Heat transfer between nanoparticles: Thermal conductance for near-field interactions

We analyze the heat transfer between two nanoparticles separated by a distance lying in the near-field domain in which energy interchange is due to the Coulomb interactions. The thermal conductance is computed by assuming that the particles have charge distributions characterized by fluctuating multipole moments in equilibrium with heat baths at two different temperatures. This quantity follows from the fluctuation-dissipation theorem for the fluctuations of the multipolar moments. We compare the behavior of the conductance as a function of the distance between the particles with the result obtained by means of molecular dynamics simulations. The formalism proposed enables us to provide a comprehensive explanation of the marked growth of the conductance when decreasing the distance between the nanoparticles.

Long-range-interactions induced ordered structures in deposition processes

We present a new model of sequential adsorption in which the adsorbing particles experience dipolar interactions. We show that in the presence of these long-range interactions, highly ordered structures in the adsorbed layer may be induced at low temperatures. The new phenomenology is manifest through significant variations of the pair correlation function and the jamming limit, with respect to the case of noninteracting particles. Our study could be relevant in understanding the adsorption of magnetic colloidal particles in the presence of a magnetic field.

Molecular dynamics study of orientational cooperativity in water

Recent experiments on liquid water show collective dipole orientation fluctuations dramatically slower than expected (with relaxation time >tation, the self-dipole randomization time tr, which is an upper limit on ta; we find that tr5ta. Third, to check if there are correlated domains of dipoles in water which have large relaxation times compared to the individual dipoles, we calculate the randomization time tbox of the site-dipole field, the net dipole moment formed by a set of molecules belonging to a box of edge Lbox. We find that the site-dipole randomization time tbox2.5ta for Lbox3 , i.e., it is shorter than the same quantity calculated for the self-dipole. Finally, we find that the orientational correlation length is short even at low T.

Dimerization of polyacetylene treated as a spin-Peierls distortion of the Heisenberg Hamiltonian

Extracting a bond-length-dependent Heisenberg-like Hamiltonian from the potential-energy surfaces of the two lowest states of ethylene, it is possible to study the geometry of polyacetylene by minimization of the cohesive energy, using both variational-cluster and Rayleigh-Schrödinger perturbative expansions. The dimerization amplitude is satisfactorily reproduced. Optimizing the variational-cluster-expansion total energy with the equal-bond-length constraint, the barrier to reversal of alternation is obtained. The alternating-to-regular phase transition is treated from the Néel-state starting function and appears to be of second order.

Valence-bond treatment of distortions in polyacene polymers

Distortions of polyacene polymers are studied within a many-body valence-bond framework using a powerful transfer-matrix technique for the valence-bond (or Heisenberg) model of the system. The computations suggest that the ground-state geometry is either totally symmetric or possibly exhibits a slight (A2 or B2 symmetry) bond-alternation distortion. The lowest-energy (nonsymmetric, in-plane) distortions are the A2 and B2 modes, which, within our approximations, are degenerate.

Colloidal assembly on magnetically vibrated stripes

We investigate the collective organization of paramagnetic colloidal particles externally driven above the periodic stripes of a uniaxial ferrimagnetic garnet film. An external field modulation induces vibration of the stripe walls and produces random motion of the particles. Defects in the stripe pattern break the symmetry of the potential and favor particle nucleation into large clusters above a critical density. Mismatch between particle size and pattern wavelength generates assemblies with different morphological order. At even higher field strengths, repulsive dipolar interactions between the particles induce cluster melting. We propose a novel approach to generate and externally control a variety of colloidal assemblies.

Quasi-two-dimensional electrodeposition under forced fluid flow

Experimental quasi-two-dimensional Zn electrodeposits are grown under forced convection conditions. Large-scale effects, with preferential growth towards the impinging flow, together with small-scale roughness suppression effects are evidenced and separately analyzed by using two different radial cell configurations. Interpretations are given in terms of primary concepts concerning current and concentration distributions.

Nonequilibrium orientational patterns in two-component Langmuir monolayers

A model of a phase-separating two-component Langmuir monolayer in the presence of a photoinduced reaction interconverting two components is formulated. An interplay between phase separation, orientational ordering, and reaction is found to lead to a variety of nonequilibrium self-organized patterns, both stationary and traveling. Examples of the patterns, observed in numerical simulations, include flowing droplets, traveling stripes, wave sources, and vortex defects.

Further insights on dynamic morphological transitions in quasi-two-dimensional electrodeposition

Dynamic morphological transitions in thin-layer electrodeposits obtained from copper sulphate solutions have been studied. The chemical composition of the electrodeposits indicates that they appear as a consequence of the competition between copper and cuprous oxide formation. In addition, the Ohmic control of the process is verified at initial stages of the deposit growth. At higher deposit developments, gravity-induced convection currents play a role in the control of the whole process and affect the position of these transitions.

Actively maintained lipid nanodomains in biomembranes

Lipid rafts, defined as domains rich in cholesterol and sphingolipids, are involved in many important plasma membrane functions. Recent studies suggest that the way cells handle membrane cholesterol is fundamental in the formation of such lateral heterogeneities. We propose to model the plasma membrane as a nonequilibrium phase-separating system where cholesterol is dynamically incorporated and released. The model shows how cellular regulation of membrane cholesterol may determine the nanoscale lipid organization when the lipid mixture is close to a phase separation boundary, providing a plausible mechanism for raft formation in vivo.

Nonequilibrium patterns and shape fluctuations in reactive membranes

A simple kinetic model of a two-component deformable and reactive bilayer is presented. The two differently shaped components are interconverted by a nonequilibrium reaction, and a phenomenological coupling between local composition and curvature is proposed. When the two components are not miscible, linear stability analysis predicts, and numerical simulations show, the formation of stationary nonequilibrium composition/curvature patterns whose typical size is determined by the reactive process. For miscible components, a linearization of the dynamic equations is performed in order to evaluate the correlation function for shape fluctuations from which the behavior of these systems in micropipet aspiration experiments can be predicted.

Generation of dynamic structures in nonequilibrium reactive membranes

We present a nonequlibrium approach for the study of a flexible bilayer whose two components induce distinct curvatures. In turn, the two components are interconverted by an externally promoted reaction. Phase separation of the two species in the surface results in the growth of domains characterized by different local composition and curvature modulations. This domain growth is limited by the effective mixing due to the interconversion reaction, leading to a finite characteristic domain size. In addition to these effects, first introduced in our earlier work [ Phys. Rev. E 71 051906 (2005)], the important new feature is the assumption that the reactive process actively affects the local curvature of the bilayer. Specifically, we suggest that a force energetically activated by external sources causes a modification of the shape of the membrane at the reaction site. Our results show the appearance of a rich and robust dynamical phenomenology that includes the generation of traveling and/or oscillatory patterns. Linear stability analysis, amplitude equations, and numerical simulations of the model kinetic equations confirm the occurrence of these spatiotemporal behaviors in nonequilibrium reactive bilayers.

Performance of correlation functionals in ab initio chemisorption cluster-model calculations: Alkali metals on Si(111)

The performance of different correlation functionals has been tested for alkali metals, Li to Cs, interacting with cluster models simulating different active sites of the Si(111) surface. In all cases, the ab initio Hartree-Fock density has been obtained and used as a starting point. The electronic correlation energy is then introduced as an a posteriori correction to the Hartree-Fock energy using different correlation functionals. By making use of the ionic nature of the interaction and of different dissociation limits we have been able to prove that all functionals tested introduce the right correlation energy, although to a different extent. Hence, correlation functionals appear as an effective and easy way to introduce electronic correlation in the ab initio Hartree-Fock description of the chemisorption bond in complex systems where conventional configuration interaction techniques cannot be used. However, the calculated energies may differ by some tens of eV. Therefore, these methods can be employed to get a qualitative idea of how important correlation effects are, but they have some limitations if accurate binding energies are to be obtained.