Magnetic excitations of the hybrid multiferroic (ND4)2FeCl5·D2O

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 polarization changes direction concurrently with the field-induced magnetic transition, from mostly aligned with the crystallographic a-axis to the c-axis. To account for such change of polarization direction, the underlying multiferroic mechanism is believed to switch from the inverse Dzyalloshinskii--Moriya model to the p-d hybridization model. We perform a detailed analysis of the inelastic neutron data of (ND4)2FeCl5D2O using linear spin-wave theory to investigate possible impact of different multiferroic mechanisms on the microscopic magnetic interactions. Our result reveals that the spin dynamics of both multiferroic phases can be well-described by a Heisenberg Hamiltonian with an easy-plane anisotropy. We find notable differences between the optimal model parameters of the two phases. In particular, the value of single-ion anisotropy shows a ~50% increase in the high-field phase. Nevertheless, the hierarchy of exchange strength and the balance among frustrated interactions do not change qualitatively between two phases, suggesting that magnetic interactions in (ND4)2FeCl5D2O are much more robust than the electric polarization in response to delicate reorganizations of the electronic degrees of freedom in an applied magnetic field.