Ultrafast Photooxidation of Mn(II)−Terpyridine Complexes Covalently Attached to TiO2 Nanoparticles
The Journal of Physical Chemistry C2007Vol. 111(32), pp. 11982–11990
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Sabas G. Abuabara, Clyde W. Cady, Jason B. Baxter, Charles A. Schmuttenmaer, Robert H. Crabtree, Gary W. Brudvig, Víctor S. Batista
Abstract
This paper reports visible-light sensitization of TiO2 nanoparticles by surface modification with Mn(II)−terpyridine complexes, as evidenced by UV−vis spectroscopy of colloidal thin films and aqueous suspensions. Photoexcitation of the [MnII(H2O)3(catechol-terpy)]2+/TiO2 (terpy = 2,2‘:6,2‘ ‘-terpyridine) complex, attached to the TiO2 surface, leads to interfacial electron transfer within 300 fs as indicated by ultrafast optical pump−terahertz probe transient measurements and computational simulations. Photoinduced interfacial electron transfer is accompanied by Mn(II) → Mn(III) photooxidation. The half-time for regeneration of the Mn(II) complex is ca. 23 s (at 6 K), as monitored by time-resolved measurements of the Mn(II) EPR signal.
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