Experimental assessment of dynamic structural parameters for homogeneous and interfacial charge-transfer reactions

case studies based on time-dependent Raman scattering methods

Stephen K. Doorn, Robert L. Blackbourn, Christopher S. Johnson, Joseph T Hupp

Research output: Contribution to journalArticle

47 Citations (Scopus)

Abstract

The application of time-dependent scattering methodologies to dynamic structural problems involving charge transfer reactions is described. We show experimentally that a time-dependent analysis of resonance-enhanced Raman scattering can lead to a complete mode-by-mode description of the vibrational structural changes accompanying charge transfer and, therefore, a complete description of the vibrational activation barrier to charge transfer. (In other words, all force constants, all mode displacements, all bond-length displacements, and all individual energy components of the barrier can be determined.) The strategy is illustrated with case studies of internal (metal-to-ligand) charge transfer, ligand-bridged metal-to-metal charge transfer, outer-sphere charge transfer, and interfacial charge transfer.

Original languageEnglish
Pages (from-to)1767-1774
Number of pages8
JournalElectrochimica Acta
Volume36
Issue number11-12
DOIs
Publication statusPublished - 1991

Fingerprint

Structural dynamics
Charge transfer
Raman scattering
Metals
Ligands
Bond length
Chemical activation
Scattering

Keywords

  • charge transfer
  • electron transfer
  • Raman scattering

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Analytical Chemistry
  • Electrochemistry

Cite this

Experimental assessment of dynamic structural parameters for homogeneous and interfacial charge-transfer reactions : case studies based on time-dependent Raman scattering methods. / Doorn, Stephen K.; Blackbourn, Robert L.; Johnson, Christopher S.; Hupp, Joseph T.

In: Electrochimica Acta, Vol. 36, No. 11-12, 1991, p. 1767-1774.

Research output: Contribution to journalArticle

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AB - The application of time-dependent scattering methodologies to dynamic structural problems involving charge transfer reactions is described. We show experimentally that a time-dependent analysis of resonance-enhanced Raman scattering can lead to a complete mode-by-mode description of the vibrational structural changes accompanying charge transfer and, therefore, a complete description of the vibrational activation barrier to charge transfer. (In other words, all force constants, all mode displacements, all bond-length displacements, and all individual energy components of the barrier can be determined.) The strategy is illustrated with case studies of internal (metal-to-ligand) charge transfer, ligand-bridged metal-to-metal charge transfer, outer-sphere charge transfer, and interfacial charge transfer.

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