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Observation of Transient Iron(II) Formation in Dye-Sensitized Iron Oxide Nanoparticles by Time-Resolved X-ray Spectroscopy

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Jordan E. Katz†‡, Benjamin Gilbert*‡, Xiaoyi Zhang§, Klaus Attenkofer§, Roger W. Falcone† and Glenn A. Waychunas*‡

^† Department of Physics, University of California Berkeley, Berkeley, California 94720

^§ X-ray Science Division, Argonne National Laboratory, Argonne, Illinois 60439

^‡ Earth Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720

J. Phys. Chem. Lett., 2010, 1 (9), pp 1372–1376

DOI: 10.1021/jz100296r

Publication Date (Web): April 13, 2010

*To whom correspondence should be addressed. E-mail: bgilbert@lbl.gov (B.G.), gawaychunas@lbl.gov (G.A.W.).

Abstract

The reduction of ferric iron in solid phase minerals leads to the mobilization of ferrous iron in the environment and is thus a crucial component of the global iron cycle. Despite the importance of this process, a mechanistic understanding of the structural and chemical changes that are caused by this electron transfer reaction is not established because the speed of the fundamental chemical steps renders them inaccessible to conventional study. Ultrafast time-resolved X-ray spectroscopy is a technique that can overcome this limitation and measure changes in oxidation state and structure occurring during chemical reactions that can be initiated by a fast laser pulse. We use this approach with 100 ps resolution to monitor the speciation of Fe atoms in iron oxide nanoparticles following photoinduced electron transfer from a surface-bound photoactive dye molecule. These data represent the first direct real-time observation of the dynamics of ferrous ion formation and subsequent reoxidation in iron oxide.

Keywords (keywords):

electron transfer; interfaces; iron chemistry; ultrafast spectroscopy; X-ray absorption spectroscopy; nanoparticle chemistry

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This article has been cited by 1 ACS Journal articles (1 most recent appear below).

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History

Published In Issue May 06, 2010
Article ASAPApril 13, 2010
Received: March 05, 2010
Accepted: April 07, 2010

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Letter

Observation of Transient Iron(II) Formation in Dye-Sensitized Iron Oxide Nanoparticles by Time-Resolved X-ray Spectroscopy