Femtosecond M2,3-edge spectroscopy of transition-metal oxides: Photoinduced oxidation state change in α-Fe2O3

Josh Vura-Weis, Chang Ming Jiang, Chong Liu, Hanwei Gao, J. Matthew Lucas, Frank M.F. De Groot, Peidong Yang, A. Paul Alivisatos, Stephen R. Leone

Research output: Contribution to journalArticle

Abstract

Oxidation-state-specific dynamics at the Fe M2,3-edge are measured on the sub-100 fs time scale using tabletop high-harmonic extreme ultraviolet spectroscopy. Transient absorption spectroscopy of α-Fe 2O3 thin films after 400 nm excitation reveals distinct changes in the shape and position of the 3p → valence absorption peak at ∼57 eV due to a ligand-to-metal charge transfer from O to Fe. Semiempirical ligand field multiplet calculations of the spectra of the initial Fe 3+ and photoinduced Fe2+ state confirm this assignment and exclude the alternative d-d excitation. The Fe2+ state decays to a long-lived trap state in 240 fs. This work establishes the ability of time-resolved extreme ultraviolet spectroscopy to measure ultrafast charge-transfer processes in condensed-phase systems.

Original languageEnglish (US)
Pages (from-to)3667-3671
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume4
Issue number21
DOIs
StatePublished - Nov 7 2013
Externally publishedYes

Keywords

  • X-ray
  • extreme ultraviolet"
  • hematite
  • high-harmonic generation
  • ligand-to-metal charge transfer
  • transient absorption

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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    Vura-Weis, J., Jiang, C. M., Liu, C., Gao, H., Lucas, J. M., De Groot, F. M. F., Yang, P., Alivisatos, A. P., & Leone, S. R. (2013). Femtosecond M2,3-edge spectroscopy of transition-metal oxides: Photoinduced oxidation state change in α-Fe2O3. Journal of Physical Chemistry Letters, 4(21), 3667-3671. https://doi.org/10.1021/jz401997d