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Terahertz pulses are applied as an all-optical bias to ferroelectric thin-film BiFeO3 while monitoring the time-dependent ferroelectric polarization through its nonlinear optical response. Modulations in the intensity of the second harmonic light generated by the film correspond to on-off ratios of 220× gateable on femtosecond timescales. Polarization modulations comparable to the built-in static polarization are observed.

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