Mode-selective chemical processes have been widely utilized in photochemistry, photobiology or laser micromachining. Chemical reaction induced via vibrational excitation is a good candidate for mode-selective process, which enables the functional-group selective reaction. Scanning tunneling microscope is an ideal electron source for the mode-selective vibrational excitations of a single molecule through inelastic electron tunneling process. Several attempts have been made to apply such a process to the manipulation of single adsorbates, but the experimental realization of a vibrationally driven single-molecule reaction is a challenging object. Here, we report a mode-selective, molecule-to-molecule conversion by scanning tunneling microscope; a trans-2-butene to a 1,3-butadiene on palladium (110) surface, where the reaction product is chemically identified with single-molecule vibrational spectroscopy. The underlying mechanism is experimentally confirmed as a multiple vibrational excitation of a single adsorbed molecule via inelastic electron tunneling process. |