Abstract
We report evidence for ferroelectricity in bismuth manganite epitaxial films from optical second-harmonic generation (SHG). The change in the polar symmetry of SHG signals under external electric fields is correlated to specific changes in the ferroelectric domain microstructures. We also observe giant enhancement of SHG by 3 to 4 orders of magnitude with effective ${d}_{f}\ensuremath{\sim}193\mathrm{p}\mathrm{m}/\mathrm{V}$ under electric fields of \ensuremath{\sim}707 V/mm. The material also exhibits a large third-order nonlinear optical response with nonlinear absorption coefficient ${\ensuremath{\alpha}}_{I}\ensuremath{\sim}\ensuremath{-}0.08\mathrm{c}\mathrm{m}/\mathrm{k}\mathrm{W}$ and nonlinear refractive index ${n}_{I}\ensuremath{\sim}\ensuremath{-}0.53\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}9}{\mathrm{cm}}^{2}/\mathrm{W}.$
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