By Boschke F.L.
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Extra info for Triplet States I
Example text
This is readily explained in terms of MO's. The ~1 and n2 MO's of aerolein are bonding between C2 and Ca and are therefore destabilized b y the rotation around C2Ca. On the other hand, ~2 is antibonding in that region and is stabilized. ) In the nn* triplet three electrons are destabilized (those in ~:1 and ~:3) and two are stabilized (in 7~2). The resulting net destabilization is therefore smaller than the destabilization of the 7;n* triplet, where three electrons are destabilized (in ~1 and =s) but only one is stabilized (in ~2).
In order to obtain a Energy (kcal/mole) 80 . y 96 / , , , . o , // Relaxation , T~,y 4'7 90 ~ Fig. 6. Potential energy sheets of the two lowest triplet states of s - t r a n s acrolein 153) qualitatively exact description of the actual acroleinic system, the calculated 3=~* surface has been lowered by 20 kcal/mole. The two vertical 3n~* and 8~rc* states are then nearly degenerate, as they have been found to be experimentally. The true calculated surfaces are represented in Fig. 7 (Ref. la3)). The important fact here is that these two potential energy sheets present two regions of avoided crossing.
A more efficient method of reducing S12 is to twist one of the p= orbitals through 90 ~ around the C1C2 axis. The (unconjugated) orthogonal triplet thus obtained is more stable than the (conjugated) planar triplet. These straightforward predictions have been verified by "ab-initio" calculations. 50 eV. 60 eV) 139). 19 eV 141)). The twisting potential energy curve (the CC bond length being kept constant) of the 3B3 triplet state is represented in Fig, 1 together with the 1A ground state (N) curve (closed-shell treatment with CI).