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By Caldeira A.O., Leggert A.J.
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10), and we will try to use the equivalent of the compensation between the kinetic energy and the nuclear attraction (T and -Z/r) found in the atomic case. In fact, it turns out that the compensation between the kinetic energy and the nuclear attraction does lead to a qualitative description of the optimum orbitals in molecular systems, but only in the frame of the following restrictive conditions. i) Global versus local description. In the case of molecular systems, the one electron part of the electronic hamiltonian includes a sum over the electron-nuclear attraction of all the nuclei: Therefore it appears that the above mentionned compensation takes place separatly in the vicinity of each atom.
9) that the s wave of the optimum orbital is also very close to the genuine 1s orbital of the H atom. 4% in all the considered range of r. A similar conclusion cannot be reached concerning the p waves (l = 1). (22)) is not small here and correspondingly the p wave of the molecular system cannot be expected to THEORY OF ORBITAL OPTIMIZATION IN SCF AND MCSF CALCULATIONS 33 be close of any atomic-like orbital. 2. OPTIMISATION IN THE ASYMPTOTIC REGION When expanding the orbital in partial waves with origin at the midpoint of the molecule (center of charge of the molecule-minus-one-electron) the p wave vanishes, and only the s wave has to be considered.
Of the orbitals resulting from SCF calculations or from MCSCF calculations involving a valence CI : we do not present here a new formal development (although some formalism is necessary), nor a new computational method, nor an actual calculation of an observable quantity ... but merely the description of the orbitals. In fact, it turns out that the orbitals resulting from SCF or valence MCSCF calculations in molecules can be described in extremely simple terms by comparing them with the RHF orbitals of the separated atoms.
Influence of Damping on Quantum Interference: An exactly Soluble Model by Caldeira A.O., Leggert A.J.
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