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Register a new userCharging-driven coarsening and melting of a colloidal nanoparticle monolayer at an ionic liquid-vacuum interface
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We induce and investigate the coarsening and melting dynamics of an initially static nanoparticle colloidal monolayer at an ionic liquid-vacuum interface, driven by a focused, scanning electron beam. Coarsening occurs through grain interface migration and larger-scale motions such as grain rotations, often facilitated by sliding dislocations. The progressive decrease in area fraction that drives melting of the monolayer is explained using an electrowetting model whereby particles at the interface are solvated once their accumulating charge recruits sufficient counterions to subsume the particle. Subject to stochastic particle removal from the monolayer, melting is recapitulated in simulations with a Lennard-Jones potential. This new driving mechanism for colloidal systems, whose dynamical timescales we show can be controlled with the accelerating voltage, opens the possibility to manipulate particle interactions dynamically without need to vary particle intrinsic properties or surface treatments. Furthermore, the decrease in particle size availed by electron imaging presents opportunities to observe force and time scales in a lesser-explored regime intermediate between typical colloidal and molecular systems.
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We simulate colloids (radius $R sim 1mu$m) trapped at the interface between a cholesteric liquid crystal and an immiscible oil, at which the helical order (pitch p) in the bulk conflicts with the orientation induced at the interface, stabilizing an ordered array of disclinations. For weak anchoring strength W of the director field at the colloidal surface, this creates a template, favoring particle positions eitheron top of or midway between defect lines, depending on $alpha = R/p$. For small $alpha$, optical microscopy experiments confirm this picture, but for larger $alpha$ no templating is seen. This may stem from the emergence at moderate W of a rugged energy landscape associated with defect reconnections.
We propose a simple scaling theory describing the variation of the mean first passage time (MFPT) $tau(N,M)$ of a regular block copolymer of chain length $N$ and block size $M$ which is dragged through a selective liquid-liquid interface by an external field $B$. The theory predicts a non-Arrhenian $tau$ vs. $B$ relationship which depends strongly on the size of the blocks, $M$, and rather weakly on the total polymer length, $N$. The overall behavior is strongly influenced by the degree of selectivity between the two solvents $chi$. The variation of $tau(N,M)$ with $N$ and $M$ in the regimes of weak and strong selectivity of the interface is also studied by means of computer simulations using a dynamic Monte Carlo coarse-grained model. Good qualitative agreement with theoretical predictions is found. The MFPT distribution is found to be well described by a $Gamma$ - distribution. Transition dynamics of ring- and telechelic polymers is also examined and compared to that of the linear chains. The strong sensitivity of the ``capture time $tau(N,M)$ with respect to block length $M$ suggests a possible application as a new type of chromatography designed to separate and purify complex mixtures with different block sizes of the individual macromolecules.
The ordering of nanoparticles into predetermined configurations is of importance to the design of advanced technologies. In this work, we moderate the surface anchoring against the bulk elasticity of liquid crystals to dynamically shape nanoparticle assemblies at a fluid interface. By tuning the degree of nanoparticle hydrophobicity with surfactants that alter the molecular anchoring of liquid crystals, we pattern nanoparticles at the interface of cholesteric liquid crystal emulsions. Adjusting the particle hydrophobicity more finely further modifies the rigidity of assemblies. We establish that patterns are tunable by varying both surfactant and chiral dopant concentrations. Since particle assembly occurs at the interface with the desired structures exposed to the surrounding phase, we demonstrate that particles can be readily crosslinked and manipulated, forming structures that retain their shape under external perturbations. This study establishes the templating of nanomaterials into reconfigurable arrangements. Interfacial assembly is tempered by elastic patterns that arise from the geometric frustration of confined cholesterics. This work serves as a basis for creating materials with chemical heterogeneity and with linear, periodic structures, essential for optical and energy applications.
Recently it was shown that the WAC model for liquid silica [L. V. Woodcock, C. A. Angell, and P. Cheeseman, J. Chem. Phys. 65, 1565 (1976)] is remarkably close to having a liquid-liquid critical point (LLCP). We demonstrate that increasing the ion charge separates the global maxima of the response functions, while reducing the charge smoothly merges them into a LLCP; a phenomenon that might be experimentally observable with charged colloids. An analysis of the Si and O coordination numbers suggests that a sufficiently low Si/O coordination number ratio is needed to attain a LLCP.
Deformations of liquid interfaces by the optical radiation pressure of a focused laser wave were generally expected to display similar behavior, whatever the direction of propagation of the incident beam. Recent experiments showed that the invariance of interface deformations with respect to the direction of propagation of the incident wave is broken at high laser intensities. In the case of a beam propagating from the liquid of smaller refractive index to that of larger one, the interface remains stable, forming a nipple-like shape, while for the opposite direction of propagation, an instability occurs, leading to a long needle-like deformation emitting micro-droplets. While an analytical model successfully predicts the equilibrium shape of weakly deformed interface, very few work has been accomplished in the regime of large interface deformations. In this work, we use the Boundary Integral Element Method (BIEM) to compute the evolution of the shape of a fluid-fluid interface under the effect of a continuous laser wave, and we compare our numerical simulations to experimental data in the regime of large deformations for both upward and downward beam propagation. We confirm the invariance breakdown observed experimentally and find good agreement between predicted and experimental interface hump heights below the instability threshold.
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