The pulsed-laser-deposition (PLD) method is particularly well suited for the growth of oxide thin films, but in the case of other compounds, such as nitrides, PLD presents some limitations which are mainly due to the low reactivity of nitrogen in comparison with oxygen. A possible way to overcome this problem is to increase the reactivity of the constituent species, via plasma assisted-pulsed-laser deposition. A plasma is coupled to the ablation chamber, in order to increase the density of reactive atomic species, which can be further incorporated in the growing film. This approach is described in this paper as well as the nature, energy, and concentration of the atomic and molecular species in the plasma as determined by various plasma diagnostics. These results are correlated to the growth of thin films in the particular case of the aluminum nitride compound. The composition and structure of the films are studied as a function of the growth conditions, and the positive effects of the additional discharge are evidenced on the film purity and properties. The fundamental problem with the PLD technique, especially with metallic targets, is the production of unwanted droplets that significantly worsen the properties of the films. To eliminate these droplets, a thin film has been grown with an experimental setup using two targets and crossed laser beams which gave positive results.