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Ligand-localized electron trapping at sensitized semiconductor interfaces.

Paul G Hoertz1, David W Thompson, Lee A Friedman

  • 1Department of Chemistry, Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, USA.

Journal of the American Chemical Society
|August 15, 2002
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Summary

Ruthenium and osmium complexes derivatized onto mesoporous TiO2 films exhibit ultrafast electron injection and long-lived charge-separated states. These intermediates, crucial for solar energy conversion, are observable and their dynamics are characterized.

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Area of Science:

  • Materials Science
  • Photochemistry
  • Electrochemistry

Background:

  • Nanocrystalline, mesoporous titanium dioxide (TiO2) thin films are vital components in advanced material applications.
  • Ruthenium (Ru) and Osmium (Os) polypyridyl complexes are extensively studied for their photophysical properties.

Purpose of the Study:

  • To investigate the interfacial electron transfer dynamics of Ru and Os complexes derivatized onto TiO2 films.
  • To characterize the formation, lifetime, and properties of excited states and charge-separated intermediates.

Main Methods:

  • Surface derivatization of TiO2 films with specific Ru and Os complexes.
  • Electrochemical measurements to determine reduction potentials.
  • Transient absorption spectroscopy with nanosecond pulsed laser excitation to probe excited states and intermediates.
  • Quantum yield measurements at various excitation wavelengths.

Main Results:

  • Complexes [Ru(bpy)2(deebq)](PF6)2 and [Os(bpy)2(deebq)](PF6)2 bind to TiO2 with defined surface coverages.
  • Ultrafast electron injection into TiO2 is observed, followed by ligand-localized trapping.
  • Long-lived charge-separated intermediates (MII(deebq-)(bpy)2+/TiO2 and MIII(deebq)(bpy)23+/TiO2) are formed, with concentrations observable by the naked eye.
  • Quantum yield for charge-separated state formation is excitation wavelength-dependent.

Conclusions:

  • The study elucidates a mechanism involving ultrafast electron injection and subsequent trapping, leading to long-lived charge-separated states.
  • The observed intermediates and their millisecond-scale decay kinetics are critical for understanding energy conversion processes in these systems.
  • The findings provide insights into the design of efficient photoactive materials for applications like solar cells.