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We extend the simple and efficient lowest order expansion (LOE) for inelasticelectron tunneling spectroscopy (IETS) to include variations in the electronicstructure on the scale of the vibration energies. This enables first-principlescalculations of IETS lineshapes for molecular junctions close to resonances andband edges. We demonstrate how this is relevant for the interpretation ofexperimental IETS using both a simple model and atomistic first-principlessimulations.

Efficient calculation of inelastic vibration signals in electron transport: Beyond the wide-band approximation