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Register a new userCharge and Salt Driven Reentrant Order-Disorder and Gas-Solid Transitions in Charged Colloids
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Monte Carlo simulations have been performed for aqueous charged colloidal suspensions as a function of charge density on the particles and salt concentration. We vary the charge density in our simulations over a range where a reentrant solid-liquid transition in suspensions of silica and polymer latex particles has been reported by Yamanaka et al. [Phys. Rev. Lett. 80 5806 (1998)]. We show that at low ionic strengths a homogeneous liquid-like ordered suspension undergoes crystallization upon increasing charge density . Further increase in charge density resulted once again a disordered state which is in agreement with experimental observations. In addition to this reentrant order-disorder transition, we observe an inhomogeneous to homogeneous transition in our simulations when salt is added to the disordered inhomogeneous state. This inhomogeneous to homogeneous disordered transition is analogous to the solid-gas transition of atomic systems and has not yet been observed in charged colloids. The reported experimental observations on charged colloidal suspensions are discussed in the light of present simulation results.
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Aqueous suspensions of highly charged polystyrene particles with different volume fractions have been investigated for structural ordering and phase behavior using static light scattering (SLS) and confocal laser scanning microscope (CLSM). Under deionized conditions, suspensions of high charge density colloidal particles remained disordered whereas suspensions of relatively low charge density showed crystallization by exhibiting iridescence for the visible light. Though for unaided eye crystallized suspensions appeared homogeneous, static light scattering measurements and CLSM observations have revealed their inhomogeneous nature in the form of coexistence of voids with dense ordered regions. CLSM investigations on disordered suspensions showed their inhomogeneous nature in the form coexistence of voids with dense disordered (amorphous) regions. Our studies on highly charged colloids confirm the occurrence of gas-solid transition and are in accordance with predictions of Monte Carlo simulations using a pair-potential having a long-range attractive term [Mohanty and Tata, Journal of Colloid and Interface Science 2003, 264, 101]. Based on our experimental and simulation results we argue that the reported reentrant disordered state [Yamanaka et al Phys. Rev. Lett. 1998, 80, 5806 and Toyotama et al Langmuir, 2003, 19, 3236] in charged colloids observed at high charge densities is a gas-solid coexistence state.
The influence of hydrodynamic interactions on lane formation of oppositely charged driven colloidal suspensions is investigated using Brownian dynamics computer simulations performed on the Rotne-Prager level of the mobility tensor. Two cases are considered, namely sedimentation and electrophoresis. In the latter case the Oseen contribution to the mobility tensor is screened due to the opposite motion of counterions. The simulation results are compared to that resulting from simple Brownian dynamics where hydrodynamic interactions are neglected. For sedimentation, we find that hydrodynamic interactions strongly disfavor laning. In the steady-state of lanes, a macroscopic phase separation of lanes is observed. This is in marked contrast to the simple Brownian case where a finite size of lanes was obtained in the steady-state. For strong Coulomb interactions between the colloidal particles a lateral square lattice of oppositely driven lanes is stable similar to the simple Brownian dynamics. In an electric field, on the other hand, the behavior is found in qualitative and quantitative accordance with the case of neglected hydrodynamics.
Capillary bridges can form between colloids immersed in a two phase fluid, e.g., in a binary liquid mixture, if the surface of the colloids prefers the species other than the one favored in the bulk liquid. Here, we study the formation of liquid bridges induced by confining colloids to a slit, with the slit walls having a preference opposite to the one of the colloid surface. Using mean field theory, we show that there is a line of first-order phase transitions between the bridge and the no-bridge states, which ends at a critical point. By decreasing the slit width, this critical point is shifted towards smaller separations between the colloids. However, at very small separations, and far from criticality, we observe only a minor influence of the slit width on the location of the transition. Monte Carlo simulations of the Ising model, which mimics incompressible binary liquid mixtures, confirm the occurrence of the bridging transitions, as manifested by the appearance of bistable regions where both the bridge and the no-bridge configurations are (meta)stable. Interestingly, we find no bistability in the case of small colloids, but we observe a sharpening of the transition when the colloid size increases. In addition, we demonstrate that the capillary force acting between the colloids can depend sensitively on the slit width, and varies drastically with temperature, thus achieving strengths orders of magnitude higher than at criticality of the fluid.
The phenomenon of group motion is common in nature, ranging from the schools of fish, birds and insects, to avalanches, landslides and sand drift. If we treat objects as collectively moving particles, such phenomena can be studied from a physical point of view, and the research on many-body systems has proved that marvelous effects can arise from the simplest individuals. The motion of numerous individuals presents different dynamic phases related to the ordering of the system. However, it is usually difficult to study the dynamic ordering and their transitions through experiments. Electron bubble states formed in a two-dimensional electron gas, as a type of electron solids, can be driven by an external electric field and provide a platform to study the dynamic collective behaviors. Here, we demonstrate that noise spectrum is a powerful method to investigate the dynamics of bubble states. We observed not only the phenomena from dynamically ordered and disordered structures, but also unexpected alternations between them. Our results show that a dissipative system can convert between chaotic structures and ordered structures when tuning global parameters, which is concealed in conventional transport measurements of resistance or conductance. Moreover, charging the objects to study electrical noise spectrum in collective motions can be an additional approach to revealing dynamic ordering transitions.
The ionic composition and pair correlations in fluid phases of realistically salt-free charged colloidal sphere suspensions are calculated in the primitive model. We obtain the number densities of all ionic species in suspension, including low-molecular weight microions, and colloidal macroions with acidic surface groups, from a self-consistent solution of a coupled physicochemical set of nonlinear algebraic equations and non-mean-field liquid integral equations. Here, we study suspensions of colloidal spheres with sulfonate or silanol surface groups, suspended in demineralized water that is saturated with carbon dioxide under standard atmosphere. The only input required for our theoretical scheme are the acidic dissociation constants pKa, and effective sphere diameters of all involved ions. Our method allows for an ab initio calculation of colloidal bare and effective charges, at high numerical efficiency.
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