A synthetic method is presented for the production of isotetrasilane, a higher order perhydridosilane, with the purity and volume necessary for use in extensive studies of the chemical vapor deposition (CVD) of epitaxial silicon (e-Si) thin films. The chemical characteristics, thermodynamic properties, and epitaxial film growth of isotetrasilane are compared with those of other perhydridosilanes. A film-growth mechanism distinct from linear perhydridosilanes H(SiH2)(n)H, where n <= 4, is reported. Preliminary findings are summarized for CVD of both unstrained e-Si and strained e-Si doped with germanium (Ge) and carbon (C) employing isotetrasilane as the source precursor at temperatures of 500-550 degrees C. The results suggest that bis-(trihydridosilyl)silylene is the likely deposition intermediate under processing conditions in which gas-phase depletion reactions are not observed.