Dynamical study on polaron formation in a metal/polymer/metal structure

By considering a metal/polymer/metal structure within a tight-binding one-dimensional model, we have investigated the polaron formation in the presence of an electric field. When a sufficient voltage bias is applied to one of the metal electrodes, an electron is injected into the polymer chain, then a self-trapped polaron is formed at a few hundreds of femtoseconds while it moves slowly under a weak electric field (not larger than $$ V/cm). At an electric field between $1.0\times 10^4$ V/cm and $$ V/cm, the polaron is still formed, since the injected electron is bounded between the interface barriers for quite a long time. It is shown that the electric field applied at the polymer chain reduces effectively the potential barrier in the metal/polymer interface

Holstein polarons in a strong electric field: delocalized and stretched states

The coherent dynamics of a Holstein polaron in strong electric fields is considered under different regimes. Using analytical and numerical analysis, we show that even for small hopping constant and weak electron-phonon interaction, the original discrete Wannier-Stark (WS) ladder electronic states are each replaced by a semi-continuous band if a resonance condition is satisfied between the phonon frequency and the ladder spacing. In this regime, the original localized WS states can become {\em delocalized}, yielding both `tunneling' and `stretched' polarons. The transport properties of such a system would exhibit a modulation of the phonon replicas in typical tunneling experiments. The modulation will reflect the complex spectra with nearly-fractal structure of the semi-continuous band. In the off-resonance regime, the WS ladder is strongly deformed, although the states are still localized to a degree which depends on the detuning: Both the spacing between the levels in the deformed ladder and the localization length of the resulting eigenfunctions can be adjusted by the applied electric field. We also discuss the regime beyond small hopping constant and weak coupling, and find an interesting mapping to that limit via the Lang-Firsov transformation, which allows one to extend the region of validity of the analysis.Comment: 10 pages, 13 figures, submitted to PR

Rate-equation calculations of the current flow through two-site molecular device and DNA-based junction

Here we present the calculations of incoherent current flowing through the two-site molecular device as well as the DNA-based junction within the rate-equation approach. Few interesting phenomena are discussed in detail. Structural asymmetry of two-site molecule results in rectification effect, which can be neutralized by asymmetric voltage drop at the molecule-metal contacts due to coupling asymmetry. The results received for poly(dG)-poly(dC) DNA molecule reveal the coupling- and temperature-independent saturation effect of the current at high voltages, where for short chains we establish the inverse square distance dependence. Besides, we document the shift of the conductance peak in the direction to higher voltages due to the temperature decrease.Comment: 12 pages, 6 figure

Tight-binding parameters for charge transfer along DNA

We systematically examine all the tight-binding parameters pertinent to charge transfer along DNA. The $\pi$ 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 $\pi$ 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