Snapshots of Light Induced Accumulation of Two Charges on Methylviologen using a Sequential Nanosecond Pump-Pump Photoexcitation.

Methylviologen (MV2+) is perhaps the most used component as a reversible electron acceptor in photophysical studies. While MV2+ is most commonly implicated as a reversible one-electron mediator, its electrochemical properties clearly evidence two successive one-electron reduction processes. In this report, we have investigated on the light driven two-charge accumulation on MV2+ using a multicomponent system composed of the prototypical molecular photosensitizer [Ru(bpy)3]2+ and MV2+ in the presence of ascorbate as reversible electron donor. The sequential addition of two electrons on the methylviologen was tracked upon sequential excitation of the [Ru(bpy)3]2+ at optimized concentration of the electron acceptor. The charge accumulated state carries an energy of 0.9 eV above the ground state and has a lifetime of ca. 50 μs. We have reached a fairly good global yield of approximately 9% for the two-charge accumulation. This result clearly demonstrates the potential of this simple approach for applications in artificial photosynthesis.