Jahn-Teller Effect of Mn(2+) in Zinc-Blende ZnS Crystal

摘要

The excited states of Mn(2+) in zinc-blende ZnS crystal have been studied by theIntermediate Neglect of Differential Overlap model parameterized for spectroscopy (INDO/S) within the Restricted Open-Shell Hartree-Fock (ROHF)-Configuration Interaction (CI) approximation. The effect of the Jahn-Teller (JT) active e-mode on the first excited state (a(4)T1) has been examined with respect to energy barriers and geometric distortions. The dynamical JT effect has been studied and the excited state absorption (ESA) profiles for different e-mode conformations have been calculated. Good reproduction of the experimental ESA spectrum has been obtained for nuclear arrangements corresponding to small S-Mn-S angle distortions. The off-center Tau 2-mode vibrations were found to promote the JT coupling by reducing the barriers between the stable structures. jg.