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U.S. Department of Energy
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Photochemistry of metalloporphyrins

Technical Report ·
OSTI ID:6188754

During the current period our efforts have been focussed on the characterization of porphyrin radical cations, anions, and excited states, and of oxo-metal prophyrins, using resonance Raman (RR) spectroscopy. RR spectra of octaethyl porphyrin and tetraphenylporphyrin radical cations showed different frequency shift patterns, which were interpreted in terms of the expected behavior of a{sub 1u} and a{sub 2u} radicals. Anomalously polarized RR bands were discovered whose frequencies and isotope shifts differed greatly from those of the neutral parents, and which signalled pseudo-Jahn-Teller activity in A{sub 2g} modes which mix the A{sub 1u} and A{sub 2u} ground and low-lying excited states. The RR spectrum of the ZnTPP radical anion showed modest frequency downshifts in Jahn-Teller (J-T) active B{sub 1g} and B{sub 2g} modes, but no significant polarized scattering from these modes, indicating that the J-T effect is dynamic in character. Manganyl porphyrins were found to have anomalously low metal-oxo stretching frequencies, and the weakness of the bond was related to electronic properties of the d{sup 3} Mn(IV) ion and its interactions with the porphyrin orbitals. Vanadyl porphyrins were used to assess the influence of solvents and axial ligands and of the effects of porphyrin radical cation formation on the metal-oxo bond. 13 refs.

Research Organization:
Princeton Univ., NJ (USA). Dept. of Chemistry
Sponsoring Organization:
DOE; USDOE, Washington, DC (USA)
DOE Contract Number:
FG02-88ER13876
OSTI ID:
6188754
Report Number(s):
DOE/ER/13876-1; ON: DE91009136
Country of Publication:
United States
Language:
English