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Reaction dynamics of photochromic dithienylethene derivates
J. Ern, A. T. Bens, H.-D. Martin, S. Mukamel, D. Schmid, S. Tretiak,
E. Tsiper and C. Kryschi
Department of Chemistry, University of Rochester, Rochester, NY 14627
The reaction dynamics of the photochromic ring-opening reaction of
1,2-bis (5-formyl-2-methyl-thien-3-yl) perfluoro-cyclopentene
(CHO-BMTFP) in dichloromethane solution was investigated using
femtosecond transient absorption spectroscopy. The data were analyzed
in terms of a model potential and single-electron density matrices,
which were calculated using the collective electronic oscillator (CEO)
approach and the INDO/S semiempirical Hamiltonian. The S0-S1 and
S0-S2 transitions of the closed isomer were resonantly excited using
120 fs pump pulses at 610 and 410 nm, respectively. A temporally
delayed white light continuum probe pulse monitors the decay of the S1
or S2 state as well as the recovery of the S0 state. Within the first
picosecond after excitation, CHO-BMTFP was observed to undergo a fast
structural relaxation along the S1 potential energy surface into a
minimum constituting a precursor of the ring-opening process. The
rather long lifetime of the precursor, t(2) = 13 ps, was consistent
with the calculated potential barrier in front of the conical
intersection with the S0 potential energy surface, which may arise
from stabilization of the nearly planar closed isomer by an
efficiently delocalized p-electron system.
246 , 115 (1999)
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