title: Non-adiabatic molecular dynamics investigation of photoionization state formation and lifetime in Mn²⁺-doped ZnO quantum dots.
abstract: The unique electronic structure of Mn(2+)-doped ZnO quantum dots gives rise to photoionization states that can be used to manipulate the magnetic state of the material and to generate zero-reabsorption luminescence. Fast formation and long non-radiative decay of this photoionization state is a necessary requirement for these important applications. In this work, surface hopping based non-adiabatic molecular dynamics are used to demonstrate the fast formation of a metal-to-ligand charge transfer state in a Mn(2+)-doped ZnO quantum dot. The formation occurs on an ultrafast timescale and is aided by the large density of states and significant mixing of the dopant Mn(2+) 3dt2 levels with the valence-band levels of the ZnO lattice. The non-radiative lifetime of the photoionization states is also investigated.
authors.affiliation: Department of Chemistry, University of Washington, Seattle, Washington, USA. li@chem.washington.edu.
authors.forename: Sean A
authors.initials: SA
authors.lastname: Fischer
authors.forename: David B
authors.initials: DB
authors.lastname: Lingerfelt
authors.forename: Joseph W
authors.initials: JW
authors.lastname: May
authors.forename: Xiaosong
authors.initials: X
authors.lastname: Li
mesh_terms: D003198:Computer Simulation; D004735:Energy Transfer; D007477:Ions / Q000737:chemistry / Q000528:radiation effects; D008027:Light; D008345:Manganese / Q000737:chemistry* / Q000528:radiation effects; D008956:Models, Chemical; D056004:Molecular Dynamics Simulation; D045663:Quantum Dots; D011829:Radiation Dosage; D015034:Zinc Oxide / Q000737:chemistry* / Q000528:radiation effects
chemical_list: D007477:Ions; D008345:Manganese; D015034:Zinc Oxide