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We have epitaxially grown undoped β-FeSi2films on Si(111) substrates via atomic-hydrogen-assisted molecular-beam epitaxy.β-FeSi2filmsgrown without atomic hydrogen exhibited p-type conduction with a hole density of over 1019 cm−3 at room temperature (RT). In contrast, those prepared with atomic hydrogen showed n-type conduction and had a residual electron density that was more than two orders of magnitude lower than the hole density of filmsgrown without atomic hydrogen (of the order of 1016 cm−3 at RT). The minority-carrier diffusion length was estimated to be approximately 16 μm using an electron-beam-induced current technique; this value is twice as large as that for β-FeSi2 prepared without atomic hydrogen. This result could be well explained in terms of the minority-carrier lifetimes measured by a microwave photoconductance decay technique. The 1/e decay time using a 904 nm laser pulse was approximately 17 μs, which is much longer than that for β-FeSi2 prepared without atomic hydrogen (3 μs). The photoresponsivity reached 13 mA/W at 1.31 μm, which is the highest value ever reported for β-FeSi2films.