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Register a new userAngular Independent Photonic Pigments via the Controlled Micellization of Amphiphilic Bottlebrush Block Copolymers
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Photonic materials with angular independent structural colour are highly desirable because they offer the broad viewing angles required for application as colorants in paints, cosmetics, textiles or displays. However, they are challenging to fabricate as they require isotropic nanoscale architectures with only short-range correlation. In this article, porous microparticles with such a structure are produced in a single, scalable step from an amphiphilic bottlebrush block copolymer. This is achieved by exploiting a novel controlled micellization self-assembly mechanism within emulsified toluene-in-water droplets. By restricting water permeation through the droplet interface, the size of the pores can be precisely addressed, resulting in structurally coloured pigments. Furthermore, the reflected colour can be tuned to reflect across the full visible spectrum using only a single polymer (Mn = 290 kDa) by altering the initial emulsification conditions. Such photonic pigments have several key advantages over their crystalline analogues, as they provide isotropic structural coloration that suppresses iridescence and improves colour purity without the need for either refractive index matching or the inclusion of a broadband absorber.
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We report on the structural properties of mixed aggregates made from rare-earth inorganic nanoparticles (radius 20 Angstroms) and polyelectrolyte-neutral block copolymers in aqueous solutions. Using scattering experiments and Monte Carlo simulations, we show that these mixed aggregates have a hierarchical core-shell microstructure. The core is made of densely packed nanoparticles and it is surrounded by a corona of neutral chains. This microstructure results from a process of controlled association and confers to the hybrid aggregates a remarkable colloidal stability.
We present a simple model to study micellization of amphiphiles condensed on a rodlike polyion. Although the mean field theory leads to a first order micellization transition for sufficiently strong hydrophobic interactions, the simulations show that no such thermodynamic phase transition exists. Instead, the correlations between the condensed amphiphiles can result in a structure formation very similar to micelles.
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.
We investigate self-avoiding walk models of linear block copolymers adsorbed at a surface and desorbed by the action of a force. We rigorously establish the dependence of the free energy on the adsorption and force parameters, and the form of the phase diagram for several cases, including $AB$-diblock copolymers and $ABA$-triblock copolymers, pulled from an end vertex and from the central vertex. Our interest in block copolymers is partly motivated by the occurrence of a novel mixed phase in a directed walk model of diblock copolymers cite{Iliev} and we believe that this paper is the first rigorous treatment of a self-avoiding walk model of the situation.
The self-assembly of amphiphilic molecules usually takes place in a liquid phase, near room temperature. Here, using small angle X-ray scattering (SAXS) experiments performed in real time, we show that freezing of aqueous solutions of copolymer amphiphilic molecules can induce self-assembly below 0{deg}C.
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