Pulsed-laser deposition has proved to be a promising method for producing complex inorganic thin films. One of its major advantages, relative to other methods, is the capability of controlling many process parameters, such as laser pulse width, energy, and wavelength along with background reactive gas pressure and substrate bias. Adjusting these parameters provides a pre-tuning of the laser plasma thereby allowing for optimum process conditions in a particular thin film deposition. Understanding and fully characterizing such highly-dynamic and rapidly-streaming plasmas requires multiple techniques for monitoring the plasmas at different stages. By combining different diagnostic methods, it is possible to analyze the broad time window over which these ablation plasmas develop and to understand the related processes that occur. We present in this work new results involving correlation of time-resolved Langmuir probe data, optical emission spectroscopy, and electrostatic energy analysis to characterize the laser-induced plasmas generated from targets of titanium, tin-dioxide and aluminum. Two laser sources, an 80 fs Ti:Sapphire laser (780 nm) and a 6 ns Nd:YAG laser (1.06 micrometer), were used in this work. Examples of very high quality, epitaxial tin-dioxide films grown on sapphire by femtosecond-laser MBE are presented. These films are evaluated by high-resolution, cross-sectional TEM and x-ray diffraction. Film quality is considered in relation to the ablation plasma parameters, wherein femtosecond and nanosecond plasmas are compared.