The fundamental surface chemical interactions involved in the epitaxial growth of gallium arsenide from organometallic precursors are investigated using molecular-beam scattering techniques and surface-sensitive probes such as electron diffraction and photoelectron spectroscopy. Supersonic beam techniques are a powerful means to probe adsorption, the prerequisite to epitaxy. Behavior of the adsorbed intermediates on the surface, including reaction, diffusion, and decomposition, are assessed by modulated beam techniques and by modulation of surface temperature. Several crystallographic orientations are studied. Attempts are made to synthesize adsorbed decomposition products such as hydrogen and carbonaceous species in order to assess their influence on the growth kinetics and the composition of the film. This work provides the fundamental information needed to develop processes for more precise and uniform production of gallium arsenide crystals for microelectronic applications. The data produced will also find use in the simulation of existing processes employing epitaxial growth.