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• W1993486421 abstract "By exciting cyclohexene in the gas phase at 200 nm and probing it by nonresonant multiphoton ionization with mass-selective detection of the ion yields, we found four time constants τi (20, 47, 43, 350 fs). Whereas deuteration lengthens τ2 by a factor of 1.4, the other constants do not change. τ1−τ3 represent traveling times through observation windows on excited surfaces, whereas τ4 reflects a process in the hot ground state. We assign τ1 (20 fs) to departure from the Franck−Condon regions of the Rydberg and ππ* states, which are both populated at 200 nm, and τ2 (47 fs) to traveling along the ππ* surface and suggest that a [1,3]-sigmatropic H shift begins in this state. This rationalizes the deuterium effect on τ2. To explain why this window is followed by a process not subject to a D effect, we postulate that the ππ* surface is crossed late (i.e., at low energy) by the zwitterionic state Z and that formation of a carbene (the known photochemical product, cyclopentylcarbene) begins there. The corresponding 1,2-shift of a CC bond is then (within τ4 = 350 fs) largely reversed on the ground-state surface, while a smaller part of the carbene forms products such as methylenecyclopentane within the same time. Carbene formation is probably accompanied by some cis−trans isomerization. The wavelength dependence of carbene formation is attributed to a memory for the initially excited state, based on momentum conservation. The processes are most likely typical of simple olefins. The fragmentation pattern showed that butadiene is not formed until at least 500 ps. The retro-Diels−Alder reaction, known to take place in the ground state, thus only occurs later." @default.
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• W1993486421 date "2001-06-26" @default.
• W1993486421 modified "2023-09-26" @default.
• W1993486421 title "Ultrafast Dynamics of Cyclohexene and Cyclohexene-<i>d</i>₁₀ Excited at 200 nm" @default.
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• W1993486421 doi "https://doi.org/10.1021/ja004115e" @default.
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