arXiv subjects

P. Manuel

Publications and source records attributed to P. Manuel.

At least 73 records · Page 4Linked to original sources

arXiv2018

Understanding the magnetism in noncentrosymmetric CeIrGe3: Muon spin relaxation and neutron scattering studies

The magnetic properties of a pressure induced noncentrosymmetric heavy-fermion superconductor CeIrGe$_3$ have been investigated by muon spin relaxation ($μ$SR), powder neutron diffraction (ND) and inelastic neutron scattering (INS) techniques at ambient pressure. For completeness we have also measured the ac magnetic susceptibility $χ_{\rm ac}(T)$, dc magnetic susceptibility $χ(T)$, dc isothermal magnetization $M(H)$ and heat capacity $C_{\rm p}(T,H)$ down to 2 K. CeIrGe$_{3}$ is known to exhibit pressure induced superconductivity ($T_{\rm c}\approx 1.5$ K) at a pressure of 20 GPa and antiferromagnetic ordering at 8.7 K, 4.7 K and 0.7 K at ambient pressure. Our $χ_{\rm ac}(T)$ and $χ(T)$ data show an additional anomaly near 6.2 K which is also captured in $C_{\rm p}(T)$ data. From $χ_{\rm ac}(T)$, $χ(T)$ and $C_{\rm p}(T)$ measurements we infer three antiferromagnetic transitions above 2 K at $T_{\rm N1}= 8.5$ K, $T_{\rm N2}= 6.0$ K and $T_{\rm N3}= 4.6$ K. Our $μ$SR study also confirms the presence of three transitions through the observation of one frequency for $T_{\rm N2} < T\leq T_{\rm N1}$, two frequencies for $T_{\rm N3} < T\leq T_{\rm N2}$ and three frequencies for $T\leq T_{\rm N3}$ in the oscillatory asymmetry. The ND data reveal an incommensurate nature of the magnetic ordering at $T=7$ K with the propagation vector k = (0,0,0.688(3)), and a commensurate magnetic structure at $T=1.5$ K with the propagation vector locked to the value k = (0,0,2/3) and magnetic moments oriented along the $c$ axis. The commensurate structure couples a macroscopic ferromagnetic component, resulting in a strong dependence of the lock-in transition temperature on external magnetic field. The INS data show two well defined crystal electric field (CEF) excitations arising from the CEF-split Kramers doublet ground state of Ce$^{3+}$.

cond-mat.str-el↗

arXiv2017

Strain and Magnetic Field Induced Spin-Structure Transitions in Multiferroic BiFeO3

The magnetic-field-dependent spin ordering of strained BiFeO3 films is determined using nuclear resonant scattering and Raman spectroscopy. The critical field required to destroy the cycloidal modulation of the Fe spins is found to be significantly lower than in the bulk, with appealing implications for field-controlled spintronic and magnonic devices.

cond-mat.mtrl-sci↗

arXiv2017

Magnetic excitations from the two-dimensional interpenetrating Cu framework in Ba$_2$Cu$_3$O$_4$Cl$_2$

We report detailed neutron scattering studies on Ba$_2$Cu$_3$O$_4$Cl$_2$. The compound consists of two interpenetrating sublattices of Cu, labeled as Cu$_{\rm A}$ and Cu$_{\rm B}$, each of which forms a square-lattice Heisenberg antiferromagnet. The two sublattices order at different temperatures and effective exchange couplings within the sublattices differ by an order of magnitude. This yields an inelastic neutron spectrum of the Cu$_{\rm A}$ sublattice extending up to 300 meV and a much weaker dispersion of Cu$_{\rm B}$ going up to around 20 meV. Using a single-band Hubbard model we derive an effective spin Hamiltonian. From this, we find that linear spin-wave theory gives a good description to the magnetic spectrum. In addition, a magnetic field of 10 T is found to produce effects on the Cu$_{\rm B}$ dispersion that cannot be explained by conventional spin-wave theory.

cond-mat.str-el↗

arXiv2017

Universal magneto-orbital ordering in the divalent $A$-site quadruple perovskite manganites $A$Mn$_7$O$_{12}$ ($A$ = Ca, Sr, Cd, and Pb)

Through analysis of variable temperature neutron powder diffraction data, we present solutions for the magnetic structures of SrMn$_7$O$_{12}$, CdMn$_7$O$_{12}$, and PbMn$_7$O$_{12}$ in all long-range ordered phases. The three compounds were found to have magnetic structures analogous to that reported for CaMn$_7$O$_{12}$. They all feature a higher temperature lock-in phase with \emph{commensurate} magneto-orbital coupling, and a delocked, multi-\textbf{k} magnetic ground state where \emph{incommensurate} magneto-orbital coupling gives rise to a constant-moment magnetic helix with modulated spin helicity. CdMn$_7$O$_{12}$ represents a special case in which the orbital modulation is commensurate with the crystal lattice and involves stacking of fully and partially polarized orbital states. Our results provide a robust confirmation of the phenomenological model for magneto-orbital coupling previously presented for CaMn$_7$O$_{12}$. Furthermore, we show that the model is universal to the $A^{2+}$ quadruple perovskite manganites synthesised to date, and that it is tunable by selection of the $A$-site ionic radius.

cond-mat.str-el↗

arXiv2017

Pr-magnetism in the quasi-skutterudite compound PrFe$_2$Al$_8$

The intermetallic compound \PFA\ that possesses a three-dimensional network structure of Al polyhedra centered at the transition metal element Fe and the rare earth Pr is investigated through neutron powder diffraction and inelastic neutron scattering in order to elucidate the magnetic ground state of Pr and Fe and the crystal field effects of Pr. Our neutron diffraction study confirms long-range magnetic order of Pr below $T_N $ = 4.5~K in this compound. Subsequent magnetic structure estimation reveals a magnetic propagation vector $k$ = ($\frac{1}{2}$~0~$\frac{1}{2}$) with a magnetic moment value of 2.5~$μ_\mathrm{B}$/Pr along the orthorhombic $c$-axis and evidence the lack of ordering in the Fe sublattice. The inelastic neutron scattering study reveals one crystalline electric field excitation near 19~meV at 5~K in \PFA. The energy-integrated intensity of the 19~meV excitation as a function of |$Q$| $(A^{-1})$ follows the square of the magnetic form factor of Pr$^{3+}$ thereby confirming that the inelastic excitation belongs to the Pr sublattice. The second sum rule applied to the dynamic structure factor indicates only 1.6(2)~$μ_\mathrm{B}$ evolving at the 19~meV peak compared to the 3.58~$μ_\mathrm{B}$ for free Pr$^{3+}$, indicating that the crystal field ground state is magnetic and the missing moment is associated with the resolution limited quasi-elastic line. The magnetic order occurring in Pr in \PFA\ is counter-intuitive to the symmetry-allowed crystal field level scheme, hence, is suggestive of exchange-mediated mechanisms of ordering stemming from the magnetic ground state of the crystal field levels.

cond-mat.str-el↗

arXiv2017

Classical Spin Nematic Transition in LiGa$_{0.95}$In$_{0.05}$Cr$_4$O$_8$

We present the results of a combined $^7$Li NMR and diffraction study on LiGa$_{0.95}$In$_{0.05}$Cr$_4$O$_8$, a member of LiGa$_{1-x}$In$_{x}$Cr$_4$O$_8$ "breathing" pyrochlore family. Via specific heat and NMR measurements, we find that the complex sequence of first-order transitions observed for $x=0$ is replaced by a single, apparently second-order transition at $T_f=11$ K. Neutron and X-ray diffraction rule out both structural symmetry lowering and magnetic long-range order as the origin of this transition. Instead, reverse Monte Carlo fitting of the magnetic diffuse scattering indicates that the low temperature phase may be described as a collinear spin nematic state, characterized by a quadrupolar order parameter. This state also shows signs of short range order between collinear spin arrangements on tetrahedra, revealed by mapping the reverse Monte Carlo spin configurations onto a three-state color model describing the manifold of nematic states.

cond-mat.str-el↗

arXiv2017

Evolution of spin correlations in SrDy2O4 in an applied magnetic field

The development of short- and long-range magnetic order induced in a frustrated zig-zag ladder compound SrDy2O4 by an applied field is studied using neutron diffraction techniques. In zero field, SrDy2O4 lacks long-range magnetic order down to temperatures as low as 60 mK, and the observed powder neutron diffraction (PND) patterns are dominated by very broad diffuse scattering peaks. Single crystal neutron diffraction reveals that the zero-field magnetic structure consists of a collection of antiferromagnetic chains running along the c axis and that there is very little correlation between the chains in the ab plane. In an applied magnetic field, the broad diffuse scattering features in PND are gradually replaced by much sharper peaks, however, the pattern remains rather complex, reflecting the highly anisotropic nature of SrDy2O4. Single crystal neutron diffraction shows that a moderate field applied along the b axis induces an up-up-down magnetic order associated with a 1/3-magnetisation plateau, in which magnetic correlation length in the ab plane is significantly increased, but it nevertheless remains finite. The resolution limited k = 0 peaks associated with a ferromagnetic arrangement appear in powder and single crystal neutron diffraction patterns in fields of 2.5 T and above.

cond-mat.str-el↗

arXiv2017

Temperature induced phase transition from cycloidal to collinear antiferromagnetism in multiferroic Bi$_{0.9}$Sm$_{0.1}$FeO$_3$ driven by $f$-$d$ induced magnetic anisotropy

In multiferroic BiFeO$_3$ a cycloidal antiferromagnetic structure is coupled to a large electric polarization at room temperature, giving rise to magnetoelectric functionality that may be exploited in novel multiferroic-based devices. In this paper, we demonstrate that by substituting samarium for 10% of the bismuth ions the periodicity of the room temperature cycloid is increased, and by cooling below $\sim15$ K the magnetic structure tends towards a simple G-type antiferromagnet, which is fully established at 1.5 K. We show that this transition results from $f-d$ exchange coupling, which induces a local anisotropy on the iron magnetic moments that destroys the cycloidal order - a result of general significance regarding the stability of non-collinear magnetic structures in the presence of multiple magnetic sublattices.

cond-mat.str-el↗

arXiv2016

Bulk superconductivity at 84 K in the strongly overdoped regime of cuprates

By means of magnetization, specific heat and muon-spin relaxation measurements, we investigate high-pressure oxidized \mohpo, in which overdoping is achieved up to $p \sim 0.45$ hole/Cu, well beyond the $T_c - p$ superconducting dome of cuprates, where Fermi liquid behavior is expected. Surprisingly, we find bulk superconductivity with $T_c$=84 K and superfluid density similar to those of optimally doped Y123. On the other hand, specific heat data display a large electronic contribution at low temperature, comparable to that of nonsuperconducting overdoped La214. These results point at an unusual high-$T_c$ phase with a large fraction of unpaired holes. Further experiments may assess the Fermi liquid properties of the present phase, which would put into question the paradigm that the high $T_c$ of cuprates originates from a non-Fermi liquid ground state.

cond-mat.supr-con↗

arXiv2016

Magnetodielectric detection of magnetic quadrupole order in Ba(TiO)Cu$_4$(PO$_4$)$_4$ with Cu$_4$O$_{12}$ square cupolas

In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal, monopole, and quadrupole moments. So far, however, the ME-activity of these multipole moments has only been established experimentally for the toroidal moment. Here, we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu$_4$(PO$_4$)$_4$. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.

cond-mat.str-el↗

arXiv2016

Modulated spin helicity stabilized by incommensurate orbital density waves in a quadruple perovskite manganite

Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48 K, the primary magnetic order parameter is locked into the orbital wave by an admixture of helical and collinear spin density wave structures. Furthermore, our model naturally explains the lack of a sharp dielectric anomaly at TN1 and the unusual temperature dependence of the electrical polarisation.

cond-mat.str-el↗

arXiv2016

Robust singlet dimers with fragile ordering in two-dimensional honeycomb lattice of Li$_2$RuO$_3$

When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.

cond-mat.str-el↗

arXiv2016

Incommensurate Counterrotating Magnetic Order Stabilized by Kitaev Interactions in the Layered Honeycomb $α$-Li$_2$IrO$_3$

The layered honeycomb magnet $α$-Li$_2$IrO$_3$ has been theoretically proposed as a candidate to display novel magnetic behaviour associated with Kitaev interactions between spin-orbit entangled $j_{\rm eff}=1/2$ magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate magnetic order in the honeycomb layers with Ir magnetic moments counter-rotating on nearest-neighbour sites. This type of magnetic structure has not been reported experimentally before in honeycomb magnets and cannot be explained by a spin Hamiltonian with dominant isotropic (Heisenberg) couplings. The magnetic structure shares many key features with the magnetic order in the structural polytypes $β$ and $γ$-Li$_2$IrO$_3$, understood theoretically to be stabilized by dominant Kitaev interactions between Ir moments located on the vertices of three-dimensional hyperhoneycomb and stripyhoneycomb lattices, respectively. Based on this analogy and a theoretical soft-spin analysis of magnetic ground states for candidate spin Hamiltonians, we propose that Kitaev interactions also dominate in $α$-Li$_2$IrO$_3$, indicative of universal Kitaev physics across all three members of the harmonic honeycomb family of Li$_2$IrO$_3$ polytypes.

cond-mat.str-el↗

arXiv2015

The monoclinic crystal structure of $α$-RuCl$_3$ and the zigzag antiferromagnetic ground state

The layered honeycomb magnet alpha-RuCl3 has been proposed as a candidate to realize a Kitaev spin model with strongly frustrated, bond-dependent, anisotropic interactions between spin-orbit entangled jeff=1/2 Ru4+ magnetic moments. Here we report a detailed study of the three-dimensional crystal structure using x-ray diffraction on untwinned crystals combined with structural relaxation calculations. We consider several models for the stacking of honeycomb layers and find evidence for a crystal structure with a monoclinic unit cell corresponding to a stacking of layers with a unidirectional in-plane offset, with occasional in-plane sliding stacking faults, in contrast with the currently-assumed trigonal 3-layer stacking periodicity. We report electronic band structure calculations for the monoclinic structure, which find support for the applicability of the jeff=1/2 picture once spin orbit coupling and electron correlations are included. We propose that differences in the magnitude of anisotropic exchange along symmetry inequivalent bonds in the monoclinic cell could provide a natural mechanism to explain the spin gap observed in powder inelastic neutron scattering, in contrast to spin models based on the three-fold symmetric trigonal structure, which predict a gapless spectrum within linear spin wave theory. Our susceptibility measurements on both powders and stacked crystals, as well as neutron powder diffraction show a single magnetic transition at TN ~ 13K. The analysis of the neutron data provides evidence for zigzag magnetic order in the honeycomb layers with an antiferromagnetic stacking between layers. Magnetization measurements on stacked single crystals in pulsed field up to 60T show a single transition around 8T for in-plane fields followed by a gradual, asymptotic approach to magnetization saturation, as characteristic of strongly anisotropic exchange interactions.

cond-mat.str-el↗

arXiv2015

The magnetic ground state of two isostructual polymeric quantum magnets, [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ and [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, investigated with neutron powder diffraction

The magnetic ground state of two isostructural coordination polymers (i) the quasi two-dimensional S = 1/2 square-lattice antiferromagnet [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$; and (ii) a new compound [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, were examined with neutron powder diffraction measurements. We find the ordered moments of the Heisenberg S = 1/2 Cu(II) ions in [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 0.6(1)$μ_{B}$, whilst the ordered moments for the Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 3.02(6)$μ_{B}$. For Cu(II), this reduced moment indicates the presence of quantum fluctuations below the ordering temperature. We show from heat capacity and electron spin resonance measurements, that due to the crystal electric field splitting of the S = 3/2 Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, this isostructual polymer also behaves as an effective spin-half magnet at low temperatures. The Co moments in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ show strong easy-axis anisotropy, neutron diffraction data which do not support the presence of quantum fluctuations in the ground state and heat capacity data which are consistent with 2D or close to 3D spatial exchange anisotropy.

cond-mat.str-el↗

arXiv2015

Magnetic structure of an incommensurate phase of La-doped BiFe0.5Sc0.5O3: Role of antisymmetric exchange interactions

A 20% substitution of Bi with La in the perovskite Bi1-xLaxFe0.5Sc0.5O3 system obtained under high-pressure and high-temperature conditions has been found to induce an incommensurately modulated structural phase. The room temperature X-ray and neutron powder diffraction patterns of this phase were successfully refined using the Imma(0,0,g)s00 superspace group (g=0.534(3)) with the modulation applied to Bi/La- and oxygen displacements. The modulated structure is closely related to the prototype antiferroelectric structure of PbZrO3 which can be considered as the lock-in variant of the latter with g =0.5. Below T_N = 220 K, the neutron diffraction data provide evidence for a long-range G-type antiferromagnetic ordering commensurate with the average Imma structure. Based on a general symmetry consideration, we show that the direction of the spins is controlled by the antisymmetric exchange imposed by the two primary structural distortions, namely oxygen octahedral tilting and incommensurate atomic displacements. The tilting is responsible for the onset of a weak ferromagnetism, observed in magnetization measurements, whereas the incommensurate displacive mode is dictated by the symmetry to couple a spin-density wave. The obtained results demonstrate that antisymmetric exchange is the dominant anisotropic interaction in Fe3+ based distorted perovskites with a nearly quenched orbital degree of freedom.

cond-mat.str-el↗

arXiv2015

Antiferromagnetism at T > 500 K in the Layered Hexagonal Ruthenate SrRu2O6

We report an experimental and computational study of magnetic and electronic properties of the layered Ru(V) oxide SrRu2O6 (hexagonal, P-3 1m), which shows antiferromagnetic order with a Néel temperature of 563(2) K, among the highest for 4d oxides. Magnetic order occurs both within edge-shared octahedral sheets and between layers and is accompanied by anisotropic thermal expansivity that implies strong magnetoelastic coupling of Ru(V) centers. Electrical transport measurements using focused ion beam induced deposited contacts on a micron-scale crystallite as a function of temperature show p-type semiconductivity. The calculated electronic structure using hybrid density functional theory successfully accounts for the experimentally observed magnetic and electronic structure and Monte Carlo simulations reveals how strong intralayer as well as weaker interlayer interactions are a defining feature of the high temperature magnetic order in the material.

cond-mat.str-el↗

arXiv2015

Haydeeite: a spin-1/2 kagome ferromagnet

The mineral haydeeite, alpha-MgCu3(OD)6Cl2, is a S=1/2 kagome ferromagnet that displays long-range magnetic order below TC=4.2 K with a strongly reduced moment. Our inelastic neutron scattering data show clear spin-wave excitations that are well described by a Heisenberg Hamiltonian with ferromagnetic nearest-neighbor exchange J1=-38 K and antiferromagnetic exchange Jd=+11 K across the hexagons of the kagome lattice. These values place haydeeite very close to the quantum phase transition between ferromagnetic order and non-coplanar twelve-sublattice cuboc2 antiferromagnetic order. Diffuse dynamic short-range ferromagnetic correlations observed above TC persist well into the ferromagnetically ordered phase with a behavior distinct from critical scattering.

cond-mat.str-el↗