The control of multiferroic domains through external electric fields has been studied by dielectric measurements and by polarized neutron diffraction on single-crystalline TbMnO$_3$. Full hysteresis cycles were recorded by varying an external field of the order of several kV/mm and by recording the chiral magnetic scattering as well as the charge in a sample capacitor. Both methods yield comparable coercive fields that increase upon cooling.
Detailed investigation of the incommensurate magnetic ordering in a single crystal of multiferroic NdMn2O5 has been performed using both non-polarized and polarized neutron diffraction techniques. Below TN = 30.5 K magnetic Bragg reflections corresponding to the non-chiral type magnetic structure with propagation vector k1 = (0.5 0 kz1) occurs. Below about 27 K a new distorted magnetic modulation with a similar vector kz2 occurs, which is attributed to the magnetization of the Nd3+ ions by the Mn-sub-lattice. Strong temperature hysteresis in the occurrence of the incommensurate magnetic phases in NdMn2O5 was observed depending on the cooling or heating history of the sample. Below about 20 K the magnetic structure became of a chiral type. From spherical neutron polarimetry measurements, the resulting low-temperature magnetic structure kz3 was approximated by the general elliptic helix. The parameters of the magnetic helix-like ellipticity and helical plane orientation in regard to the crystal structure were determined. A reorientation of the helix occurs at an intermediate temperature between 4 K and 18 K. A difference between the population of right- and left-handed chiral domains of about 0.2 was observed in the as-grown crystal when cooling without an external electric field. The magnetic chiral ratio can be changed by the application of an external electric field of a few kV/cm, revealing strong magnetoelectric coupling. A linear dependence of the magnetic chirality on the applied electric field in NdMn2O5 was found. The results are discussed within the frame of the antisymmetric super-exchange model for Dzyaloshinsky-Moria interaction.
Magneto-electric multiferroics exemplified by TbMnO3 possess both magnetic and ferroelectric long-range order. The magnetic order is mostly understood, whereas the nature of the ferroelectricity has remained more elusive. Competing models proposed to explain the ferroelectricity are associated respectively with charge transfer and ionic displacements. Exploiting the magneto-electric coupling, we use an electric field to produce a single magnetic domain state, and a magnetic field to induce ionic displacements. Under these conditions, interference charge-magnetic X-ray scattering arises, encoding the amplitude and phase of the displacements. When combined with a theoretical analysis, our data allow us to resolve the ionic displacements at the femtoscale, and show that such displacements make a significant contribution to the zero-field ferroelectric moment.
We have used in-field neutron and X-ray single crystal diffraction to measure the incommensurability δ of the crystal and magnetic structure of multiferroic TbMnO3 . We show that the flop in the electric polarization at the critical field HC, for field H along the a− and b−axis coincides with a 1st order transition to a commensurate phase with propagation vector κ = (0, 1/4, 0). In-field X-ray diffraction measurements show that the quadratic magneto-elastic coupling breaks down with applied field as shown by the observation of the 1st harmonic lattice reflections above and below HC . This indicates that magnetic field induces a linear magneto-elastic coupling. We argue that the commensurate phase can be described by an ordering of Mn-O-Mn bond angles.
We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales.
Multiferroic TbMnO3 is investigated using x-ray diffraction in high magnetic fields. Measurements on first and second harmonic structural reflections due to modulations induced by the Mn and Tb magnetic order are presented as function of temperature and field oriented along the a and b-directions of the crystal. The relation to changes in ordering of the rare earth moments in applied field is discussed. Observations below T_N(Tb) without and with applied magnetic field point to a strong interaction of the rare earth order, the Mn moments and the lattice. Also, the incommensurate to commensurate transition of the wave vector at the critical fields is discussed with respect to the Tb and Mn magnetic order and a phase diagram on basis of these observations for magnetic fields H||a and H||b is presented. The observations point to a complicated and delicate magneto-elastic interaction as function of temperature and field.