| Abstract
| - An algorithm for computation of density-functional-based orbital reactivity indices, such as orbitally resolvedhardness and softness tensors, total hardness and softness, and the Fukui indices, has been extended for systemswith degenerate electronic states and implemented in the deMon computer code. The method treats explicitlydegenerate orbitals, thus avoiding spurious numerical errors in hardness tensor computations. Benchmarkcalculations for a series of small molecules and some larger, highly degenerate systems reveal goodcomputational performance and numerical stability. The influence of the choice of auxiliary basis functionson the results is also examined and discussed. The predicted orbital and total reactivity index values arefound to be insensitive to the applied exchange-correlation functionals. Applications of the orbital Fukuiindices to a series of (4n + 2) π-electron [n]-annulenes show the possibility of rationalizing the reactivity ofindividual molecular orbital contributions.
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