Tracking electrons and atoms in a photoexcited metalloporphyrin by X-ray transient absorption spectroscopy

Lin X. Chen*, Xiaoyi Zhang, Erik C. Wasinger, Klaus Attenkofer, Guy Jennings, Ana Z. Muresan, Jonathan S. Lindsey

*Corresponding author for this work

Research output: Contribution to journalArticle

67 Scopus citations

Abstract

Simultaneously tracking electronic and molecular structures of a photoexcited metalloporphyrin, present for only 200 ps in a dilute solution, has been realized using X-ray transient absorption spectroscopy (XTA). Using laser pulses as excitation sources and delayed X-ray pulses as probes, we were able to identify the excited state electronic configuration of a nickel porphyrin as singly occupied 3dx2-y2 and 3dz2 molecular orbitals (MOs) with an energy gap of 2.2 eV, and energy shifts 4pz MOs to 1.5 eV higher relative to that of the ground state, and an expanded porphyrin ring characterized by lengthening of Ni-N and Ni-C bonds. Moreover, kinetic XTA signals at different X-ray photon energies demonstrate the capability for acquiring the correlation and coherence between different optically excited states with the same technique. These results provide guidance for theoretical calculations as well as insightful understanding of optically excited states that play important roles in photochemical processes.

Original languageEnglish (US)
Pages (from-to)9616-9618
Number of pages3
JournalJournal of the American Chemical Society
Volume129
Issue number31
DOIs
StatePublished - Aug 8 2007

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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