An electronic structure theory has been developed for an inelastic electric current of electron-intramolecular vibration coupling origin in terms of the Keldysh Green function method and the self-consistent Born approximation. Numerical calculations were made for the benzenedithiol molecule linking the two Au(111) electrodes. The calculations successfully reproduce typical features commonly observed in inelastic tunneling spectroscopy. The vibrational excitation energy due to the inelastic current was estimated. The inelastic electric current is quite important for the structural stability and the switching possibility of the molecular device.

• Received 7 April 2004

DOI:https://doi.org/10.1103/PhysRevLett.93.246102