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

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

2002-10-09

arxiv.org/abs/cond-mat/0210215v1

Physics

Condensed Matter

submitted to the Proceedings of "Dynamics Days Asia-Pacific: Second International Conference on Nonlinear Science", HangZhou,

Scientific paper

10.1142/S0217979203021903

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.

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