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Neutron diffraction with static and pulsed magnetic fields is used to directly probe the magnetic structures in LiNiPO4 up to 25 T and 42 T, respectively. By combining these results with magnetometry and electric polarization measurements under pulsed fields, the magnetic and magnetoelectric phases are investigated up to 56 T applied along the easy c-axis. In addition to the already known transitions at lower fields, three new ones are reported at 37.6, 39.4 and 54 T. Ordering vectors are identified with Q VI = (0, 1 3 , 0) in the interval 37.6 − 39.4 T and QVII = (0, 0, 0) in the interval 39.4 − 54 T. A quadratic magnetoelectric effect is discovered in the QVII = (0, 0, 0) phase and the field-dependence of the induced electric polarization is described using a simple mean-field model. The observed magnetic structure and magnetoelectric tensor elements point to a change in the lattice symmetry in this phase. We speculate on the possible physical mechanism responsible for the magnetoelectric effect in LiNiPO4.

Magnetic structures are investigated by means of neutron diffraction to shine light on the intricate details which are believed key to understanding the magnetoelectric effect in LiCoPO4. At zero field, a spontaneous spin canting of ϕ = 7(1) • is found. The spins tilt away from the easy b-axis towards c. Symmetry considerations lead to the magnetic point group m ′ z which is consistent with the previously observed magnetoelectric tensor form and weak ferromagnetic moment along b. For magnetic fields applied along a, the induced ferromagnetic moment couples via the Dzyaloshinskii-Moriya interaction to yield an additional field-induced spin canting. An upper limit to the size of the interaction is estimated from the canting angle.