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Neutron spherical polarimetry, which is directly sensitive to the absolute magnetic configuration and domain population, has been used in this work to unambiguously prove the multiferroicity of (ND4)2[FeCl5(D2O)]. We demonstrate that the application of an electric field upon cooling results in the stabilization of a single-cycloidal magnetic domain below 6.9 K, while poling in the opposite electric field direction produces the full population of the domain with opposite magnetic chirality. We prove the complete switchability of the magnetic domains at low temperature by the applied electric field, which constitutes a direct proof of the strong magnetoelectric coupling. Additionally, we refine the magnetic structure of the ordered ground state, determining the underlying magnetic space group consistent with the direction of the ferroelectric polarization, and we provide evidence of a collinear amplitude-modulated state with magnetic moments along the a-axis in the temperature region between 6.9 and 7.2 K.
Our results describe an unprecedented example of change in the mechanism of magnetically-induced electric polarization from spin current to spin-dependent p-d hybridization model. We have followed the evolution of the magnetic structures of (ND4)2[Fe
The number of magnetoelectric multiferroic materials reported to date is scarce, as magnetic structures that break inversion symmetry and induce an improper ferroelectric polarization typically arise through subtle competition between different magne
We report a comprehensive inelastic neutron scattering study of the hybrid molecule-based multiferroic compound (ND4)2FeCl5D2O in the zero-field incommensurate cycloidal phase and the high-field quasi-collinear phase. The spontaneous electric polariz
An investigation of the spatially resolved distribution of domains in the multiferroic phase of MnWO$_4$ reveals that characteristic features of magnetic and ferroelectric domains are inseparably entangled. Consequently, the concept of multiferroic h
We employ neutron spherical polarimetry to determine the nature and population of the coexisting antiferromagnetic domains in multiferroic YMn2O5. By applying an electric field, we prove that reversing the electrical polarization results in the popul