Theory of Dissipative Electron Transfer of a Molecule at the Interface

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  • Tsukada Masaru
    Department of Nano-Science and Nano-Technology, Advanced School of Science and Engineering, Waseda University WPI—Advanced Institute for Materials Research, Tohoku University
  • Mitsutake Kunihiro
    Frontier Research Center, Canon Inc.

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Dissipating electron transfer processes between the electrodes and a molecule due to the coupling to the external degrees of freedom are theoretically analyzed. Important information is shown to be included in the energy loss spectral function, which is expressed formally in the same form for the two cases of the coupling with the molecular vibration and with the electro-magnetic environment. Magnitude of zero-bias anomaly, i.e., suppression of the conductance around zero bias region is given by the integrated function of the energy loss spectral function and the reduction ratio at the zero bias is obtained by the Debye–Waller type factor. For the case of coupling to the molecular vibration, the first-principles DFT method is applied for the calculation of the energy loss spectral function. A crucial role of the energy loss spectral function for determining the net current and the average charge of the molecule is discussed in the dissipating electron transfer regime. The relation of the present theory with the Marcus theory is discussed.

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