Quantum-state-resolved probing of molecular inner-sphere reorganization using a single-molecule transistor

The coupling of electron transport through a single molecule to various degrees of freedom, such as spin, charge, and vibrations, can be probed using a single molecule transistor. The addition or subtraction of electrons usually accompanies a change in molecular geometry, a phenomenon known as inner-sphere reorganization. We have studied the effects of inner-sphere reorganization on electron transport using two complexes, ferrocene and Fe(bpy)$_{3}^{n+}$ (n = 1, 2, 3), as model systems. The reported energies of vibrational excitations in Fe(bpy)$_{3}^{n+}${\-} are in agreement with existing IR and Raman spectroscopic data.