Direct Observation of Anapoles by Neutron Diffraction.

The scope of magnetic neutron scattering has been expanded by the observation of electronic Dirac dipoles (anapoles) that are polar (parity odd) and magnetic (time odd). A zero-magnetization ferromagnet Sm_{0.976}Gd_{0.024}Al_{2} with a diamond-type structure presents Dirac multipoles at basis-forbidden reflections that include the standard (2, 2, 2) reflection. Magnetic amplitudes measured at four such reflections are in full accord with a structure factor calculated from the appropriate magnetic space group.

Magnetic excitations in frustrated fcc type-III antiferromagnet MnS2.

Spin wave dispersion in the frustrated fcc type-III antiferromagnet MnS2 has been determined by inelastic neutron scattering using a triple-axis spectrometer. Existence of multiple spin wave branches, with significant separation between high-energy and low-energy modes highlighting the intrinsic magnetic frustration effect on the fcc lattice, is explained in terms of a spin wave analysis carried out for the antiferromagnetic Heisenberg model for this S = 5/2 system with nearest and next-nearest-neighbor exchange interactions. Comparison of the calculated dispersion with spin wave measurement also reveals small suppression of magnetic frustration resulting from reduced exchange interaction between frustrated spins, possibly arising from anisotropic deformation of the cubic structure.

Quasielastic and low-energy inelastic neutron scattering study of HoCrO3 by high resolution time-of-flight neutron spectroscopy.

In order to understand the origin of the huge quasielastic magnetic scattering observed previously with a back-scattering neutron spectrometer, we have re-investigated the low energy excitations in HoCrO3 by inelastic neutron scattering in a much wider energy range with time-of-flight neutron spectrometers. The inelastic signals are due to the excitations between the ground state doublet of the Ho ion. The quasielastic signal is due to the fluctuation of the disordered Ho moments. At low temperature the intensity of quasielastic scattering is small. It starts increasing as the temperature increases above 30 K. At the same temperature, the elastic intensity due to Ho moment ordering decreases in a similar way. This observation strengthens the hypothesis that the quasielastic scattering is due the fluctuations of the disordered Ho moments. The time scale of fluctuations has been determine from the quasielastic scattering and was found to vary from about 22 ps at [Formula: see text] K to about 2.5 ps at [Formula: see text] K. The stretched exponential line shape indicates a distribution of decay rates at low temperatures.

Single crystal polarized neutron diffraction study of the magnetic structure of HoFeO3.

Polarised neutron diffraction measurements have been made on HoFeO3 single crystals magnetised in both the [0 0 1] and [1 0 0] directions (Pbnm setting). The polarisation dependencies of Bragg reflection intensities were measured both with a high field of [Formula: see text] T parallel to [0 0 1] at [Formula: see text] K and with the lower field [Formula: see text] T parallel to [1 0 0] at [Formula: see text] K. A Fourier projection of magnetization induced parallel to [0 0 1], made using the hk0 reflections measured in 9 T, indicates that almost all of it is due to alignment of Ho moments. Further analysis of the asymmetries of general reflections in these data showed that although, at 70 K, 9 T applied parallel to [0 0 1] hardly perturbs the antiferromagnetic order of the Fe sublattices, it induces significant antiferromagnetic order of the Ho sublattices in the [Formula: see text] plane, with the antiferromagnetic components of moment having the same order of magnitude as the induced ferromagnetic ones. Strong intensity asymmetries measured in the low temperature [Formula: see text] structure with a lower field, 0.5 T [Formula: see text] [1 0 0] allowed the variation of the ordered components of the Ho and Fe moments to be followed. Their absolute orientations, in the [Formula: see text] domain stabilised by the field were determined relative to the distorted perovskite structure. This relationship fixes the sign of the Dzyalshinski-Moriya (D-M) interaction which leads to the weak ferromagnetism. Our results indicate that the combination of strong y-axis anisotropy of the Ho moments and Ho-Fe exchange interactions breaks the centrosymmetry of the structure and could lead to ferroelectric polarization.

Hyperfine and crystal field interactions in multiferroic HoCrO3.

We report a comprehensive specific heat and inelastic neutron scattering study to explore the possible origin of multiferroicity in HoCrO3. We have performed specific heat measurements in the temperature range 100 mK-290 K and inelastic neutron scattering measurements were performed in the temperature range 1.5-200 K. From the specific heat data we determined hyperfine splitting at 22.5(2) µeV and crystal field transitions at 1.379(5) meV, 10.37(4) meV, 15.49(9) meV and 23.44(9) meV, indicating the existence of strong hyperfine and crystal field interactions in HoCrO3. Further, an effective hyperfine field is determined to be 600(3) T. The quasielastic scattering observed in the inelastic scattering data and a large linear term [Formula: see text] mJ mol(-1) K(-2) in the specific heat is attributed to the presence of short range exchange interactions, which is understood to be contributing to the observed ferroelectricity. Further the nuclear and magnetic entropies were computed to be, ∼17.2 Jmol(-1) K(-1) and ∼34 Jmol(-1) K(-1), respectively. The entropy values are in excellent agreement with the limiting theoretical values. An anomaly is observed in the peak position of the temperature dependent crystal field spectra around 60 K, at the same temperature an anomaly in the pyroelectric current is reported. From this we could elucidate a direct correlation between the crystal electric field excitations of Ho(3+) and ferroelectricity in HoCrO3. Our present study, along with recent reports, confirm that HoCrO3, and RCrO3 (R = rare earth) in general, possess more than one driving force for the ferroelectricity and multiferroicity.

Strain heterogeneity and magnetoelastic behaviour of nanocrystalline half-doped La, Ca manganite, La0.5Ca0.5MnO3.

Elastic and anelastic properties of La0.5Ca0.5MnO3 determined by resonant ultrasound spectroscopy in the frequency range ∼100-1200 kHz have been used to evaluate the role of grain size in determining the competition between ferromagnetism and Jahn-Teller/charge order of manganites which show colossal magneto resistance. At crystallite sizes of ∼75 and ∼135 nm the dominant feature is softening of the shear modulus as the charge order transition point, Tco (∼225 K), is approached from above and below, matching the form of softening seen previously in samples with 'bulk' properties. This is consistent with a bilinear dominant strain/order parameter coupling, which occurs between the tetragonal shear strain and the Jahn-Teller (Γ3(+)) order parameter. At crystallite sizes of ∼34 and ∼42 nm the charge ordered phase is suppressed but there is still softening of the shear modulus, with a minimum near Tco. This indicates that some degree of pseudoproper ferroelastic behaviour is retained. The primary cause of the suppresion of the charge ordered structure in nanocrystalline samples is therefore considered to be due to suppression of macroscopic strain, even though MnO6 octahedra must develop some Jahn-Teller distortions on a local length scale. This mechanism for stabilizing ferromagnetism differs from imposition of either an external magnetic field or a homogeneous external strain field (from a substrate), and is likely to lead both to local strain heterogeneity within the nanocrystallites and to different tilting of octahedra within the orthorhombic structure. An additional first order transition occurs near 40 K in all samples and appears to involve some very small strain contrast between two ferromagnetic structures.

Magnetic, magnetocaloric and magnetoresistive properties of cubic Laves phase HoAl2 single crystal.

We report the magnetization (M) and magnetoresistance (MR) results of HoAl2 single crystals oriented along the ⟨100⟩ and ⟨110⟩ directions. Although HoAl2 has cubic Laves phase structure, a large anisotropy is observed in M and MR below the Curie temperature (TC). A satisfactory correlation between magnetic entropy change (ΔSM) and MR could be established along ⟨110⟩ and also ⟨100⟩, except for the temperature (T) region around which spin reorientation takes place. Large inverse magnetocaloric effect is observed at low T, which is associated with the spin reorientation process in the ⟨100⟩ direction. A theoretical model based on the Landau theory of phase transition can describe the T-variation of -ΔSM for T > TC.

CoF2: a model system for magnetoelastic coupling and elastic softening mechanisms associated with paramagnetic ↔ antiferromagnetic phase transitions.

Resonant ultrasound spectroscopy has been used to monitor variations in the elastic and anelastic behaviour of polycrystalline CoF2 through the temperature interval 10-290 K and in the frequency range ∼0.4-2 MHz. Marked softening, particularly of the shear modulus, and a peak in attenuation occur as the Néel point (TN=39 K) is approached from both high and low temperatures. Although the effective thermodynamic behaviour can be represented semiquantitatively with a Bragg-Williams model for a system with spin 1/2, the magnetoelastic coupling follows a pattern which is closely analogous to that of a Landau tricritical transition which is co-elastic in character. Analysis of lattice parameter data from the literature confirms that linear spontaneous strains scale with the square of the magnetic order parameter and combine to give effective shear and volume strains on the order of 1‰. Softening of the shear modulus at T>TN is attributed to coupling of acoustic modes with dynamical local ordering of spins and can be represented by a Vogel-Fulcher expression. At T

Elastic anomalies associated with structural and magnetic phase transitions in single crystal hexagonal YMnO3.

Resonant ultrasound spectroscopy has been used to measure the elastic and anelastic behaviour through known structural and magnetic phase transitions in single crystal hexagonal YMnO3. Anomalous elastic behaviour is observed at the high temperature structural transition at ∼1260 K, with a discontinuity in the elastic constants and nonlinear recovery below Tc, consistent with [Formula: see text] coupling. There is no change in dissipation associated with this high temperature transition, and no evidence in the elastic or anelastic behaviour for any secondary transition at ∼920 K, thus supporting the thesis of a single high temperature transformation. Elastic stiffening is observed on cooling through TN, in accordance with previous studies, and the excess elastic constant appears to scale with the square of the magnetic order parameter. The strains incurred at TN are a factor of ∼20 smaller than those at the structural transition, implying very weak [Formula: see text] coupling and a dominant contribution to the variation in the elastic constants from [Formula: see text]. The increased acoustic dissipation above TN is consistent with an order-disorder process.

Direct observation of low energy nuclear spin excitations in HoCrO3 by high resolution neutron spectroscopy.

We have investigated low energy nuclear spin excitations in the strongly correlated electron compound HoCrO3. We observe clear inelastic peaks at E = 22.18 ± 0.04 µeV in both energy loss and gain sides. The energy of the inelastic peaks remains constant in the temperature range 1.5-40 K at which they are observed. The intensity of the inelastic peak increases at first with increasing temperature and then decreases at higher temperatures. The temperature dependence of the energy and intensity of the inelastic peaks is very unusual compared to that observed in other Nd, Co, V and also simple Ho compounds. Huge quasielastic scattering appears at higher temperatures presumably due to the fluctuating electronic moments of the Ho ions that get increasingly disordered at higher temperatures. The strong quasielastic scattering may also originate in the first Ho crystal-field excitations at about 1.5 meV.

Polarization dependence of magnetic Bragg scattering in YMn2O5.

The polarization dependence of the intensity of elastic magnetic scattering from YMn2O5 single crystals has been measured at 25 K in magnetic fields between 1 and 9 T. A significant polarization dependence was observed in the intensities of magnetic satellite reflections, propagation vector τ = ½, 0, », measured with both the [100] and [010] axes parallel to the common polarization and applied field direction. The intensity asymmetries A observed in sets of orthorhombic equivalent reflections show systematic relationships which allow the phase relationship between different components of their magnetic interaction vectors to be determined. They fix the orientation relationships between the small y and z moments on the Mn(4+) and Mn(3+) sub-lattices and have allowed a further refinement of the magnetic structure, which determines the phases of the vector Fourier components with much higher precision. Systematic differences found between values of A(hkl) and A(h¯k¯l¯) suggest that there is a small modulation of the nuclear structure which has the same wavevector as the magnetic modulation and gives rise to a small nuclear structure factor for the satellite reflections. The magnitudes of the differences suggest shifts in the atomic positions of the order of 0.05 Å.

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.

Understanding the insulating phase in colossal magnetoresistance manganites: shortening of the Jahn-Teller long-bond across the phase diagram of La1-xCaxMnO3.

The detailed evolution of the magnitude of the local Jahn-Teller (JT) distortion in La(1-x)Ca(x)MnO3 is obtained across the phase diagram for 0< or =x< or =0.5 from high-quality neutron diffraction data using the atomic pair distribution function method. A local JT distortion is observed in the insulating phase for all Ca concentrations studied. However, in contrast with earlier local structure studies, its magnitude is not constant, but decreases continuously with increasing Ca content. This observation is at odds with a simple small-polaron picture for the insulating state.

Charge ordering and spin dynamics in NaV(2)O(5).

We report high-resolution neutron inelastic scattering experiments on the spin excitations of NaV(2)O(5). Below T(c), two branches with distinct energy gaps are identified. From the dispersion and intensity of the spin excitation modes, we deduce the precise zigzag charge distribution on the ladder rungs and the corresponding charge order: Delta(c) approximately 0.6. We argue that the spin gaps observed in the low-T phase of this compound are primarily due to the charge transfer.

DNA cleavage by 7-methylbenzopentathiepin: a simple analog of the antitumor antibiotic varacin.

The compound 7-methylbenzopentathiepin, a simple analog of the benzopentathiepin antitumor antibiotic varacin, was shown to be a potent thiol-dependent DNA-cleaving agent. Biological experiments previously suggested that DNA cleavage might play a role in the cytotoxicity of varacin; however, this is the first direct evidence that benzopentathiepins can cause DNA strand breaks under physiologically relevant conditions.

Carcinoma of the hypopharynx: results of combined therapy.

Hypopharyngeal carcinoma is an aggressive cancer with a guarded prognosis. Results of 64 patients with-hypopharyngeal cancer, 59 of whom were in stage III or IV, undergoing curative therapy during a six-year period were analysed. A combined modality resulted in a 62% and 38.4% 2-year disease free survival incases with pyriform sinus and postcricoid tumours respectively. Results of radiotherapy failed salvage surgery were much poorer for either site.