We have paid special attention to Barium disilicide (BaSi2), which shows great promise as a new material for thin-film solar cells. In this study, we fabricated 500-nm-thick BaSi2 layers by molecular beam epitaxy on n-Si (111) substrates and investigated the effect of increasing growth temperature on optical properties and crystalline quality of BaSi2 light absorbers. By raising growth temperature from 580 to 650 °C, the optimum Ba to Si deposition rate ratio $(R_{mathrm{Ba}}/R_{mathrm{Si}})$ shifted from 3 to 4 from the viewpoint of crystalline orientation along the surface normal. This shift is interpreted to be determined by the actual Ba/Si atomic ratio. On the other hand, photoresponsivity reached a maximum at $R_{mathrm{Ba}}/R_{mathrm{Si}}=1.2$, meaning that the optimum $R_{mathrm{Ba}}/R_{mathrm{Si}}$ shifted to a Si-rich side from the viewpoint of minority-carrier properties. The achieved photoresponsivity is about 3 times higher than that ever reported. Raman spectroscopy suggested that Si vacancies decreased without forming Si precipitates for BaSi2 films grown at $R_{mathrm{Ba}}/R_{mathrm{Si}}=1.2$. However, further decrease in $R_{mathrm{Ba}}/R_{mathrm{Si}}$ generated Si precipitates proved by Raman spectroscopy. Based on these results, we can state that the highest photoresponsivity is obtained for the smallest $R_{mathrm{Ba}}/R_{mathrm{Si}}$ regardless of growth temperature, wherein Si precipitates do not form.
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