A Nonlinear Dynamical Model for Ultrafast Catalytic Transfer of Electrons at Zero Temperature

The complex amplitudes of the electronic wavefunctions on different sites are used as Kramers variables for describing Electron Transfer. The strong coupling of the electronic charge to the many nuclei, ions, dipoles, etc, of the environment, is modeled as a thermal bath better considered classically. After elimination of the bath variables, the electron dynamics is described by a discrete nonlinear Schrodinger equation with norm preserving dissipative terms and Langevin random noises (at finite temperature). The standard Marcus results are recovered far from the inversion point, where atomic thermal fluctuations adiabatically induce the electron transfer. Close to the inversion point, in the non-adiabatic regime, electron transfer may become ultrafast (and selective) at low temperature essentially because of the nonlinearities, when these are appropriately tuned. We demonstrate and illustrate numerically that a weak coupling of the donor site with an extra appropriately tuned (catalytic) site, can trigger an ultrafast electron transfer to the acceptor site at zero degree Kelvin, while in the absence of this catalytic site no transfer would occur at all (the new concept of Targeted Transfer initially developed for discrete breathers is applied to polarons in our theory). Among other applications, this theory should be relevant for describing the ultrafast electron transfer observed in the photosynthetic reaction centers of living cells.Comment: submitted to the Proceedings of "Dynamics Days Asia-Pacific: Second International Conference on Nonlinear Science", HangZhou, China, August 8-12, 200

Energy thresholds for discrete breathers

Discrete breathers are time-periodic, spatially localized solutions of the equations of motion for a system of classical degrees of freedom interacting on a lattice. An important issue, not only from a theoretical point of view but also for their experimental detection, are their energy properties. We considerably enlarge the scenario of possible energy properties presented by Flach, Kladko, and MacKay [Phys. Rev. Lett. 78, 1207 (1997)]. Breather energies have a positive lower bound if the lattice dimension is greater than or equal to a certain critical value d_c. We show that d_c can generically be greater than two for a large class of Hamiltonian systems. Furthermore, examples are provided for systems where discrete breathers exist but do not emerge from the bifurcation of a band edge plane wave. Some of these systems support breathers of arbitrarily low energy in any spatial dimension.Comment: 4 pages, 4 figure

Discrete Nonlinear Schr{\"o}dinger Breathers in a Phonon Bath

We study the dynamics of the discrete nonlinear Schr{\"o}dinger lattice initialized such that a very long transitory period of time in which standard Boltzmann statistics is insufficient is reached. Our study of the nonlinear system locked in this {\em non-Gibbsian} state focuses on the dynamics of discrete breathers (also called intrinsic localized modes). It is found that part of the energy spontaneously condenses into several discrete breathers. Although these discrete breathers are extremely long lived, their total number is found to decrease as the evolution progresses. Even though the total number of discrete breathers decreases we report the surprising observation that the energy content in the discrete breather population increases. We interpret these observations in the perspective of discrete breather creation and annihilation and find that the death of a discrete breather cause effective energy transfer to a spatially nearby discrete breather. It is found that the concepts of a multi-frequency discrete breather and of internal modes is crucial for this process. Finally, we find that the existence of a discrete breather tends to soften the lattice in its immediate neighborhood, resulting in high amplitude thermal fluctuation close to an existing discrete breather. This in turn nucleates discrete breather creation close to a already existing discrete breather

On inward motion of the magnetopause preceding a substorm

Magnetopause inward motion preceding magnetic storms observed by means of OGO-E magnetomete

Transition to Chaos in a Shell Model of Turbulence

We study a shell model for the energy cascade in three dimensional turbulence at varying the coefficients of the non-linear terms in such a way that the fundamental symmetries of Navier-Stokes are conserved. When a control parameter $\epsilon$ related to the strength of backward energy transfer is enough small, the dynamical system has a stable fixed point corresponding to the Kolmogorov scaling. This point becomes unstable at $\epsilon=0.3843...$ where a stable limit cycle appears via a Hopf bifurcation. By using the bi-orthogonal decomposition, the transition to chaos is shown to follow the Ruelle-Takens scenario. For $\epsilon > 0.3953..$ the dynamical evolution is intermittent with a positive Lyapunov exponent. In this regime, there exists a strange attractor which remains close to the Kolmogorov (now unstable) fixed point, and a local scaling invariance which can be described via a intermittent one-dimensional map.Comment: 16 pages, Tex, 20 figures available as hard cop

Absence of Wavepacket Diffusion in Disordered Nonlinear Systems

We study the spreading of an initially localized wavepacket in two nonlinear chains (discrete nonlinear Schroedinger and quartic Klein-Gordon) with disorder. Previous studies suggest that there are many initial conditions such that the second moment of the norm and energy density distributions diverge as a function of time. We find that the participation number of a wavepacket does not diverge simultaneously. We prove this result analytically for norm-conserving models and strong enough nonlinearity. After long times the dynamical state consists of a distribution of nondecaying yet interacting normal modes. The Fourier spectrum shows quasiperiodic dynamics. Assuming this result holds for any initially localized wavepacket, a limit profile for the norm/energy distribution with infinite second moment should exist in all cases which rules out the possibility of slow energy diffusion (subdiffusion). This limit profile could be a quasiperiodic solution (KAM torus)

Multi-peaked localized states of DNLS in one and two dimensions

Multi-peaked localized stationary solutions of the discrete nonlinear Schrodinger (DNLS) equation are presented in one (1D) and two (2D) dimensions. These are excited states of the discrete spectrum and correspond to multi-breather solutions. A simple, very fast, and efficient numerical method, suggested by Aubry, has been used for their calculation. The method involves no diagonalization, but just iterations of a map, starting from trivial solutions of the anti-continuous limit. Approximate analytical expressions are presented and compared with the numerical results. The linear stability of the calculated stationary states is discussed and the structure of the linear stability spectrum is analytically obtained for relatively large values of nonlinearity.Comment: 34 pages, 12 figure

The Exact Ground State of the Frenkel-Kontorova Model with Repeated Parabolic Potential: I. Basic Results

The problem of finding the exact energies and configurations for the Frenkel-Kontorova model consisting of particles in one dimension connected to their nearest-neighbors by springs and placed in a periodic potential consisting of segments from parabolas of identical (positive) curvature but arbitrary height and spacing, is reduced to that of minimizing a certain convex function defined on a finite simplex.Comment: 12 RevTeX pages, using AMS-Fonts (amssym.tex,amssym.def), 6 Postscript figures, accepted by Phys. Rev.