Undoped 0.5-lm-thick BaSi 2 epitaxial films were grown on Si(111) substrates with various ratios of the Ba deposition rate to the Si deposition rate (R Ba /R Si) ranging from 1.0 to 5.1, and their electrical and optical properties were characterized. The photoresponse spectra drastically changed as a function of R Ba /R Si , and the quantum efficiency reached a maximum at R Ba /R Si ¼ 2.2. Hall measurements and capacitance versus voltage measurements revealed that the electron concentration drastically decreased as R Ba /R Si approached 2.2, and the BaSi 2 films with R Ba /R Si ¼ 2.0, 2.2, and 2.6 exhibited p-type conductivity. The lowest hole concentration of approximately 1 Â 10 15 cm À3 was obtained for the BaSi 2 grown with R Ba /R Si ¼ 2.2, which is the lowest value ever reported. First-principles calculations suggest that Si vacancies give rise to localized states within the bandgap of BaSi 2 and therefore degrade the minority-carrier properties.