arXiv subjects

P. G. Radaelli

Publications and source records attributed to P. G. Radaelli.

At least 55 records · Page 3Linked to original sources

arXiv2007

Orbital degeneracy removed by charge order in triangular antiferromagnet AgNiO2

We report a high-resolution neutron diffraction study on the orbitally-degenerate spin-1/2 hexagonal antiferromagnet AgNiO2. A structural transition to a tripled unit cell with expanded and contracted NiO6 octahedra indicates root(3) x root(3) charge order on the Ni triangular lattice. This suggests charge order as a possible mechanism of lifting the orbital degeneracy in the presence of charge fluctuations, as an alternative to Jahn-Teller distortions. A novel magnetic ground state is observed at base temperatures with the electron-rich S = 1 Ni sites arranged in alternating ferromagnetic rows on a triangular lattice, surrounded by a honeycomb network of non-magnetic and metallic Ni ions. We also report first-principles band-structure calculations that explain microscopically the origin of these phenomena.

cond-mat.str-el↗

arXiv2007

Symmetry constraints on the electrical polarization in novel multiferroic materials

The symmetry conditions for the development of a macroscopic electrical polarization as a secondary order parameter to a magnetic ordering transition, and the constraints on the direction of the polarization vector, are determined by a non-conventional application of the theory of irreducible co-representations. In our approach, which is suitable for both magnetic and structural modulations, anti-unitary operators are employed to describe symmetry operations that exchange the propagation vector $\textbf{k}$ with $\textbf{-k}$, rather than operations combined with time-reversal as in classical \textit{corep} analysis. Unlike the conventional irreducible representations, co-representations can capture the full symmetry properties of the system even if the propagation vector is in the interior of the Brillouin zone. It is shown that ferroelectricity can develop even for a completely collinear structure, and that helical and cycloidal magnetic structures are not always polar. In some cases, symmetry allows the development of polarization parallel to the magnetic propagation vector. Our analysis also highlights the unique importance of magnetic commensurability, enabling one to derive the different symmetry properties of equivalent commensurate and incommensurate phases even for a completely generic propagation vector.

cond-mat.str-el↗

arXiv2007

Structural anomalies at the magnetic transition in centrosymmetric BiMnO$_3$

The structural properties of BiMn$O_3$ were determined from neutron powder diffraction data as a function of temperature and magnetic field. The structure at all temperatures was found to be centrosymmetric with space group $C2/c$, which is incompatible with ferroelectricity. At T$_C\simeq 100 K$, we observed the onset of a large magnetoelastic strain, proportional to the square of the magnetization. We interpret this structural rearrangement, together with the previously observed magnetodielectric anomalies, as due to the need to optimize the partially frustrated magnetic interactions.

cond-mat.str-el↗

arXiv2006

Understanding the insulating phase in CMR manganites: Shortening of the Jahn-Teller long-bond across the phase diagram of La_{1-x} Ca_x Mn O_3

The detailed evolution of the magnitude of the local Jahn-Teller (JT) distortion in La_{1-x} Ca_x Mn O_3 is obtained across the phase diagram for 0 < x < 0.5 from high quality neutron diffraction data using the atomic pair distribution function (PDF) 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.

cond-mat.str-el↗

arXiv2006

Magnetoelastic coupling across the metamagnetic transition in Ca$_{2-x}$Sr$_x$RuO$_4$ (0.2 < x < 0.5)

The magnetoelastic coupling in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ and in Ca$_{1.5}$Sr$_{0.5}$RuO$_4$ has been studied combining high-resolution dilatometer and diffraction techniques. Both compounds exhibit strong anomalies in the thermal-expansion coefficient at zero and at high magnetic field as well as an exceptionally large magnetostriction. All these structural effects, which are strongest in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$, point to a redistribution of electrons between the different $t_{2g}$ orbitals tuned by temperature and magnetic field. The temperature and the field dependence of the thermal-expansion anomalies in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ yield evidence for a critical end-point lying close to the low-temperature metamagnetic transition; however, the expected scaling relations are not well fulfilled.

cond-mat.str-el↗

arXiv2006

Structural phase transition and magnetism in hexagonal srmno

The structural and magnetic properties of the hexagonal four-layer form of SrMnO$_3$ have been investigated by combining magnetization measurements, electron diffraction and high-resolution synchrotron X-ray and neutron powder diffraction. Below 350K, there is subtle structural phase transition from hexagonal symmetry (space group $P6_3/mmc$) to orthorhombic symmetry (space group $C222_1$) where the hexagonal metric is preserved. The second-order phase transition involves a slight tilting of the corner-sharing Mn$_{2}$O$_{9}$ units composed of 2 face-sharing MnO$_6$ octahedra and the associated displacement of Sr$^{2+}$ cations. The phase transition is described in terms of symmetry-adapted displacement modes of the high symmetry phase. Upon further cooling, long range magnetic order with propagation vector $\mathbf{k}=(0,0,0)$ sets in below 300K. The antiferromagnetic structure, analyzed using representation theory, shows a considerably reduced magnetic moment indicating the crucial role played by direct exchange between Mn centers of the Mn$_{2}$O$_{9}$ units.

cond-mat.str-el↗

arXiv2006

Non-collinear long-range magnetic ordering in HgCr2S4

The low-temperature magnetic structure of \HG has been studied by high-resolution powder neutron diffraction. Long-range incommensurate magnetic order sets in at T$_N\sim$22K with propagation vector \textbf{k}=(0,0,$\sim$0.18). On cooling below T$_N$, the propagation vector increases and saturates at the commensurate value \textbf{k}=(0,0,0.25). The magnetic structure below T$_N$ consists of ferromagnetic layers in the \textit{ab}-plane stacked in a spiral arrangement along the \textit{c}-axis. Symmetry analysis using corepresentations theory reveals a point group symmetry in the ordered magnetic phase of 422 (D$_4$), which is incompatible with macroscopic ferroelectricity. This finding indicates that the spontaneous electric polarization observed experimentally cannot be coupled to the magnetic order parameter.

cond-mat.mtrl-sci↗

arXiv2006

Competing magnetic interactions in the extended Kagome system YBaCo4O7

YBaCo4O7 belongs to a new class of geometrically frustrated magnets like the pyrochlores, in which Co-spins occupy corners of tetrahedra. The structure can be viewed as an alternating stacking of Kagome and triangular layers. Exactly half of the triangular units of the Kagome plane are capped by Co ions to form columns running perpendicular to the Kagome sheets. Neutron powder diffraction reveals a broad temperature range of diffuse magnetic scattering, followed by long range magnetic ordering below 110K. A unique low-temperature magnetic structure simultaneously satisfies an S=0 arrangement in the uncapped triangular units and antiferromagnetic coupling along the columns. A spin reorientation above 30K tracks the relative strengths of the in-plane and out-of-plane interactions.

cond-mat.mtrl-sci↗

arXiv2005

Ferroelectricity induced by acentric spin-density waves in YMn$_2$O$_5$

The commensurate and incommensurate magnetic structures of the magnetoelectric system YMn$_{2}$O$_{5}$, as determined from neutron diffraction, were found to be spin-density waves lacking a global center of symmetry. We propose a model, based on a simple magneto-elastic coupling to the lattice, which enables us to predict the polarization based entirely on the observed magnetic structure. Our data accurately reproduce the temperature-dependence of the spontaneous polarization, in particular its sign reversal at the commensurate-incommensurate transition.

cond-mat.mtrl-sci↗

arXiv2005

Spin structure and magnetic frustration in multiferroic RMn2O5 (R = Tb, Ho, Dy)

We have studied the crystal and magnetic structures of the magnetoelectric materials RMn2O5 (R = Tb, Ho, Dy) using neutron diffraction as a function of temperature. All three materials display incommensurate antiferromagnetic ordering below 40 K, becoming commensurate on further cooling. For R = Tb, Ho, a commensurate-incommensurate transition takes place at low temperatures. The commensurate magnetic structures have been solved and are discussed in terms of competing exchange interactions. The spin configuration within the ab plane is essentially the same for each system, and the radius of R determines the sign of the magnetic exchange between adjacent planes. The inherent magnetic frustration in these materials is lifted by a small lattice distortion, primarily involving shifts of the Mn3+ cations and giving rise to a canted antiferroelectric phase.

cond-mat.str-el↗

arXiv2004

The structure of intercalated water in superconducting Na$_{0.35}$CoO$_{2}\cdot$1.37D$_{2}$O: Implications for the superconducting phase diagram

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 $y$.

cond-mat.supr-con↗

arXiv2003

Spin singlet formation in MgTi$_2$O$_4$: evidence of a helical dimerization pattern

The transition metal spinel MgTi$_2$O$_4$ undergoes a metal-insulator transition on cooling below $T_{M-I} = 260$ K. A sharp reduction of the magnetic susceptibility below $T_{M-I}$ suggests the onset of a magnetic singlet state. Using high-resolution synchrotron and neutron powder diffraction, we have solved the low-temperature crystal structure of MgTi$_2$O$_4$, which is found to contain dimers with short Ti-Ti distances (the locations of the spin singlets) alternating with long bonds to form helices. Band structure calculations based on hybrid exchange density functional theory show that, at low temperatures, MgTi$_2$O$_4$ is an orbitally ordered band insulator.

cond-mat↗

arXiv2003

Temperature-induced barium de-trapping from a double-well potential in Ba6Ge25

The crystal structure of barium-germanium clathrate Ba6Ge25 was studied using neutron powder diffraction in the temperature range 20-300K. The compound was found to be cubic (S.G. P4_1 23) in the entire temperature range. However, the fully-ordered model of the crystal structure (no split sites) is marginal at room temperature, and clearly fails at low temperature. A much better description of the crystal structure below 250K is given in terms of two split Ba sites, with random occupancies, for two out of three types of cages present in the Ba6Ge25 structure. The Ba atoms were found to interact strongly with the Ge host. The separation of the split Ba sites grows with decreasing temperature, with a sudden increase on cooling through the 200-250K temperature range, accompanied by an expansion of the entire crystal structure. We propose a simple model for this transition, based on temperature-induced de- trapping of Ba from a deep double-well potential. This transition is associated with sizeable anomalies in the transport and magnetic properties. The most significant of these effects, that is, the drop in electrical conductivity on cooling, can be easily explained within our model through the enhanced structural disorder, which would affect the relaxation time for all portions of the Fermi surface. We suggest that the other anomalies (increase in the absolute value of the negative Seebeck coefficient, decrease in the magnetic susceptibility) can be explained within the framework of the one-electron semi- classical model, without any need to invoke exotic electron-electron interaction mechanisms.

cond-mat.mtrl-sci↗

arXiv2002

X-ray-induced disordering of the dimerization pattern and apparent low-temperature enhancement of lattice symmetry in spinel CuIr$_2$S$_4$

At low temperatures, spinel CuIr$_2$S$_4$ is a charge-ordered spin-dimerized insulator with triclinic lattice symmetry. We find that x-rays induce a structural transition in which the local triclinic structure is preserved, but the average lattice symmetry becomes tetragonal. These structural changes are accompanied by a thousandfold reduction in the electrical resistivity. The transition is persistent, but the original state can be restored by thermal annealing. We argue that x-ray irradiation disorders the lattice dimerization pattern, producing a state in which the orientation of the dimers is preserved, but the translational long-range order is destroyed.

cond-mat↗

arXiv2002

Structural and magnetic ordering in Pr0.65(CaySr1-y)0.35MnO3: "quantum critical point" versus phase segregation scenarios

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.

cond-mat.str-el↗

arXiv2002

Large Anisotropic Thermal Expansion Anomaly near the Superconducting Transition Temperature in MgB2

An anisotropic lattice anomaly near the superconducting transition temperature, Tc, was observed in MgB2 by high-resolution neutron powder diffraction. The a-axis thermal expansion becomes negative near Tc, while the c-axis thermal expansion is unaffected. This is qualitatively consistent with a depletion of the boron-boron s-band as the superconducting gap opens, resulting in weaker bonding. However, the observed anomaly is much larger than predicted by the Ehrenfest relation, strongly suggesting that the phonon thermal expansion also changes sign, as commonly observed in hexagonal layered crystals. These two effects may be connected through subtle changes in the phonon spectrum at Tc.

cond-mat.supr-con↗

arXiv2001

Long Range Charge Ordering in Magnetite Below the Verwey Transition

The crystal structure of Fe3O4 below the 122 K Verwey transition has been refined using high-resolution X-ray and neutron powder diffraction data. The refinements give direct evidence for charge ordering (CO) over four independent octahedral Fe sites, two with a charge of +2.4 and the other two of +2.6. CO schemes consistent with our model do not meet the widely-accepted Anderson condition of minimum electrostatic repulsion. Instead we propose that CO is driven primarily by a [001] electronic instability, which opens a gap at the transition through a charge density wave mechanism.

cond-mat.str-el↗

arXiv2001

Local Atomic Strain in ZnSe(1-x)Te(x) from High Real Space Resolution Neutron Pair Distribution Function Measurements

High real-space resolution atomic pair distribution functions (PDFs) have been obtained from ZnSe(1-x)Te(x) using neutron powder diffraction. Distinct Zn-Se and Zn-Te nearest neighbor (nn) bonds, differing in length by delta_r= 0.14Angstroms, are resolved in the measured PDF allowing the evolution with composition of the individual bond-lengths to be studied. The local bond-lengths change much more slowly with doping than the average bond-length obtained crystallographically. The nn bond-length distributions are constant with doping but higher-neighbor pair distributions broaden significantly indicating that most of the strain from the alloying is accommodated by bond-bending forces in the alloy. The PDFs of alloys across the whole doping range are well fit using a model based on the Kirkwood potential. The resulting PDFs give excellent agreement with the measured PDFs over the entire alloy range with no adjustable parameters.

cond-mat.mtrl-sci↗