Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 130, Issue 43, Pages 14105-+Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja805949s
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Funding
- U.S. Department of Energy [DE-FG02-01ER15282]
- Mathies Royalty Fund
- U.S. Department of Energy (DOE) [DE-FG02-01ER15282] Funding Source: U.S. Department of Energy (DOE)
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A combination of femtosecond electronic absorption and stimulated Raman spectroscopies has been employed to determine the kinetics associated with low-spin to high-spin conversion following charge-transfer excitation of a Fell spin-crossover system in solution. A time constant of T = 190 +/- 50 fs; for the formation of the 5T(2) ligand-field state was assigned based on the establishment of two isosbestic points in the ultraviolet in conjunction with changes in ligand stretching frequencies and Raman scattering amplitudes: additional dynamics observed in both the electronic and vibrational spectra further indicate that vibrational relaxation in the high-spin state occurs with a time constant of ca. 10 ps. The results set an important precedent for extremely rapid, formally forbidden (Delta S = 2) nonradiative relaxation as well as defining the time scale for intramolecular optical switching between two electronic states possessing vastly different spectroscopic, geometric, and magnetic properties.
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