Plasma interactions determine the composition in pulsed laser deposited thin films

Plasma chemistry and scattering strongly affect the congruent, elemental transfer during pulsed laser deposition of target metal species in an oxygen atmosphere. Studying the plasma properties of La_0.6Sr_0.4MnO₃, we demonstrate for as grown La_0.6Sr_0.4MnO_3-δ films that a congruent transfer of metallic species is achieved in two pressure windows: ∼10⁻³ mbar and ∼2 × 10⁻¹ mbar. In the intermediate pressure range, La_0.6Sr_0.4MnO_3-δ becomes cation deficient and simultaneously almost fully stoichiometric in oxygen. Important for thin film growth is the presence of negative atomic oxygen and under which conditions positive metal-oxygen ions are created in the plasma. This insight into the plasma chemistry shows why the pressure window to obtain films with a desired composition and crystalline structure is narrow and requires a careful adjustment of the process parameters.