Large third-order optical nonlinearities were observed in epitaxial thin films of BiMnO3 grown on SrTiO3 substrates. Using 140 fs laser pulses at 900 nm, a negative nonlinear refractive index (nI∼−0.53 cm2/GW) and a nonlinear absorption coefficient I∼−0.08 cm/kW) for BiMnO3 are measured at room temperature. Large electric-field-induced enhancement of three to four orders of magnitude in the second-harmonic response at 450 nm is observed with effective nonlinear coefficients of deff∼40(115) pm/V at 300 (473) K under applied fields of ∼707 (177) V/mm, respectively, from a 110 nm multivariant thin film.

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