5 research outputs found
Two-level system with a thermally fluctuating transfer matrix element: Application to the problem of DNA charge transfer
Charge transfer along the base-pair stack in DNA is modeled in terms of
thermally-assisted tunneling between adjacent base pairs. Central to our
approach is the notion that tunneling between fluctuating pairs is rate-limited
by the requirement of their optimal alignment. We focus on this aspect of the
process by modeling two adjacent base pairs in terms of a classical damped
oscillator subject to thermal fluctuations as described by a Fokker-Planck
equation. We find that the process is characterized by two time scales, a
result that is in accord with experimental findings.Comment: original file is revtex4, 10 pages, three eps figure
Tight-binding parameters for charge transfer along DNA
We systematically examine all the tight-binding parameters pertinent to
charge transfer along DNA. The molecular structure of the four DNA bases
(adenine, thymine, cytosine, and guanine) is investigated by using the linear
combination of atomic orbitals method with a recently introduced
parametrization. The HOMO and LUMO wavefunctions and energies of DNA bases are
discussed and then used for calculating the corresponding wavefunctions of the
two B-DNA base-pairs (adenine-thymine and guanine-cytosine). The obtained HOMO
and LUMO energies of the bases are in good agreement with available
experimental values. Our results are then used for estimating the complete set
of charge transfer parameters between neighboring bases and also between
successive base-pairs, considering all possible combinations between them, for
both electrons and holes. The calculated microscopic quantities can be used in
mesoscopic theoretical models of electron or hole transfer along the DNA double
helix, as they provide the necessary parameters for a tight-binding
phenomenological description based on the molecular overlap. We find that
usually the hopping parameters for holes are higher in magnitude compared to
the ones for electrons, which probably indicates that hole transport along DNA
is more favorable than electron transport. Our findings are also compared with
existing calculations from first principles.Comment: 15 pages, 3 figures, 7 table