Semiempirical Hamiltonians for spatially confined π-electron systems
✍ Scribed by J. Planelles; C. Zicovich-Wilson; W. Jaskólski; A. Corma
- Publisher
- John Wiley and Sons
- Year
- 1996
- Tongue
- English
- Weight
- 764 KB
- Volume
- 60
- Category
- Article
- ISSN
- 0020-7608
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✦ Synopsis
A study of .n-electron systems confined by impenetrable surfaces is presented. The study results in a nonempirical-based approach to obtain confinement-adapted semiempirical .n-Hamiltonians including repulsive terms (PPP or Hubbard). The impenetrable surface confinement of a physical system involves changes in the boundary conditions that the eigenvectors of its differential Hamiltonian operator have to fulfill, while the Hamiltonian itself remains unchanged. However, if this Hamiltonian is written in second quantization language, then confinement only involves changes of the Hamiltonian scalar factors (integrals). Semiempirical Hamiltonian integrals are replaced by parameters; therefore, confinement involves only changes of these parameters. It is shown that confinement changes Coulomb (a,) and exchange ( p,,), while repulsion (y,,) parameters remain unaffected. Next, the influence of confinement upon the electron correlation of (i) .n-electron molecular systems, (ii) atoms, and (iii) an electron gas is discussed. The behaviour of the correlation energy vs. the confinement size is found to be different for each type of system. A neat explanation of this variety is given in terms of the Coulomb attractive fields of the systems. Some chemical confinement effects such as an increase in the reactivity of .n-electron systems is also outlined.
📜 SIMILAR VOLUMES
A formalism is developed to obtain the energy eigenvalues of spatially confined quantum mechanical systems in the framework of the usual Ž . Ž . Wentzel᎐Kramers᎐Brillouin WKB and modified airy function MAF methods. To illustrate the working rule, the techniques are applied to three different cases,