13 research outputs found
Theory of bound polarons in oxide compounds
We present a multilateral theoretical study of bound polarons in oxide
compounds MgO and \alpha-Al_2O_3 (corundum). A continuum theory at arbitrary
electron-phonon coupling is used for calculation of the energies of thermal
dissociation, photoionization (optically induced release of an electron (hole)
from the ground self-consistent state), as well as optical absorption to the
non-relaxed excited states. Unlike the case of free strong-coupling polarons,
where the ratio \kappa of the photoionization energy to the thermal
dissociation energy was shown to be always equal to 3, here this ratio depends
on the Froehlich coupling constant \alpha and the screened Coulomb interaction
strength \beta. Reasonable variation of these two parameters has demonstrated
that the magnitude of \kappa remains usually in the narrow interval from 1 to
2.5. This is in agreement with atomistic calculations and experimental data for
hole O^- polarons bound to the cation vacancy in MgO. The thermal dissociation
energy for the ground self-consistent state and the energy of the optically
induced charge transfer process (hops of a hole between O^{2-} ions) have been
calculated using the quantum-chemical method INDO. Results obtained within the
two approaches for hole O polarons bound by the cation vacancies (V^-) in
MgO and by the Mg^{2+} impurity (V_{Mg}) in corundum are compared to
experimental data and to each other. We discuss a surprising closeness of the
results obtained on the basis of independent models and their agreement with
experiment.Comment: 13 pages, 2 figures, 2 tables, E-mail addresses:
[email protected], [email protected]