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Antiferromagnetic (AFM) materials possess a well-recognized potential for ultrafast data processing thanks to their intrinsic ultrafast spin dynamics, absence of stray fields, and large spin transport effects. The very same properties, however, make their manipulation difficult, requiring frequencies in THz range and magnetic fields of tens of Teslas. Switching of AFM order implies going into the nonlinear regime, a largely unexplored territory. Here we use THz light from a free electron laser to drive antiferromagnetic NiO into a highly nonlinear regime and steer it out of nonlinearity with magnetic field from a 33-Tesla Bitter magnet. This demonstration of large-amplitude dynamics represents a crucial step towards ultrafast resonant switching of AFM order.

Abstract Third-order non-linearities are important because they allow control over light pulses in ubiquitous high-quality centro-symmetric materials like silicon and silica. Degenerate four-wave mixing provides a direct measure of the third-order non-linear sheet susceptibility χ (3) L (where L represents the material thickness) as well as technological possibilities such as optically gated detection and emission of photons. Using picosecond pulses from a free electron laser, we show that silicon doped with P or Bi has a value of χ (3) L in the THz domain that is higher than that reported for any other material in any wavelength band. The immediate implication of our results is the efficient generation of intense coherent THz light via upconversion (also a χ (3) process), and they open the door to exploitation of non-degenerate mixing and optical nonlinearities beyond the perturbative regime.