Search

Magnetic order and excitations in multiferroic DyMnO3 were studied by neutron scattering experiments using a single crystal prepared with enriched 162Dy isotope. The ordering of Mn moments exhibits pronounced hysteresis arising from the interplay between Mn and Dy magnetism which possesses a strong impact on the ferroelectric polarization. The magnon dispersion resembles that reported for TbMnO3. We identify the excitations at the magnetic zone center and near the zone boundary in the b direction, which can possess electromagnon character. The lowest frequency of the zone-center magnons is in good agreement with a signal in a recent optical measurement so that this mode can be identified as the electromagnon coupled by the same Dzyaloshinski-Moriya interaction as the static multiferroic phase.

We report the discovery of a ferroelectric ground state below 4.5 K in highly underdoped La_2CuO_(4+x) accompanied by slow charge dynamics which develop below T~40 K. An anisotropic magnetoelectric response has also been observed, indicating considerable spin-charge coupling in this lightly doped "parent" high temperature copper-oxide superconductor. The ferroelectric state is proposed to develop from polar nanoregions, in which spatial inversion symmetry is locally broken due to non-stoichiometric carrier doping., Comment: 7 Pages, 6 Figures, supplementary material

We study spin liquid in the frustrated diamond lattice antiferromagnet CoAl2O4 by means of single crystal neutron scattering in zero and applied magnetic field. The magnetically ordered phase appearing below TN=8 K remains nonconventional down to 1.5 K. The magnetic Bragg peaks at the q=0 positions remain broad and their profiles have strong Lorentzian contribution. Additionally, they are connected by weak diffuse streaks along the <111> directions. These observations are explained within the spiral spin liquid model as short-range magnetic correlations of spirals populated at these finite temperatures, as the energy minimum around q=0 is flat and the energy of excited states with q=(111) is low. The agreement is only qualitative, leading us to suspect that microstructure effects are also important. Magnetic field significantly perturbs spin correlations. The 1.5 K static magnetic moment increases from 1.58 mB/Co at zero field to 2.08 mB/Co at 10 T, while the magnetic peaks, being still broad, acquire almost Gaussian profile. Spin excitations are rather conventional spin waves at zero field, resulting in the exchange parameters J1=0.92(1) meV, J2=0.101(2) meV and the anisotropy term D=-0.0089(2) meV for CoAl2O4. The application of a magnetic field leads to a pronounced broadening of the excitations at the zone center, which at 10 T appear gapless and nearly featureless.

{\alpha}-CaCr2O4 is a distorted triangular antiferromagnet. The magnetic Cr3+ ions which have spin-3/2 and interact with their nearest neighbors via Heisenberg direct exchange interactions, develop long-range magnetic order below T_N=42.6 K. Powder and single-crystal neutron diffraction reveal a helical magnetic structure with ordering wavevector k=(0,~1/3,0) and angles close to 120{\deg} between neighboring spins. Spherical neutron polarimetry unambiguously proves that the spins lie in the ac plane perpendicular to k. The magnetic structure is therefore that expected for an ideal triangular antiferromagnet where all nearest neighbor interactions are equal, in spite of the fact that {\alpha}-CaCr2O4 is distorted with two inequivalent Cr3+ ions and four different nearest neighbor interactions. By simulating the magnetic order as a function of these four interactions it is found that the special pattern of interactions in {\alpha}-CaCr2O4 stabilizes 120{\deg} helical order for a large range of exchange interactions., Comment: 13 pages, 12 figures

Chuang et al (Reports, 8th of January 2010, p. 181)1 report quasiparticle interference (QPI) imaging that shows pronounced C2 asymmetry. They interpreted this result as indication of an electronic nematic phase with an electron band dispersive only along the b-axis of this orthorhombic material. We argue that this asymmetry is consistent with the underlying long range magnetic order and that LDA electronic structure provides a better description of the QPI images than the 1D band structure conjectured by Chuang et al.

Magnetic order of the manganese and rare-earth lattices according to different symmetry representations is observed in multiferroic hexagonal (h-) DyMnO$_3$ by optical second harmonic generation and neutron diffraction. The incompatibility reveals that the 3d-4f coupling in the h-$R$MnO$_3$ system ($R$ = Sc, Y, In, Dy - Lu) is substantially less developed than commonly expected. As a consequence, magnetoelectric coupling effects in this type of split-order parameter multiferroic that were previously assigned to a pronounced 3d-4f coupling have now to be scrutinized with respect to their origin.

Synchrotron X-ray diffraction investigations of two single crystals of Na_xCoO_2 from different batches with composition x = 0.525-0.530 reveal homogeneous incommensurate sodium ordering with propagation vector (0.53 0.53 0) at room-temperature. The incommensurate (qq0) superstructure exists between 220 K and 430 K. The value of q varies between q = 0.514 and 0.529, showing a broad plateau at the latter value between 260 K and 360 K. On cooling, unusual reversible phase segregation into two volume fractions is observed. Below 220 K, one volume fraction shows the well-known commensurate orthorhombic x = 0.50 superstructure, while a second volume fraction with x = 0.55 exhibits another commensurate superstructure, presumably with a 6a x 6a x c hexagonal supercell. We argue that the commensurate-to-incommensurate transition is an intrinsic feature of samples with Na concentrations x = 0.5 + d with d ~ 0.03., Comment: Corrected/improved version

The iron chalcogenide Fe1+y(Te1-xSex) is structurally the simplest of the Fe-based superconductors. Although the Fermi surface is similar to iron pnictides, the parent compound Fe1+yTe exhibits antiferromagnetic order with in-plane magnetic wave-vector (pi, 0). This contrasts the pnictide parent compounds where the magnetic order has an in-plane magnetic wave-vector (pi, pi) that connects hole and electron parts of the Fermi surface. Despite these differences, both the pnictide and chalcogenide Fe-superconductors exhibit superconducting spin resonances around (pi, pi), suggesting a common symmetry for their superconducting order parameter. A central question in this burgeoning field is therefore how (pi, pi) superconductivity can emerge from a (pi, 0) magnetic instability. Here, we report that the magnetic soft mode evolving from the (pi, 0)-type magnetic long-range order is associated with weak charge carrier localization. Bulk superconductivity occurs only as the magnetic mode at (pi, pi) becomes dominant upon doping. Our results suggest a common magnetic origin for superconductivity in iron chalcogenide and pnictide superconductors., Comment: 17 pages, 4 figures

Charge carriers in low-doped semiconductors may distort the atomic lattice and trap themselves forming so-called small polarons. High carrier concentrations can lead to short range ordered polarons (large polarons) and even to long range charge and orbital order. Both systems should be insulating with a large electrical resistivity, which decreases with increasing temperature. However, photoemission measurements recently found a polaronic pseudogap, in a metallic phase of La2-2xSr1+2xMn2O7. This layered manganite is famous for colossal magnetoresistance (CMR) associated with a phase transition from this low-temperature metallic phase to a high temperature insulating phase. Broad charge order peaks due to large polarons observed by neutron and x-ray scattering in the insulating phase disappear when La2-2xSr1+2xMn2O7 becomes metallic. We report results of inelastic neutron scattering measurements showing that polarons remain inside the metallic phase as fluctuations that strongly broaden and soften certain phonons near the wave vectors where the charge order peaks appeared in the insulating phase. Our findings imply that polaronic signatures in metals may generally come from a competing insulating charge-ordered phase. It is highly relevant to cuprate superconductors with both a pseudogap, and a similar phonon effect associated with a competing stripe order.

We report on inelastic neutron scattering measurements that find incommensurate itinerant like magnetic excitations in the normal state of superconducting FeTe$_{0.6}$Se$_{0.4}$ (\Tc=14K) at wave-vector $\mathbf{Q}_{inc}=(1/2\pm\epsilon,1/2\mp\epsilon)$ with $\epsilon$=0.09(1). In the superconducting state only the lower energy part of the spectrum shows significant changes by the formation of a gap and a magnetic resonance that follows the dispersion of the normal state excitations. We use a four band model to describe the Fermi surface topology of iron-based superconductors with the extended $s(\pm)$ symmetry and find that it qualitatively captures the salient features of these data., Comment: 7 pages and 5 figures

Sizeable b and c components of the 4f moments and pronounced circular dichroism are observed in the ferroelectric phase of DyMnO_3 by soft X-ray diffraction at the Dy-M_5 resonance. This points to cycloidal order of the 4f moments and indicates that inversion-symmetry breaking in this material is not characteristic of the Mn spins alone. The circular dichroism allows to image chiral domains that are imprinted on the surface of a DyMnO$_3$ single crystal, exploiting the local charging by the X-ray beam via the photoelectric effect. These findings suggest a novel approach to control and image domains and domain walls in multiferroic materials.

Ga for Mn substitution in multiferroic TbMnO$_{3}$ has been performed in order to study the influence of Mn-magnetic ordering on the Tb-magnetic sublattice. Complete characterization of TbMn$_{1-x}$Ga$_x$O$_{3}$ ($x$ = 0, 0.04, 0.1) samples, including magnetization, impedance spectroscopy, and x-ray resonant scattering and neutron diffraction on powder and single crystals has been carried out. We found that keeping the same crystal structure for all compositions, Ga for Mn substitution leads to the linear decrease of $T_{\rm N}^{\rm Mn}$ and $\tau^{\rm Mn}$, reflecting the reduction of the exchange interactions strength $J_{\rm Mn-Mn}$ and the change of the Mn-O-Mn bond angles. At the same time, a strong suppression of both the induced and the separate Tb-magnetic ordering has been observed. This behavior unambiguously prove that the exchange fields $J_{\rm Mn-Tb}$ have a strong influence on the Tb-magnetic ordering in the full temperature range below $T_{\rm N}^{\rm Mn}$ and actually stabilize the Tb-magnetic ground state., Comment: 9 pages, 8 figures

CaFe2As2 single crystals under uniaxial pressure applied along the c axis exhibit the coexistence of several structural phases at low temperatures. We show that the room-temperature tetragonal phase is stabilized at low temperatures for pressures above 0.06 GPa, and its weight fraction attains a maximum in the region where superconductivity is observed under applied uniaxial pressure. Simultaneous resistivity measurements strongly suggest that this phase is responsible for the superconductivity in CaFe2As2 found below 10 K in samples subjected to nonhydrostatic pressure conditions., Comment: 5 pages, 3 figures

We present a comprehensive ellipsometric study of an untwinned, nearly stoichiometric LaMnO_3 crystal in the spectral range 1.2-6.0 eV at temperatures 20 K < T < 300 K. The complex dielectric response along the b and c axes of the Pbnm orthorhombic unit cell, \epsilon^b(\nu) and \epsilon^c(\nu), is highly anisotropic over the spectral range covered in the experiment. The difference between \epsilon^b(\nu) and \epsilon^c(\nu) increases with decreasing temperature, and the gradual evolution observed in the paramagnetic state is strongly enhanced by the onset of A-type antiferromagnetic long-range order at T_N = 139.6 K. In addition to the temperature changes in the lowest-energy gap excitation at 2 eV, there are opposite changes observed at higher energy at 4 - 5 eV, appearing on a broad-band background due to the strongly dipole-allowed O 2p -- Mn 3d transition around the charge-transfer energy 4.7 eV. Based on the observation of a pronounced spectral-weight transfer between low- and high-energy features upon magnetic ordering, they are assigned to high-spin and low-spin intersite d^4d^4 - d^3d^5 transitions by Mn electrons. The anisotropy of the lowest-energy optical band and the spectral weight shifts induced by antiferromagnetic spin correlations are quantitatively described by an effective spin-orbital superexchange model. An analysis of the multiplet structure of the intersite transitions by Mn e_g electrons allowed us to estimate the effective intra-atomic Coulomb interaction, the Hund exchange coupling, and the Jahn-Teller splitting energy between e_g orbitals in LaMnO_3. This study identifies the lowest-energy optical transition at 2 eV as an intersite d-d transition, whose energy is substantially reduced compared to that obtained from the bare intra-atomic Coulomb interaction., Comment: 10 pages, 14 figures

More discussion from the theory is suggested, Comment: This paper has been withdrawn

Magnetic rare earths R have been proven to have a significant effect on the multiferroic properties of the orthorhombic manganites RMnO3. A re-examination of previous results from synchrotron based x-ray scattering experiments suggests that symmetric exchange striction between neighboring R and Mn ions may account for the enhancement of the ferroelectric polarization in DyMnO3 as well as the magnetic-field induced ferroelectricity in GdMnO3. In general, adding a second magnetic species to a multiferroic material may be a route to enhance its ferroelectric properties., Comment: Contribution to ICM 2009; accepted for publication in Journal of Physics: Conference Series

X-ray resonant magnetic scattering studies of rare earth magnetic ordering were performed on perovskite manganites RMnO3 (R = Dy, Gd) in an applied magnetic field. The data reveal that the field-induced three-fold polarization enhancement for H || a (H approx. 20 kOe) observed in DyMnO3 below 6.5 K is due to a re-emergence of the Mn-induced Dy spin order with propagation vector k(Dy) = k(Mn) = 0.385 b*, which accompanies the suppression of the independent Dy magnetic ordering, k(Dy) = 1/2 b*. For GdMnO3, the Mn-induced ordering of Gd spins is used to track the Mn-ordering propagation vector. The data confirm the incommensurate ordering reported previously, with k(Mn) varying from 0.245 to 0.16 b* on cooling from T_N(Mn) down to a transition temperature T'. New superstructure reflections which appear below T' suggest a propagation vector k(Mn) = 1/4 b* in zero magnetic field, which may coexist with the previously reported A-type ordering of Mn. The Gd spins order with the same propagation vector below 7 K. Within the ordered state of Gd at T = 1.8 K we find a phase boundary for an applied magnetic field H || b, H = 10 kOe, which coincides with the previously reported transition between the ground state paraelectric and the ferroelectric phase of GdMnO3. Our results suggest that the magnetic ordering of Gd in magnetic field may stabilize a cycloidal ordering of Mn that, in turn, produces ferroelectricity., Comment: 8 Figures, v2: improved figure layout

Using in-field single crystal neutron diffraction we have determined the magnetic structure of TbMnO3 in the high field P||a phase. We unambiguously establish that the ferroelectric polarization arises from a cycloidal Mn spins ordering, with spins rotating in the ab plane. Our results demonstrate directly that the flop of the ferroelectric polarization in TbMnO3 with applied magnetic field is caused from the flop of the Mn cycloidal plane., Comment: 5 pages, 3 figures

At ambient pressure CaFe2As2 has been found to undergo a first order phase transition from a high temperature, tetragonal phase to a low temperature orthorhombic / antiferromagnetic phase upon cooling through T ~ 170 K. With the application of pressure this phase transition is rapidly suppressed and by ~ 0.35 GPa it is replaced by a first order phase transition to a low temperature collapsed tetragonal, non-magnetic phase. Further application of pressure leads to an increase of the tetragonal to collapsed tetragonal phase transition temperature, with it crossing room temperature by ~ 1.7 GPa. Given the exceptionally large and anisotropic change in unit cell dimensions associated with the collapsed tetragonal phase, the state of the pressure medium (liquid or solid) at the transition temperature has profound effects on the low temperature state of the sample. For He-gas cells the pressure is as close to hydrostatic as possible and the transitions are sharp and the sample appears to be single phase at low temperatures. For liquid media cells at temperatures below media freezing, the CaFe2As2 transforms when it is encased by a frozen media and enters into a low temperature multi-crystallographic-phase state, leading to what appears to be a strain stabilized superconducting state at low temperatures., Comment: review for Special Physica C issue

Inelastic neutron scattering measurements of CaFe2As2 under applied hydrostatic pressure show that the antiferromagnetic spin fluctuations observed in the ambient pressure, paramagnetic, tetragonal (T) phase are strongly suppressed, if not absent, in the collapsed tetragonal (cT) phase. These results are consistent with a quenched Fe moment in the cT phase and the strong decrease in resistivity observed upon crossing the boundary from the T to cT phase. The suppression or absence of static antiferromagnetic order and dynamic spin fluctuations in the non-superconducting cT phase supports the notion of a coupling between spin fluctuations and superconductivity in the iron arsenides., Comment: 14 pages, 3 figures

Anomalous low temperature electronic and structural behaviour has been discovered in PbRuO3. The structure (space group Pnma, a = 5.56314(1), b = 7.86468(1), c = 5.61430(1) A) and metallic conductivity at 290 K are similar to those of SrRuO3 and other ruthenate perovskites, but a sharp metal-insulator transition at which the resistivity increases by four orders of magnitude is discovered at 90 K. This is accompanied by a first order structural transition to an Imma phase (a = 5.56962(1), b = 7.74550(1), c = 5.66208(1) A at 25 K) that shows a coupling of Ru4+ 4d orbital order to distortions from Pb2+ 6s6p orbital hybridization. The Pnma to Imma transition is an unconventional reversal of the group-subgroup symmetry relationship. No long range magnetic order is evident down to 1.5 K. Electronic structure calculations show that hybridization of Pb 6s6p and Ru 4d orbitals and strong spin-orbit coupling stabilise this previously hidden ground state for ruthenate perovskites

The crystal and magnetic structures of the spinel compounds ZnCr$_2$S$_4$ and ZnCr$_2$Se$_4$ were investigated by high resolution powder synchrotron and neutron diffraction. ZnCr$_2$Se$_4$ exhibits a first order phase transition at $T_N=21$ K into an incommensurate helical magnetic structure. Magnetic fluctuations above $T_N$ are coupled to the crystal lattice as manifested by negative thermal expansion. Both, the complex magnetic structure and the anomalous structural behavior can be related to magnetic frustration. Application of an external magnetic field shifts the ordering temperature and the regime of negative thermal expansion towards lower temperatures. Thereby, the spin ordering changes into a conical structure. ZnCr$_2$S$_4$ shows two magnetic transitions at $T_{N1}=15$ K and $T_{N2}=8$ K that are accompanied by structural phase transitions. The crystal structure transforms from the cubic spinel-type (space group $Fd$\={3}$m$) at high temperatures in the paramagnetic state, via a tetragonally distorted intermediate phase (space group $I4_1$ / $amd$) for $T_{N2} < T < T_{N1}$ into a low temperature orthorhombic phase (space group $I m m a$) for $T < T_{N2}$. The cooperative displacement of sulfur ions by exchange striction is the origin of these structural phase transitions. The low temperature structure of ZnCr$_2$S$_4$ is identical to the orthorhombic structure of magnetite below the Verwey transition. When applying a magnetic field of 5 T the system shows an induced negative thermal expansion in the intermediate magnetic phase as observed in ZnCr$_2$Se$_4$., Comment: 11 pages, 13 figures, to be published in PRB

Single crystal neutron and high-energy x-ray diffraction have identified the phase lines corresponding to transitions between the ambient-pressure tetragonal (T), the antiferromagnetic orthorhombic (O) and the non-magnetic collapsed tetragonal (cT) phases of CaFe2As2. We find no evidence of additional structures for pressures up to 2.5 GPa (at 300 K). Both the T-cT and O-cT transitions exhibit significant hysteresis effects and we demonstrate that coexistence of the O and cT phases can occur if a non-hydrostatic component of pressure is present. Measurements of the magnetic diffraction peaks show no change in the magnetic structure or ordered moment as a function of pressure in the O phase and we find no evidence of magnetic ordering in the cT phase. Band structure calculations show that the transition results in a strong decrease of the iron 3d density of states at the Fermi energy, consistent with a loss of the magnetic moment., Comment: List of authors in metadata and typos in labeling of inset in Fig. 1(a) corrected. One ref. added. No other changes

We report the structure and magnetism of PrOFeAs, one of the parent phases of the newly discovered Fe-As superconductors, as measured by neutron powder diffraction. In common with other REOFeAs materials, a tetragonal-orthorhombic phase transition is found on cooling below 136 K and striped Fe magnetism with $k =$(1,0,1) is detected below $\sim$ 85 K. Our magnetic order parameter measurements show that the ordered Fe moment along the a axis reaches a maximum at $\sim$ 40 K, below which an anomalous expansion of the c axis sets in, which results in a negative thermal volume expansion of 0.015 % at 2 K. We propose that this effect, which is suppressed in superconducting samples, is driven by a delicate interplay between Fe and Pr ordered moments.

Recent investigations of the superconducting iron-arsenide families have highlighted the role of pressure, be it chemical or mechanical, in fostering superconductivity. Here we report that CaFe2As2 undergoes a pressure-induced transition to a non-magnetic, volume "collapsed" tetragonal phase, which becomes superconducting at lower temperature. Spin-polarized total-energy calculations on the collapsed structure reveal that the magnetic Fe moment itself collapses, consistent with the absence of magnetic order in neutron diffraction., Comment: accepted for publication in Phys. Rev. B

Neutron diffraction measurements of a high quality single crystal of CaFe2As2 are reported. A sharp transition was observed between the high temperature tetragonal and low temperature orthorhombic structures at TS = 172.5K (on cooling) and 173.5K (on warming). Coincident with the structural transition we observe a rapid, but continuous, ordering of the Fe moments, in a commensurate antiferromagnetic structure is observed, with a saturated moment of 0.80(5)muB/Fe directed along the orthorhombic a-axis. The hysteresis of the structural transition is 1K between cooling and warming and is consistent with previous thermodynamic, transport and single crystal x-ray studies. The temperature onset of magnetic ordering shifts rigidly with the structural transition providing the clearest evidence to date of the coupling between the structural and magnetic transitions in this material and the broader class of iron arsenides., Comment: submitted to PRB

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., Comment: 12 pages, 15 figures, 2 references added

The field-induced multiferroic transition in TbMnO3 has been studied by neutron scattering. Apart strong hysteresis, the magnetic transition associated with the flop of electronic polarization exhibits a memory effect: after a field sweep, TbMnO3 does not exhibit the same phase as that obtained by zero-field cooling. The strong changes in the magnetic excitations across the transition perfectly agree with a rotation of the cycloidal spiral plane indicating that the inverse Dzyaloshinski-Moriya coupling causes the giant magnetoelectric effect at the field-induced transition. The analysis of the zone-center magnetic excitations identifies the electromagnon of the multiferroic high-field phase., Comment: 4 pages, 4 figures

We have utilized neutron powder diffraction to probe the crystal structure of layered Na$_{x}$CoO$_{2}$ near the half doping composition of $x=$0.46 over the temperature range of 2 to 600K. Our measurements show evidence of a dynamic transition in the motion of Na-ions at 300K which coincides with the onset of a near zero thermal expansion in the in-plane lattice constants. The effect of the Na-ordering on the CoO$_{2}$ layer is reflected in the octahedral distortion of the two crystallographically inequivalent Co-sites and is evident even at high temperatures. We find evidence of a weak charge separation into stripes of Co$^{+3.5+\epsilon}$ and Co$^{+3.5-\epsilon}$, $\epsilon\sim0.06e$ below \Tco=150K. We argue that changes in the Na(1)-O bond lengths observed at the magnetic transition at \tm=88K reflect changes in the electronic state of the CoO$_{2}$ layer, Comment: 7 pages, 6 figures, in press Phys. Rev. B

We report on diffraction measurements on multiferroic TbMnO3 which demonstrate that the Tb- and Mn-magnetic orders are coupled below the ferroelectric transition TFE = 28 K. For T < TFE the magnetic propagation vectors (tau) for Tb and Mn are locked so that tauTb = tauMn, while below TNTb = 7 K we find that tauTb and tauMn lock-in to rational values of 3/7 b* and 2/7 b*, respectively, and obey the relation 3tauTb - tauMn = 1. We explain this novel matching of wave vectors within the frustrated ANNNI model coupled to a periodic external field produced by the Mn-spin order. The tauTb = tauMn behavior is recovered when Tb magnetization is small, while the tauTb = 3/7 regime is stabilized at low temperatures by a peculiar arrangement of domain walls in the ordered state of Ising-like Tb spins., Comment: 5 pages, 3 figures

Ferroelectric spiral magnets DyMnO3 and TbMnO3 show similar behavior of electric polarization in applied magnetic fields. Studies of the field dependence of lattice modulations on the contrary show a completely different picture. Whereas in TbMnO3 the polarization flop from P||c to P||a is accompanied by a sudden change from incommensurate to commensurate wave vector modulation, in DyMnO3 the wave vector varies continuously through the flop transition. This smooth behavior may be related to the giant magnetocapacitive effect observed in DyMnO3.

We present measurements of the thermal conductivity $\kappa $ and the thermal expansion $\alpha$ of NdMnO$_3$ and TbMnO$_3$. In both compounds a splitting of the $4f$ multiplet of the $R^{3+}$ ion causes Schottky contributions to $\alpha$. In TbMnO$_3$ this contribution arises from a crystal-field splitting, while in NdMnO$_3$ it is due to the Nd-Mn exchange coupling. Another consequence of this coupling is a strongly enhanced canting of the Mn moments. The thermal conductivity is greatly suppressed in both compounds. The main scattering process at low temperatures is resonant scattering of phonons between different energy levels of the $4f$ multiplets, whereas the complex 3d magnetism of the Mn ions is of minor importance., Comment: 9 pages including 6 figures

The (H,T)-phase diagram of the multiferroic perovskite TbMnO$_3$ was studied by high-resolution thermal expansion $\alpha(T)$ and magnetostriction $\Delta L(H)/L$ measurements. Below $T_{N}\simeq 42$ K, TbMnO$_3$ shows antiferromagnetic order, which changes at $T_{FE}\simeq 28$ K where simultaneously a spontaneous polarization $P||c$ develops. Sufficiently high magnetic fields applied along $a$ or $b$ induce a polarization flop to $P||a$. We find that all of these transitions are strongly coupled to the lattice parameters. Thus, our data allow for a precise determination of the phase boundaries and also yield information about their uniaxial pressure dependencies. The strongly hysteretic phase boundary to the ferroelectric phase with $P||a$ is derived in detail. Contrary to previous reports, we find that even in high magnetic fields there are no direct transitions from this phase to the paraelectric phase. We also determine the various phase boundaries in the low-temperature region related to complex reordering transitions of the Tb moments., Comment: 17 pages including 9 figures

Neutron elastic, inelastic and high energy x-ray scattering techniques are used to explore the nature of the polaron order and dynamics in La0.7Ca0.3MnO3. Static polaron correlations develop within a narrow temperature regime as the Curie temperature is approached from low temperatures, with a nanoscale correlation length that is only weakly temperature dependent. The static nature of these short-range polaron correlations indicates the presence of a glass-like state, similar to the observations for the bilayer manganite in the metallic-ferromagnetic doping region. In addition to this elastic component, inelastic scattering measurements reveal dynamic correlations with a comparable correlation length, and with an energy distribution that is quasielastic. The elastic component disappears at a higher temperature T*, above which the correlations are purely dynamic. The overall behavior bears a remarkable resemblance to the magnetic fluctuation spectrum recently observed in underdoped cuprates., Comment: 11 pages, 7 figures, submitted to Phys. Rev. B

The magnetic excitations in multiferroic TbMnO3 have been studied by inelastic neutron scattering in the spiral and sinusoidally ordered phases. At the incommensurate magnetic zone center of the spiral phase, we find three low-lying magnons whose character has been fully determined using neutron-polarization analysis. The excitation at the lowest energy is the sliding mode of the spiral, and two modes at 1.1 and 2.5meV correspond to rotations of the spiral rotation plane. These latter modes are expected to couple to the electric polarization. The 2.5meV-mode is in perfect agreement with recent infra-red-spectroscopy data giving strong support to its interpretation as an hybridized phonon-magnon excitation., Comment: 4 pages, 4 figures

The antiferromagnetic - ferromagnetic phase transition in YBaCo2O5.50 and YBaCo2O5.44 cobaltites with different types of oxygen-ion ordering in the [YO0.5/0.44] layers has been studied by neutron powder diffraction. Using the magnetic symmetry arguments in combination with group-theoretical analysis, the crystal and magnetic structures above and below the phase transformation temperature, Ti, were determined and successfully refined. In both cases, the proposed models involve a spin-state ordering between diamagnetic (t2g6eg0, S = 0) and paramagnetic (t2g4eg2, S = 2) Co3+ ions with octahedral coordination. Electronic ordering results in a nonzero spontaneous magnetic moment in the high-temperature magnetic phases with isotropic negative exchange interactions. In the case of YBaCo2O5.5, the phase transformation does not change Pmma symmetry of the crystal structure. The wave vectors of magnetic structures above and below Ti are k = 0 and k = c*/2, respectively. In the case of YBaCo2O5.44, a crossover P4/nmm - I4/mmm was involved to solve the low-temperature magnetic structure. The wave vectors in both high-temperature and low-temperature magnetic phases are k = 0. Mechanisms of the phase transformation in both compositions are discussed in the light of obtained magnetic structures. The proposed spin configurations were compared with other models reported in literature., Comment: 40 pages, 16 figures, 4 tables

Neutron powder diffraction and single crystal x-ray resonant magnetic scattering measurements suggest that Dy plays an active role in enhancing the ferroelectric polarization in multiferroic DyMnO3 above TNDy = 6.5 K. We observe the evolution of an incommensurate ordering of Dy moments with the same periodicity as the Mn spiral ordering. It closely tracks the evolution of the ferroelectric polarization which reaches a maximum value of 0.2 muC/m^2. Below TNDy, where Dy spins order commensurately, the polarization decreases to values similar for those of TbMnO3.

Synchrotron x-ray diffraction and resonant magnetic scattering experiments on single crystal DyMnO3 have been carried out between 4 and 40 K. Below TN(Dy) = 5K, the Dy magnetic moments order in a commensurate structure with propagation vector 0.5 b*. Simultaneous with the Dy magnetic ordering, an incommensurate lattice modulation with propagation vector 0.905 b* evolves while the original Mn induced modulation is suppressed and shifts from 0.78 b* to 0.81 b*. This points to a strong interference of Mn and Dy induced structural distortions in DyMnO3 besides a magnetic coupling between the Mn and Dy magnetic moments., Comment: submitted to Phys. Rev. B Rapid Communications

Using Angle-Resolved Photoemission (ARPES), we present the first observation of sharp quasiparticle-like peaks in a CMR manganite. We focus on the ($\pi$,0) regions of k-space and study their electronic scattering rates and dispersion kinks, uncovering the critical energy scales, momentum scales, and strengths of the interactions that renormalize the electrons. To identify these bosons we measured phonon dispersions in the energy range of the kink by inelastic neutron scattering (INS), finding a good match in both energy and momentum to the oxygen bond-stretching phonons.

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., Comment: 6 pages, 4 figures

We present comprehensive neutron scattering studies of nonsuperconducting and superconducting electron-doped Pr0.88LaCe0.12CuO4(PLCCO). At zero field, the transition from antiferromagnetic (AF) as-grown PLCCO to superconductivity without static antiferromagnetism can be achieved by annealing the sample in pure Ar at different temperatures, which also induces an epitaxial (Pr,La,Ce)2O3 phase as an impurity. When the superconductivity first appears in PLCCO, a quasi-two-dimensional (2D) spin-density-wave (SDW) order is also induced, and both coexist with the residual three-dimensional (3D) AF state. A magnetic field applied along the [-1,1,0] direction parallel to the CuO2 plane induces a ``spin-flop'' transition, where the noncollinear AF spin structure of PLCCO is transformed into a collinear one. The spin-flop transition is continuous in semiconducting PLCCO, but gradually becomes sharp with increasing doping and the appearance of superconductivity. A c-axis aligned magnetic field that suppresses the superconductivity also enhances the quasi-2D SDW order at (0.5,0.5,0) for underdoped PLCCO. However, there is no effect on the 3D AF order in either superconducting or nonsuperconducting samples. Since the same field along the [-1,1,0] direction in the CuO2 plane has no (or little) effect on the superconductivity, (0.5,0.5,0) and (Pr,La,Ce)2O3 impurity positions, we conclude that the c-axis field-induced effect is intrinsic to PLCCO and arises from the suppression of superconductivity., Comment: 17 pages, 21 figures

Perovskite manganite compounds such as Pr_(1-x)(Ca_(1-y)Sr_y)_xMn3 can be tuned to exhibit a metastable ground state where two magnetic/crystallographic phases coexist in zero magnetic field. Field-dependent neutron diffraction measurements on both poly- and single-crystal samples with a range of Pr, Ca, and Sr dopings(0.3

We have used electron and neutron powder diffraction to elucidate the structural properties of superconducting \NaD. Our measurements show that our superconducting sample exhbits a number of supercells ranging from ${1/3}a^{*}$ to ${1/15}a^{*}$, but the most predominant one, observed also in the neutron data, is a double hexagonal cell with dimensions \dhx. Rietveld analysis reveals that \deut\space is inserted between CoO$_{2}$ sheets as to form a layered network of NaO$_{6}$ triangular prisms. Our model removes the need to invoke a 5K superconducting point compound and suggests that a solid solution of Na is possible within a constant amount of water $y$., Comment: 4 pages, 3 figures

We have studied the superconducting phase diagram of \NaH\space as a function of electronic doping, characterizing our samples both in terms of Na content $x$ and the Co valence state. Our findings are consistent with a recent report that intercalation of \oxp\space ions into Na$_{x}$CoO$_{2}$, together with water, act as an additional dopant indicating that Na sub-stochiometry alone does not control the electronic doping of these materials. We find a superconducting phase diagram where optimal \Tc\space is achieved through a Co valence range of 3.24 - 3.35, while \Tc\space decreases for materials with a higher Co valence. The critical role of dimensionality in achieving superconductivity is highlighted by similarly doped non-superconducting anhydrous samples, differing from the superconducting hydrate only in inter-layer spacing. The increase of the interlayer separation between CoO$_{2}$ sheets as Co valence is varied into the optimal \Tc\space region is further evidence for this criticality., Comment: Paper updated on 29/10/2004, 4 pages, 4 figures. Physical Review Letters (in press)

Mang et al. report the observation of a cubic (Nd,Ce)2O3 impurity phase grown epitaxially in annealed samples of electron-doped Nd2-xCexCuO4 (NCCO) and argue that our observed magnetic scattering in NCCO [Nature 423,522(2003)]is due entirely to (Nd,Ce)2O3. Here we show why this is incorrect., Comment: 1 page

We have measured the effect of a c-axis aligned magnetic field on the long-range magnetic order of insulating Nd2CuO4, as-grown nonsuperconducting and superconducting Nd1.85Ce0.15CuO4. On cooling from room temperature, Nd2CuO4 goes through a series of antiferromagnetic (AF) phase transitions with different noncollinear spin structures. In all phases of Nd2CuO4, we find that the applied c-axis field induces a canting of the AF order but does not alter the basic zero-field noncollinear spin structures. Similar behavior is also found in as-grown nonsuperconducting Nd1.85Ce0.15CuO4. These results contrast dramatically with those of superconducting Nd1.85Ce0.15CuO4, where a c-axis aligned magnetic field induces a static, anomalously conducting, long-range ordered AF state. We confirm that the annealing process necessary to make superconducting Nd1.85Ce0.15CuO4 also induces epitaxial, three-dimensional long-range ordered cubic (Nd,Ce)2O3 as an impurity phase. In addition, the annealing process makes a series of quasi two-dimensional superlattice reflections associated with lattice distortions of Nd1.85Ce0.15CuO4 in the CuO2 plane. While the application of a magnetic field will induce a net moment in the impurity phase, we determine its magnitude and eliminate this as a possibility for the observed magnetic field-induced effect in superconducting Nd1.85Ce0.15CuO4., Comment: 12 pages, 10 figures, to be published in Phys. Rev. B

A detailed investigation of mesoscopic magnetic and crystallographic phase separation in Ca(1-x)La(x)MnO3, 0.00<=x<=0.20, is reported. Neutron powder diffraction and DC-magnetization techniques have been used to isolate the different roles played by electrons doped into the eg level as a function of their concentration x. The presence of multiple low-temperature magnetic and crystallographic phases within individual polycrystalline samples is argued to be an intrinsic feature of the system that follows from the shifting balance between competing FM and AFM interactions as a function of temperature. FM double-exchange interactions associated with doped eg electrons are favored over competing AFM interactions at higher temperatures, and couple more strongly with the lattice via orbital polarization. These FM interactions thereby play a privileged role, even at low eg electron concentrations, by virtue of structural modifications induced above the AFM transition temperatures., Comment: 8 pages, 7 figures

The phase diagram of Pr0.65(CaySr1-y)0.35MnO3, 0.6 <= y <= 0.8, has been determined by neutron diffraction, magnetization and electrical conductivity measurements in order to investigate the nature of the transition between ferromagnetic metallic and charge-ordered insulating states near y=0.75. Two possible scenarios for this transition have been proposed: a "quantum critical point"-like feature, near which an associated charge-disordered paramagnetic phase is present, or a phase coexistence region. We demonstrate that the latter case is true, phase segregation occurring on a mesoscopic/macroscopic length-scale (several hundred Angstroms to several microns). Our results show that no significant amount of the charge-disordered paramagnetic phase is present at low temperatures. Our data also indicate that the charge-ordered insulator to ferromagnetic metal phase boundary is temperature as well as composition-dependent., Comment: Submitted to Phys. Rev. B

Neutron scattering measurements on a bilayer manganite near optimal doping show that the short-range polarons correlations are completely dynamic at high T, but then freeze upon cooling to a temperature T* 310 K. This glass transition suggests that the paramagnetic/insulating state arises from an inherent orbital frustration that inhibits the formation of a long range orbital- and charge-ordered state. Upon further cooling into the ferromagnetic-metallic state (Tc=114 K), where the polarons melt, the diffuse scattering quickly develops into a propagating, transverse optic phonon., Comment: 4 pages, 4 figures. Physical Review Letters (in Press)

A system of strongly-interacting electron-lattice polarons can exhibit charge and orbital order at sufficiently high polaron concentrations. In this study, the structure of short-range polaron correlations in the layered colossal magnetoresistive perovskite manganite, La1.2Sr1.8Mn2O7, has been determined by a crystallographic analysis of broad satellite maxima observed in diffuse X-ray and neutron scattering data. The resulting q=(0.3,0,1) modulation is a longitudinal octahedral-stretch mode, consistent with an incommensurate Jahn-Teller-coupled charge-density-wave fluctuations, that implies an unusual orbital-stripe pattern parallel to the <100> directions., Comment: Reformatted with RevTex