Statistics and kinetics of single-molecule electron transfer dynamics in complex environments: A simulation model study

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Electron Transport in Dye-Sensitized Solar Cells Based on ZnO Nanotubes: Evidence for Highly Efficient Charge Collection and Exceptionally Rapid Dynamics

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

The energy landscape for solvent dynamics in electron transfer reactions: A minimalist model

Energy fluctuations of a solute molecule embedded in a polar solvent are investigated to depict the energy landscape for solvation dynamics. The system is modeled by a charged molecule surrounded by two layers of solvent dipolar molecules with simple rotational dynamics. Individual solvent molecules are treated as simple dipoles that can point toward or away from the central charge (Ising spins). Single-spin-flip Monte Carlo kinetics simulations are carried out in a two-dimensional lattice for different central charges, radii of outer shell, and temperatures. By analyzing the density of states as a function of energy and temperatures, we have determined the existence of multiple freezing transitions. Each of them can be associated with the freezing of a different layer of the solvent. (C) 2002 American Institute of Physics.

Single molecule electron transfer dynamics in complex environments

We propose a new theoretical approach to study the kinetics of the electron transfer (ET) under the dynamical influence of the complex environments with the first passage times (FPT) of the reaction events. By measuring the mean and high order moments of FPT and their ratios, the full kinetics of ET, especially the dynamical transitions across different temperature zones, is revealed. The potential applications of the current results to single molecule electron transfer are discussed.

Smooth landscape solvent dynamics in electron transfer reactions

Solvent effects play a major role in controlling electron-transfer reactions. The solvent dynamics happens on a very high-dimensional surface, and this complex landscape is populated by a large number of minima. A critical problem is to understand the conditions under which the solvent dynamics can be represented by a single collective reaction coordinate. When this unidimensional representation is valid, one recovers the successful Marcus theory. In this study the approach used in a previous work [V. B. P. Leite and J. N. Onuchic; J. Phys. Chem. 100, 7680 (1996)] is extended to treat a more realistic solvent model, which includes energy correlation. The dynamics takes place in a smooth and well behaved landscape. The single shell of solvent molecules around a cavity is described by a two-dimensional system with periodic boundary conditions with nearest neighbor interaction. It is shown how the polarization-dependent effects can be inferred. The existence of phase transitions depends on a factor y proportional to the contribution from the two parameters of the model. For the present model, γ suggests the existence of weak kinetic phase transitions, which are used in the analysis of solvent effects in charge-transfer reactions. © 1999 American Institute of Physics.

On the interaction of bovine serum albumin with ionic surfactants: Temperature induced EPR changes of a maleimide nitroxide reflect local protein dynamics and probe solvent accessibility

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

Effect of electron magnetic trapping in a plasma immersion ion implantation system

In this work we describe a two-dimensional computer simulation of magnetic field enhanced plasma immersion implantation system. Negative bias voltage of 10.0 kV is applied to a cylindrical target located on the axis of a grounded vacuum chamber filled with uniform nitrogen plasma. A pair of external coils creates a static magnetic field with main vector component along the axial direction. Thus, a system of crossed ExB field is generated inside the vessel forcing plasma electrons to rotate in azimuthal direction. In addition, the axial variation of the magnetic field intensity produces magnetic mirror effect that enables axial particle confinement. It is found that high-density plasma regions are formed around the target due to intense background gas ionization by the trapped electrons. Effect of the magnetic field on the sheath dynamics and the implantation current density of the PIII system is investigated. By changing the magnetic field axial profile (varying coils separation) an enhancement of about 30% of the retained dose can be achieved. The results of the simulation show that the magnetic mirror configuration brings additional benefits to the PIII process, permitting more precise control of the implanted dose.

Histological study of the dynamics in epidermis regeneration of the carp tail fin (Cyprinus carpio, Linnaeus, 1758)

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)

Culture-dependent and culture-independent characterization of microorganisms associated with Aedes aegypti (Diptera: Culicidae) (L.) and dynamics of bacterial colonization in the midgut

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

Daily dynamics of photosynthesis of the freshwater red alga Sirodotia delicatula (Batrachospermales, Rhodophyta)

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Atomic radiative transitions in thermo field dynamics

In this work we rederive the Lamb-Retherford energy shift for an atomic electron in the presence of a thermal radiation. Using the Dalibard, Dupont-Roc and Cohen-Tannoudji (DDC) formalism, where physical observables are expressed as convolutions of suitable statistical functions, we construct the electromagnetic field propagator of thermo field dynamics in the Coulomb gauge in order to investigate finite temperature effects on the atomic energy levels. In the same context, we also analyze the problem of the ground state stability.

LATTICE-DYNAMICS OF ALKALI-METALS IN A 3-BODY INTERACTION

The original model of Das et al. is modified in extending the electron-ion interaction on a three-body forces and including the crystal equilibrium condition to reduce one independent parameter. We studied the phonon dispersion relations along the three principal symmetry directions i.e. [xi, 0, 0], [xi, xi, 0] and [xi, xi, xi] and theta-T curves of alkali metals, Na, K, Rb, Cs and Li. There is close agreement between the computed results and the experimental observations.

Lattice dynamics of noble metals on effective three-body interaction

Quite recently we modified the original model of Sarkar et al. for cubic metals in extending the ion-ion interaction, ion-electron interaction and the introduction of crystal equilibrium condition. We applied our scheme to alkali metals. We studied here the lattice dynamics of noble metals on our approach by calculating phonon dispersion relations along the three principal symmetry directions, [ξ00], [ξξ00] and [ξξξ] and the (θ-T) curves of three noble metals: copper, silver and gold. We obtained reasonable agreement with the experimental findings.

Lattice dynamics of metallic glass Ca70Mg30 on the model of Bhatia and Singh

The lattice dynamical studies of the metallic glass Ca70Mg30 by Bhatia and Singh on their model contained two shortcomings, firstly the electron-ion interaction matrix was wrong and secondly, the numerical value of the bulk modulus of the electron gas was accepted arbitrarily. By modifying the electron-ion dynamical matrix and determining all the model parameters from the experimental data, we made a fresh study of the lattice dynamics of Ca70Mg30 and compared it to the earlier studies of Bhatia and Singh and also with experimental phonons.

Dynamics of a collapsing and exploding Bose-Einstein condensed vortex state

The dynamics of small repulsive Bose-Einstein condensed vortex states of 85Rb atoms in a cylindrical traps with low angular momentum was studied. The time-dependent mean-field Gross-Pitaevskii equation was used for the study. The condensates collapsed and atoms ejected via explosion and a remnant condensate with a smaller number of atoms emerges that survived for a long time.