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Register a new userPattern formation on the surface of cationic-anionic cylindrical aggregates
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Charged pattern formation on the surfaces of self--assembled cylindrical micelles formed from oppositely charged heterogeneous molecules such as cationic and anionic peptide amphiphiles is investigated. The net incompatibility $chi$ among different components results in the formation of segregated domains, whose growth is inhibited by electrostatics. The transition to striped phases proceeds through an intermediate structure governed by fluctuations, followed by states with various lamellar orientations, which depend on cylinder radius $R_c$ and $chi$. We analyze the specific heat, susceptibility $S(q^*)$, domain size $Lambda=2pi/q^*$ and morphology as a function of $R_c$ and $chi$.
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Electrostatics plays a key role in biomolecular assembly. Oppositely charged biomolecules, for instance, can co-assembled into functional units, such as DNA and histone proteins into nucleosomes and actin-binding protein complexes into cytoskeleton components, at appropriate ionic conditions. These cationic-anionic co-assemblies often have surface charge heterogeneities that result from the delicate balance between electrostatics and packing constraints. Despite their importance, the precise role of surface charge heterogeneities in the organization of cationic-anionic co-assemblies is not well understood. We show here that co-assemblies with charge heterogeneities strongly interact through polarization of the domains. We find that this leads to symmetry breaking, which is important for functional capabilities, and structural changes, which is crucial in the organization of co-assemblies. We determine the range and strength of the attraction as a function of the competition between the steric and hydrophobic constraints and electrostatic interactions.
Energy density limitations of layered oxides with different Ni contents, i.e., of the conventional cathode materials in Li-ion batteries, are investigated across the first discharge cycle using advanced spectroscopy and state-of-the-art diffraction. For the first time unambiguous experimental evidence is provided, that redox reactions in NCMs proceed via a reversible oxidation of Ni and a hybridization with O, and not, as widely assumed, via pure cationic or more recently discussed, pure anionic redox processes. Once Ni-O hybrid states are formed, the sites cannot be further oxidized. Instead, irreversible reactions set in which lead to a structural collapse and thus, the lack of ionic Ni limits the reversible capacity. Moreover, the degree of hybridization, which varies with the Ni content, triggers the electronic structure and the operation potential of the cathodes. With an increasing amount of Ni, the covalent character of the materials increases and the potential decreases.
The surface pattern formation on a gelation surface is analyzed using an effective surface roughness. The spontaneous surface deformation on DiMethylAcrylAmide (DMAA) gelation surface is controlled by temperature, initiator concentration, and ambient oxygen. The effective surface roughness is defined using 2-dimensional photo data to characterize the surface deformation. Parameter dependence of the effective surface roughness is systematically investigated. We find that decrease of ambient oxygen, increase of initiator concentration, and high temperature tend to suppress the surface deformation in almost similar manner. That trend allows us to collapse all the data to a unified master curve. As a result, we finally obtain an empirical scaling form of the effective surface roughness. This scaling is useful to control the degree of surface patterning. However, the actual dynamics of this pattern formation is not still uncovered.
We develop continuum theory of self-assembly and pattern formation in metallic microparticles immersed in a poorly conducting liquid in DC electric field. The theory is formulated in terms of two conservation laws for the densities of immobile particles (precipitate) and bouncing particles (gas) coupled to the Navier-Stokes equation for the liquid. This theory successfully reproduces correct topology of the phase diagram and primary patterns observed in the experiment [Sapozhnikov et al, Phys. Rev. Lett. v. 90, 114301 (2003)]: static crystals and honeycombs and dynamic pulsating rings and rotating multi-petal vortices.
Using grand canonical Monte Carlo simulations, we have explored the phenomenon of capillary condensation (CC) of Ar at the triple temperature inside infinitely long, cylindrical pores. Pores of radius R= 1 nm, 1.7 nm and 2.5 nm have been investigated, using a gas-surface interaction potential parameterized by the well-depth D of the gas on a planar surface made of the same material as that comprising the porous host. For strongly attractive situations, i.e., large D, one or more (depending on R) Ar layers adsorb successively before liquid fills the pore. For very small values of D, in contrast, negligible adsorption occurs at any pressure P below saturated vapor pressure P0; above saturation, there eventually occurs a threshold value of P at which the coverage jumps from empty to full, nearly discontinuously. Hysteresis is found to occur in the simulation data whenever abrupt CC occurs, i.e. for R>= 1.7 nm, and for small D when R=1nm. Then, the pore-emptying branch of the adsorption isotherm exhibits larger N than the pore-filling branch, as is known from many experiments and simulation studies. The relation between CC and wetting on planar surfaces is discussed in terms of a threshold value of D, which is about one-half of the value found for the wetting threshold on a planar surface. This finding is consistent with a simple thermodynamic model of the wetting transition developed previously.
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