Extended Near-Infrared Resonance Raman Investigations of an Organic Mixed-Valence System: Diazatetracyclodiene Radical Cation

Resonance Raman scattering studies in the extended near-infrared region show that six modes are coupled to the intramolecular charge-transfer transition in the mixed-valence radical cation diazatetracyclodiene. Spectral analysis based on time-dependent scattering theories shows that all six modes ma...

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Published in:	The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Vol. 103; no. 50; pp. 11172 - 11180
Main Authors:	Williams, Robert D, Hupp, Joseph T, Ramm, Michael T, Nelsen, Stephen F
Format:	Journal Article
Language:	English
Published:	United States American Chemical Society 16-12-1999
Subjects:	40 CHEMISTRY CATIONS ELECTRON TRANSFER NEAR INFRARED RADIATION RADICALS RAMAN SPECTROSCOPY RESONANCE SCATTERING VALENCE
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Abstract	Resonance Raman scattering studies in the extended near-infrared region show that six modes are coupled to the intramolecular charge-transfer transition in the mixed-valence radical cation diazatetracyclodiene. Spectral analysis based on time-dependent scattering theories shows that all six modes make substantial contributions to the vibrational reorganization energy. Measured Raman scattering cross sections were found to be considerably less than would be predicted by the conventional time-dependent scattering theories utilized here, evidently owing to complications arising from avoided surface crossings and anharmonic wave packet propagation. An examination of the classical and nonclassical kinetic effects of the coupled modes indicated that a considerable influence on the rate of intramolecular electron transfer is exerted by the modes collectively.
AbstractList	Resonance Raman scattering studies in the extended near-infrared region show that six modes are coupled to the intramolecular charge-transfer transition in the mixed-valence radical cation diazatetracyclodiene. Spectral analysis based on time-dependent scattering theories shows that all six modes make substantial contributions to the vibrational reorganization energy. Measured Raman scattering cross sections were found to be considerably less than would be predicted by the conventional time-dependent scattering theories utilized here, evidently owing to complications arising from avoided surface crossings and anharmonic wave packet propagation. An examination of the classical and nonclassical kinetic effects of the coupled modes indicated that a considerable influence on the rate of intramolecular electron transfer is exerted by the modes collectively. Mixed valence compounds are those possessing two redox centers where the centers nominally exist in different formal charge states. If the centers are compositionally identical (apart from charge), then a degenerate electron exchange can occur, with the rate of exchange governed by vibrational and solvational Franck-Condon effects, together with electronic or nuclear dynamical effects. Alternatively, if the centers are very strongly interacting, in an electronic sense, then the available odd valence electron(s) are intrinsically delocalized, the redox-center charges are identical, and the oxidation states are best characterized as fractional. Resonance Raman scattering studies in the extended near-infrared region show that six modes are coupled to the intramolecular charge-transfer transition in the mixed-valence radical cation diazatetracyclodiene. Spectral analysis based on time-dependent scattering theories shows that all six modes make substantial contributions to the vibrational reorganization energy. Measured Raman scattering cross sections were found to be considerably less than would be predicted by the conventional time-dependent scattering theories utilized here, evidently owing to complications arising from avoided surface crossings and anharmonic wave packet propagation. An examination of the classical and nonclassical kinetic effects of the coupled modes indicated that a considerable influence on the rate of intramolecular electron transfer is exerted by the modes collectively.
Author	Nelsen, Stephen F Williams, Robert D Ramm, Michael T Hupp, Joseph T
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Snippet	Resonance Raman scattering studies in the extended near-infrared region show that six modes are coupled to the intramolecular charge-transfer transition in the... Mixed valence compounds are those possessing two redox centers where the centers nominally exist in different formal charge states. If the centers are...
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SubjectTerms	40 CHEMISTRY CATIONS ELECTRON TRANSFER NEAR INFRARED RADIATION RADICALS RAMAN SPECTROSCOPY RESONANCE SCATTERING VALENCE
Title	Extended Near-Infrared Resonance Raman Investigations of an Organic Mixed-Valence System: Diazatetracyclodiene Radical Cation
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