Journal
PHYSICAL REVIEW B
Volume 63, Issue 24, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.63.241104
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The rapid internal conversion to the lowest lying 2(1)A(g)(-) state following photoexcitation is studied in all-trans-beta -carotene with unprecedented time resolution. Visible optical pulses with time duration of 7 fs are used to resonantly excite and probe the optical dynamics of the molecule dissolved in solution. A picture for the relaxation dynamics during the first 100 fs following photoexcitation is proposed based on time-resolved transmission difference spectra and kinetics. Coherent nuclear motion is observed, assigned to impulsive stimulated resonant Raman scattering. Thermalization of the 2(1)A(g)(-) state, evident from excited-state spectral evolution, is rather slow, indicating that the higher lying vibrational levels are populated during energy transfer within the photosynthetic systems.
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