We have carried out first-principles molecular dynamics simulations of Al deposition on tris (8-hydroxyquinoline) aluminum ðAlq 3 Þ layers to investigate atomic geometries and electronic properties of Al=Alq 3 interfaces. Al atoms were ejected to Alq 3 one by one with the kinetic energy of 37.4 kJ/mol, which approximately corresponds to the average kinetic energy of Al at the boiling temperature of metal Al. The first Al atom interacts with two of the three O atoms of meridional Alq 3 . Following Al atoms interact with Alq 3 rather weakly and they tend to aggregate each other to form Al clusters. During the deposition process, Alq 3 was not broken and its molecular structure remained essentially intact. At the interface, weak bonds between deposited Al atoms and N and C atoms were formed. The projected density of states (PDOS) onto the Alq 3 molecular orbitals shows gap states in between the highest occupied molecular orbitals (HOMOs) and the lowest unoccupied molecular orbitals (LUMOs), which were experimentally observed by ultraviolet photoelectron spectroscopy (UPS) and metastable atom electron spectroscopy (MAES). Our results show that even though the Alq 3 molecular structure is retained, weak N-Al and C-Al bonds induce gap states. r