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The ferro-rotational order 1-3 , whose order parameter (OP) is an axial vector invariant under both time reversal (TR) and spatial inversion (SI) operations, is the last remaining category of ferroics to be observed after the ferroelectric, ferromagnetic, and ferro-toroidal orders. This order has become increasingly popular in many new quantum materials, especially in complex oxides 1,3 , and is considered responsible for a number of novel phenomena such as polar vortices 4 , giant magnetoelectric coupling 5 , and type-II multiferroics 6 . However, physical properties of the ferrorotational order have been rarely studied either theoretically or experimentally. Here, using high sensitivity rotational anisotropy second harmonic generation (RA SHG), we have, for the first time, exploited the electric quadrupole (EQ) contribution to the SHG to directly couple to this centrosymmetric ferro-rotational order in an archetype of type-II multiferroics, RbFe(MoO4)2. Surprisingly, we have found that two types of domains with opposite ferro-rotational vectors emerge with distinct populations at the critical temperature Tc ~195 K and gradually evolve to reach an even ratio at lower temperatures. Moreover, we have identified the ferro-rotational order phase transition as weak first order, and have revealed its conjugate coupling field as a unique combination of the induced EQ SHG and the incident fundamental electric fields. Our results on physical properties of a ferro-rotational order provide crucial knowledge for understanding and searching for novel phases of matter built upon the ferro-rotational order. Further, these results open the possibility of revealing unconventional centrosymmetric orders and identifying their conjugate coupling fields with second order nonlinear optics.

While the anomalous Hall effect can manifest even without an external magnetic field, time reversal symmetry is nonetheless still broken by the internal magnetization of the sample. Recently, it has been shown that certain materials without an inversion center allow for a nonlinear type of anomalous Hall effect whilst retaining time reversal symmetry. The effect may arise from either Berry curvature or through various asymmetric scattering mechanisms. Here, we report the observation of an extremely large c-axis nonlinear anomalous Hall effect in the non-centrosymmetric Td phase of MoTe2 and WTe2 without intrinsic magnetic order. We find that the effect is dominated by skew-scattering at higher temperatures combined with another scattering process active at low temperatures. Application of higher bias yields an extremely large Hall ratio of E⊥/E|| = 2.47 and corresponding anomalous Hall conductivity of order 8 × 107 S/m.

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