Journal of Physical Chemistry B, Vol.106, No.48, 12483-12490, 2002
A quantum chemical model for electric field induced electron transfer at metal electrodes. Application to halide oxidation on Cu(100)
A model based on the use of ab initio quantum chemical explicitly correlated wave functions is proposed to study the electronic transfer reaction between an adsorbate and a metallic electrode. In this model, the effects of the electrode potential are simulated through the application of a uniform external electric field. This field exerts an influence on the relative stability of the two electronic states that are mainly involved in the electron transfer. These electronic states have the transferred electron localized either in the electrode or in the adsorbate. The model has been applied to the electron transfer between halides and a cluster model representation of the Cu(100) single-crystal electrode. A linear correlation between the electric field intensity at which the two electronic states involved in the charge-transfer process become degenerate and the normal reduction electrode potential is found. The existence of this linear correlation indicates that the proposed model contains the essential physics governing the trend of halide oxidation at a metal electrode.