Pump-Pump-Probe Spectroscopy of a Molecular Triad Monitoring Detrimental Processes for Photoinduced Charge Accumulation

Kuss-Petermann, Martin and Wenger, Oliver S.. (2017) Pump-Pump-Probe Spectroscopy of a Molecular Triad Monitoring Detrimental Processes for Photoinduced Charge Accumulation. Helvetica Chimica Acta, 100. e1600283.

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Official URL: https://edoc.unibas.ch/63144/

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Controlling light‐induced accumulation of electrons or holes is desirable in view of multi‐electron redox chemistry, for example for the formation of solar fuels or for photoredox catalysis in general. Excitation with multiple photons is usually required for electron or hole accumulation, and consequently pump‐pump‐probe spectroscopy becomes a valuable spectroscopic tool. In this work, we excited a triarylamine‐Ru(bpy)32+‐anthraquinone triad (bpy = 2,2′‐bipyridine) with two temporally delayed laser pulses of different color and monitored the resulting photoproducts. Absorption of the first photon by the Ru(bpy)32+ photosensitizer generated a triarylamine radical cation and an anthraquinone radical anion by intramolecular electron transfer. Subsequent selective excitation of either one of these two radical ion species then induced rapid reverse electron transfer to yield the triad in its initial (ground) state. This shows in direct manner that after absorption of a first photon and formation of the primary photoproducts, the absorption of a second photon can lead to unproductive electron transfer events that counteract further charge accumulation. In principle, this problem is avoidable by careful excitation wavelength selection in combination with good molecular design.
Faculties and Departments:05 Faculty of Science > Departement Chemie > Chemie > Anorganische Chemie (Wenger)
UniBasel Contributors:Wenger, Oliver and Kuss-Petermann, Martin
Item Type:Article, refereed
Article Subtype:Research Article
Note:Publication type according to Uni Basel Research Database: Journal article -- The final publication is available at Wiley, see DOI link
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Last Modified:11 Jun 2018 09:22
Deposited On:16 Apr 2018 07:00

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