By Ian W. M. Smith
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Additional info for Kinetics and Dynamics of Elementary Gas Reactions
The former implies the existence of a potential well on the reaction hypersurface and the survival of a single 'supermolecule' for a time comparable with a rotational period, the latter does not. 3. Surfaces representing three different types of potential in triatomic systems: (a) the potential between a stable molecule BC and an inert-gas atom plotted as a function of r and r , the distance from A to the centre-of-mass of BC; the dashed line represents the path of minimum energy, and shows how the repulsive forces tend to compress the BC molecule; (b) here AB and BC are (identical) stable molecules but there is a potential-energy barrier to the reaction A + BC AB + C; (c) here ABC, as well as AB and BC, is stable so there is a deep 'weir at the symmetrical configuration.
The next step in improving the 'trial' wavefunction merges the M O and VB treatments. 10). 18) B where the 'primes' denote scaled wavefunctions and λ as well as ζ, the scaling factor, is optimized according to the variational principle. 1 show, this procedure leads to a further improvement in the estimates of D and r . This improvement has a straightforward physical explanation. Since the electrons repel one another they will tend not to be found close together (for the moment, we speak as if the electrons are identifiable particles).
Furthermore, one should resist any tendency to assume that the transition state for an atom-transfer reaction always has the three atoms participating most directly in the process in a straight line. In practice, increasing use is being made of qualitative theoretical arguments, overlaid with some empiricism, to predict the geometry of transition states. The arguments that are used follow the lead given by Walsh's famous s t u d i e s on small, stable, polyatomic molecules; examples are given in later chapters.