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RESEARCH PRODUCT
Quantum chemical simulations of hole self-trapping in semi-ionic crystals
Eugene A. KotominPatrick W. M. JacobsLev KantorovichArvids Stashanssubject
PhysicsValence (chemistry)Wave packetIonic bondingElectronic structureTrappingCondensed Matter PhysicsAlkali metalMolecular physicsDiatomic moleculeAtomic and Molecular Physics and OpticsPhysics::Atomic and Molecular ClustersMoleculePhysical and Theoretical ChemistryAtomic physicsdescription
A novel formalism is presented for reliable calculations of the energetics of hole self-trapping in semi-ionic solids with mixed valence bands. Unlike previous model-Hamiltonian-type approaches, it is based on self-consistent quantum chemical INDO simulations of the atomistic and electronic structure of a self-trapped hole, making no a priori assumptions about a particular form of its localization (if any). This formalism is applied to the problem of hole self-trapping in corundum crystals (a -A1203). The hole self-trapping is found to be energetically favorable in the form of a diatomic 02 molecule with strong covalent bonding quite similar to the self-trapped hole (VK-center) in alkali halides. The so-called localization energy (i.e., the energy that is required to localize the Bloch-like wave packet of the free hole on the molecule, as the first stage of further trapping) is essentially less than one-half of the upper valence hand width, which is the estimate commonly used for ionic solids. 0 i994 John Wiley & Sons, Inc.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 1994-11-15 | International Journal of Quantum Chemistry |