A. Daoud-Aladine

Thermal-history dependent magnetoelastic transition in (Mn,Fe)2(P,Si)

The thermal-history dependence of the magnetoelastic transition in (Mn,Fe)2(P,Si) compounds has been investigated using high-resolution neutron diffraction. As-prepared samples display a large difference in paramagnetic-ferromagnetic (PM-FM) transition temperature compared to cycled samples. The initial metastable state transforms into a lower-energy stable state when the as-prepared sample crosses the PM-FM transition for the first time. This additional transformation is irreversible around the transition temperature and increases the energy barrier which needs to be overcome through the PM-FM transition. Consequently, the transition temperature on first cooling is found to be lower than on subsequent cycles characterizing the so-called “virgin effect.” High-temperature annealing can restore the cycled sample to the high-temperature metastable state, which leads to the recovery of the virgin effect. A model is proposed to interpret the formation and recovery of the virgin effect.

Nature of the magnetic order in Ca3Co2O6.

We present a detailed powder and single-crystal neutron diffraction study of the spin chain compound Ca3Co2O6. Below 25 K, the system orders magnetically with a modulated partially disordered antiferromagnetic structure. We give a description of the magnetic interactions in the system which is consistent with this magnetic structure. Our study also reveals that the long-range magnetic order coexists with a shorter-range order with a correlation length scale of approximately 180 angstroms in the ab plane. Remarkably, on cooling, the volume of material exhibiting short-range order increases at the expense of the long-range order.

The nature of the magnetic order in Ca3Co2O6

We present a detailed powder and single-crystal neutron diffraction study of the spin chain compound Ca3Co2O6. Below 25 K, the system orders magnetically with a modulated partially disordered antiferromagnetic structure. We give a description of the magnetic interactions in the system which is consistent with this magnetic structure. Our study also reveals that the long-range magnetic order coexists with a shorter-range order with a correlation length scale of approximately 180 angstroms in the ab plane. Remarkably, on cooling, the volume of material exhibiting short-range order increases at the expense of the long-range order.

Magnetically driven suppression of nematic order in an iron-based superconductor

A theory of superconductivity in the iron-based materials requires an understanding of the phase diagram of the normal state. In these compounds, superconductivity emerges when stripe spin density wave (SDW) order is suppressed by doping, pressure or atomic disorder. This magnetic order is often pre-empted by nematic order, whose origin is yet to be resolved. One scenario is that nematic order is driven by orbital ordering of the iron 3d electrons that triggers stripe SDW order. Another is that magnetic interactions produce a spin-nematic phase, which then induces orbital order. Here we report the observation by neutron powder diffraction of an additional fourfold-symmetric phase in Ba1-xNaxFe2As2 close to the suppression of SDW order, which is consistent with the predictions of magnetically driven models of nematic order.

Origin and stability of the dipolar response in a family of tetragonal tungsten bronze relaxors

A new family of relaxor dielectrics with the tetragonal tungsten bronze structure (nominal composition Ba6M3+Nb9O 30, M3+ = Ga, Sc, or In) were studied using dielectric spectroscopy to probe the dynamic dipole response and correlate this with the crystal structure as determined from powder neutron diffraction. Independent analyses of real and imaginary parts of the complex dielectric function were used to determine characteristic temperature parameters, TVF and TUDR, respectively. In each composition both these temperatures correlated with the temperature of maximum crystallographic strain, T c/a, determined from diffraction data. The overall behavior is consistent with dipole freezing and the data indicate that the dipole stability increases with increasing M3+ cation size as a result of increased tetragonality of the unit cell. Crystallographic data suggests that these materials are uniaxial relaxors with the dipole moment predominantly restricted to the B1 cation site in the structure. Possible origins of the relaxor behavior are discussed.

Strain driven structural phase transformations in dysprosium doped BiFeO3 ceramics

A detailed powder neutron and synchrotron diffraction study coupled with a complementary Raman spectroscopy study of the addition of Dy3+ into BiFeO3 ceramics is reported here. It can be seen that the addition of Dy3+ destabilises the polar R3c symmetry due to chemical strain effects arising from the large size mismatch between the two A-site cations (Dy3+ and Bi3+). This results in a lowering of the symmetry to a polar Cc model and in the range 0.05 ≤ x ≤ 0.30 in Bi1−xDyxFeO3 competition develops between the strained polar Cc and non-polar Pnma symmetries with the Cc model becoming increasingly strained until approximately x = 0.12 at which point the Pnma model becomes favoured. However, phase co-existence between the Cc and Pnma phases persists to x = 0.25. Preliminary magnetic measurements also suggest weak ferromagnetic character which increases in magnitude with increasing Dy3+ content. Preliminary electrical measurements suggest that whilst Bi0.95Dy0.05FeO3 is most likely polar; Bi0.70Dy0.30FeO3 shows relaxor-type behaviour.

Electric Field Switching of Antiferromagnetic Domains in YMn2O5 : A Probe of the Multiferroic Mechanism

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 population inversion of two types of in-plane domains, related to each other by inversion. Our results are completely consistent with the exchange-striction mechanism of ferroelectricity, and support a unified model where cycloidal ordering is induced by coupling to the main magnetic order parameter.

Multiferroic properties and magnetic structure of Sm1−xYxMnO3

We have successfully induced multiferroic behavior in the A-type antiferromagnet SmMnO(3) by the substitution of Y at the Sm site. A magnetic transition develops at similar to 24 K for Sm(1-x)Y(x)MnO(3) (x = 0.4, 0.5) which is not present in the parent compound. This transition coincides with the onset of electric order, with an electric polarization measured along the c axis. It is proposed that the effect of Y doping is to bring about a subtle distortion of the MnO(6) octahedra, causing a magnetic ordering of the Mn(3+) moments similar to that reported for the well-studied multiferroic TbMnO(3). Following on from our previous study on polycrystalline samples, we present measurements of the magnetic and electric properties of single-crystal Sm(0.6)Y(0.4)MnO(3) and Sm(0.5)Y(0.5)MnO(3). The data are summarized in a phase diagram for each of the principal crystallographic axes for the x = 0.5 compound. Powder neutron diffraction experiments on SmMnO(3) and Sm(0.6)Y(0.4)MnO(3) show that the Y substitution causes a change in the Mn-O-Mn bond angle toward the value found for TbMnO(3). The magnetic structure of Sm(0.6)Y(0.4)MnO(3) has been shown to consist of two phases: a sinusoidal ordering of the Mn(3+) moments below 50 K and a cycloidal ordering below 27 K. The cycloidal ordering occurs at the same temperature as the previously observed ferroelectric polarization, suggesting a similar multiferroic mechanism to that found in TbMnO(3).

Multiferroicity and spiral magnetism inFeVO4with quenched Fe orbital moments

FeVO{sub 4} has been studied by heat capacity, magnetic susceptibility, electric polarization and single-crystal neutron-diffraction experiments. The triclinic crystal structure is made of S-shaped clusters of six Fe{sup 3+} ions, linked by VO{sub 4}{sup 3-} groups. Two long-range magnetic ordering transitions occur at T{sub N1}=22 K and T{sub N2}=15 K. Both magnetic structures are incommensurate and below T{sub N2}, FeVO{sub 4} becomes weakly ferroelectric coincidentally with the loss of the collinearity of the magnetic structure in a very similar fashion than in the classical TbMnO{sub 3} multiferroic material. However we argue that the symmetry considerations and the mechanisms invoked to explain these properties in TbMnO{sub 3} do not straightforwardly apply to FeVO{sub 4}. First, the magnetic structures, even the collinear structure, are all acentric so that ferroelectricity in FeVO{sub 4} is not correlated with the fact magnetic ordering is breaking inversion symmetry. Regarding the mechanism, FeVO{sub 4} has quenched orbital moments that questions the exact role of the spin-orbit interactions.

Magnetoelastic coupling in the phase diagram of Ba1-xK xFe2As2 as seen via neutron diffraction

We report a high resolution neutron diffraction investigation of the coupling of structural and magnetic transitions in Ba1xKxFe2As2. The tetragonal-orthorhombic and antiferromagnetic transitions are suppressed with potassium-doping, falling to zero at x ~ 0.24.