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In scanning tunneling microscopy (STM) experiments of molecules on insulatingfilms, tunneling through molecular resonances implies transiently charging themolecule. The transition back to the charge ground state by tunneling throughthe insulating film is crucial, for example, for understanding STM-inducedelectroluminescence. Here, using STM, we report on the charge-state lifetimesof individual molecules adsorbed on NaCl films of different thicknesses onCu(111) and Au(111). To that end, we approached the tip to the molecule atresonant tunnel conditions up to a regime where charge transport was limited bytunneling through the NaCl film. The resulting saturation of tunnel current isa direct measure of the molecule's charge-state lifetime, thus providing ameans to study charge dynamics and, thereby, exciton dynamics. Comparison ofanion and cation lifetimes on different substrates reveals the critical role ofthe level alignment with the insulator's conduction and valence band, and themetal-insulator interface state.

Charge-state lifetimes of single molecules on ultrathin insulating films