction, and with an increase of the attractive strength, a strong repulsion may be induced when the big colloid is close to the wall. In low density limit of small colloids, the present results agree well with those of the Asakura and Oosawa(AO) approximation.     

Electric-field-induced polarization of the layer of condensed ions on cylindrical colloids

In concentrated suspensions of charged colloids, interactions between colloids can be induced by an external electric field through the polarization of charge distributions (within the diffusive double layer and the layer of condensed ions) and/or electro-osmotic flow. In case of rod-like colloids, these field-induced inter-colloidal interactions have recently been shown to lead to anomalous orientation perpendicular to the external field, and to phase/state transitions and dynamical states, depending on the field amplitude and frequency of the external field. As a first step towards a (semi-) quantitative understanding of these phenomena, we present a linear-response analysis of the frequency-dependent polarization of the layer of condensed ions on a single, long and thin cylindrical colloid. The in-phase and out-phase response functions for the charge distribution and the electric potential are calculated for arbitrary orientation of the cylindrical colloid. The frequency-dependent degree of alignment, which is proportional to the electric-field-induced birefringence, is calculated as well, and compared to experiments on dilute fd virus suspensions.     

Microscopic relationship between colloid–colloid interactions and the rheological behaviour of suspensions: a molecular dynamics-stochastic rotation dynamics investigation

ABSTRACT

We investigate the dependence of the shear viscosity of suspensions of spherical colloids as a function of the volume fraction of the suspension, the colloid–colloid interactions and the shear rate. We couple molecular dynamics to describe the motion of the colloids with stochastic rotation dynamics (MD–SRD) for the fluid environment by means of stochastic collisions, in order to incorporate hydrodynamics effects leading to non-newtonian responses. The shear viscosity is computed using non-equilibrium simulations by imposing explicit velocity gradients. The impact of the colloid–colloid interactions is examined by modelling the inter-colloid pair potential with a repulsive power law, that allows interpolating different degrees of colloidal softness. The general rheological behaviour of our suspensions can be described with a Krieger–Dougherty like equation, which must be corrected to account for the variations in the maximum packing fraction and non-equilibrium effects arising from the flux of momentum imposed to the suspension, which appear when varying the softness of the inter-colloidal interactions. We further show evidence for non-newtonian behaviour at high Péclet numbers, characterised both by shear thinning and shear thickening, and thus demonstrate these effects can be successfully captured using MD–SRD methods.     

Can nanoscale surface charge heterogeneity really explain colloid detachment from primary minima upon reduction of solution ionic strength?

This study theoretically examined colloid detachment from primary minima with ionic strength (IS) reduction on heterogeneous collector surfaces. The chemically and physically heterogeneous collector surfaces were modeled as a planar surface carrying nanoscale patches of different zeta potentials and nanoscale pillars/hemispheroids, respectively. The surface element integration technique was used to calculate interaction energies between colloid and collector surfaces. Two boundary conditions for the double-layer interaction energy were considered, namely constant surface potential (CSP), and linear superposition approximation (LSA). In contrast to prevailing opinions in the literature, our results show that colloids attached on the chemically heterogeneous surface cannot be detached by IS reduction under CSP condition due to an increase of the adhesive force/torque with decreasing IS. Detachment from chemically heterogeneous surfaces by IS reduction can occur under LSA condition only when the flow velocity is very high. In contrast, the presence of nanoscale physical heterogeneity can cause colloid detachment from primary minima by IS reduction under both CSP and LSA conditions at flow velocities commonly used in experimental studies because of a significant reduction in the adhesive forces/torques.     

Cellular solid behaviour of liquid crystal colloids 1. Phase separation and morphology

We study the phase ordering colloids suspended in a thermotropic nematic liquid crystal below the clearing point and the resulting aggregated structure. Small () PMMA particles are dispersed in a classical liquid crystal matrix, 5CB or MBBA. With the help of confocal microscopy we show that small colloid particles densely aggregate on thin interfaces surrounding large volumes of clean nematic liquid, thus forming an open cellular structure, with the characteristic size of inversely proportional to the colloid concentration. A simple theoretical model, based on the Landau mean-field treatment, is developed to describe the continuous phase separation and the mechanism of cellular structure formation. Received 13 March 2000 and Received in final form 6 June 2000     

应用银溶胶膜探测水中抗生素的表面增强拉曼光谱研究

以自组装法制备的银溶胶膜为表面增强拉曼散射活性基底实现了对水中抗生素的痕量检测。采用微波加热法制备银溶胶,自组装法制备银溶胶膜。通过改变银溶胶的pH值及镀膜的次数,研究其对抗生素增强效果的影响。实验发现,采用不同pH值的银溶胶镀膜所获得的银溶胶膜的增强效果有很大差异,当银溶胶pH=4,且镀膜次数为五次时,增强效果最佳。以此银溶胶膜为基底对三种抗生素(氯霉素、环丙沙星、恩诺沙星)进行了SERS检测,可以检测到的最低浓度分别为120,15,120 nmol·L-1。结果表明,利用改进方法制备的银溶胶膜,可以对水中抗生素进行痕量检测,为实现养殖水中残留抗生素的检测提供了方法。     

Phase behaviour of a dispersion of charge-stabilised colloidal spheres with added non-adsorbing interacting polymer chains

We present a theory for the phase behaviour of mixtures of charge-stabilised colloidal spheres plus interacting polymer chains in good and θ -solvents within the framework of free-volume theory. We use simple but accurate combination rules for the depletion thickness around a colloidal particle and for the osmotic pressure up to the semi-dilute concentration regime. Hence, we obtain expressions for the free energy for mixtures of charged colloidal particles and non-adsorbing interacting polymers. From that, we calculate the phase behaviour, and discuss its topology in dependence on the competition between the charge-induced repulsion and the polymer-induced attraction. The homogeneous mixture of colloids and polymers becomes more stabilised against demixing when increasing the electrostatic repulsion. This charge-induced stabilisation is strongest for small polymer-to-colloid size ratios and is more pronounced for charged colloids mixed with polymers in a good solvent than for polymers in a θ -solvent. For the weakly charged regime we find that the phase diagram becomes salt-concentration-independent in the protein limit for charged colloids plus polymers in a θ -solvent. The liquid window, i.e., the concentration regimes where a colloidal liquid exists, is narrowed down upon increasing the charge-induced repulsion. Also this effect is more pronounced when charged colloids are mixed with polymer chains in a good solvent. In summary, we demonstrate that the solvent quality significantly influences the phase behaviour of mixtures of charged colloids plus non-adsorbing polymers if the range of the screened electrostatic repulsion becomes of the order of the range of the depletion-induced attraction.     

Dielectrophoresis of nanocolloids: A molecular dynamics study

Dielectrophoresis (DEP), the motion of polarizable particles in non-uniform electric fields, has become an important tool for the transport, separation, and characterization of microparticles in biomedical and nanoelectronics research. In this article we present, to our knowledge, the first molecular dynamics simulations of DEP of nanometer-sized colloidal particles. We introduce a simplified model for a polarizable nanoparticle, consisting of a large charged macroion and oppositely charged microions, in an explicit solvent. The model is then used to study DEP motion of the particle at different combinations of temperature and electric field strength. In accord with linear response theory, the particle drift velocities are shown to be proportional to the DEP force. Analysis of the colloid DEP mobility shows a clear time dependence, demonstrating the variation of friction under non-equilibrium. The time dependence of the mobility further results in an apparent weak variation of the DEP displacements with temperature.     

Monitoring the buckling threshold of drying colloidal droplets using water-ethanol mixtures

We visualize the drying of droplets of colloids suspended in a mixture of two miscible solvents, namely water and ethanol. After a period of isotropic shrinkage, droplets suddenly buckle like elastic shells. For a fixed colloid solid fraction, the buckling threshold evolves as a function of ethanol content, due to changes of the solvent mixture physical properties, such as viscosity and evaporation rate. A simplified model predicting the qualitative behavior of the buckling threshold as a function of the initial ethanol mass fraction has been developed that fits well experimental results.     

Treatment of bcc transition metals on a modified CGW model

The vibrational spectrum and specific heat of three bcc transition metals -iron, chromium and tungsten are computed on the basis of modified Clark-Gazis-Wallis angular force model which considers volume forces of Krebs' nature. The calculations are made using the Blackman's root sampling technique for a discrete subdivision in wave-vector space. The calculated lattice specific heats and the effective Debye temperatures are compared with the available experimental data. The results show a reasonably satisfactory agreement with the experimental observations.The authors are highly thankful to Dr.Jyoti Prakash, Dr. S.Chandra for helpful discussions. One of them (H. L. K.) is thankful to C. S. I. R. India for the award of J. R. F. The computational facilities received from the I. I. T. Kanpur are also acknowledged.     

软凝聚态物质物理学

软物质是指其某种物理性质在小的外力作用下能产生很大变化的凝聚态物,典型的例子包括液晶、高分子体系、胶体、微乳液等。软物质的结构和性质主要不是由内能,而是由熵来决定,较通俗地介绍了软物质的概念,仔细分析了熵在软物质中所起的作用,同时详细介绍了聚合物体系、胶体及生物膜等几种典型的软物质,通过硫化橡胶和无管虹吸等十分有趣的例子。说明了聚合物对流变性质的影响;通过分析硬球胶体的相变及相分离等行为说明了熵力的概念;仔细分仔了电稳定胶体的相互作用,并介绍了DLVO理论以及近年来发现的对这一理论的偏离,特别是约束条件下同号带电胶球的长程吸引相互作用及其对此现象的一些解释;对生物膜也作了初步介绍。人们对软物质的研究和理解目前还处于一个非常原始的阶段,深入研究和理解软物质的各种性质必将促进人类对自然和人类自身的认识。