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V. O. Garlea

Publications and source records attributed to V. O. Garlea.

At least 37 records · Page 2Linked to original sources

Crystal Field Levels and Magnetic Anisotropy in the Kagome Compounds $\rm{Nd_3Sb_3Mg_2O_{14}}$, $\rm{Nd_3Sb_3Zn_2O_{14}}$, and $\rm{Pr_3Sb_3Mg_2O_{14}}$

We report the crystal field levels of several newly-discovered rare-earth kagome compounds: $\rm{Nd_3Sb_3Mg_2O_{14}}$, $\rm{Nd_3Sb_3Zn_2O_{14}}$, and $\rm{Pr_3Sb_3Mg_2O_{14}}$. We determine the CEF Hamiltonian by fitting to neutron scattering data using a point-charge Hamiltonian as an intermediate fitting step. The fitted Hamiltonians accurately reproduce bulk susceptibility measurements, and the results indicate easy-axis ground state doublets for $\rm{Nd_3Sb_3Mg_2O_{14}}$ and $\rm{Nd_3Sb_3Zn_2O_{14}}$, and a singlet ground state for $\rm{Pr_3Sb_3Mg_2O_{14}}$. These results provide the groundwork for future investigations of these compounds and a template for CEF analysis of other low-symmetry materials.

cond-mat.str-el↗

Manifolds of magnetic ordered states and excitations in the almost Heisenberg pyrochlore antiferromagnet MgCr2O4

In spinels ACr2O4 (A=Mg, Zn) realisation of the classical pyrochlore Heisenberg antiferromagnet model is complicated by a strong spin-lattice coupling: the extensive degeneracy of the ground state is lifted by a magneto-structural transition at TN=12.5 K. We study the resulting low-temperature low-symmetry crystal structure by synchrotron x-ray diffraction. The consistent features of x-ray low-temperature patterns are explained by the tetragonal model of Ehrenberg et. al (Pow. Diff. 17, 230( 2002)), while other features depend on sample or cooling protocol. Complex partially ordered magnetic state is studied by neutron diffraction and spherical neutron polarimetry. Multiple magnetic domains of configuration arms of the propagation vectors k1=(1/2 1/2 0), k2=(1 0 1/2) appear. The ordered moment reaches 1.94(3) muB/Cr3+ for k1 and 2.08(3) muB/Cr3+ for k2, if equal amount of the k1 and k2 phases is assumed. The magnetic arrangements have the dominant components along the [110] and [1-10] diagonals and a smaller c-component. By inelastic neutron scattering we investigate the spin excitations, which comprise a mixture of dispersive spin waves propagating from the magnetic Bragg peaks and resonance modes centered at equal energy steps of 4.5 meV. We interpret these as acoustic and optical spin wave branches, but show that the neutron scattering cross sections of transitions within a unit of two corner-sharing tetrahedra match the observed intensity distribution of the resonances. The distinctive fingerprint of cluster-like excitations in the optical spin wave branches suggests that propagating excitations are localized by the complex crystal structure and magnetic orders.

cond-mat.str-el↗

Non-Fermi surface nesting driven commensurate magnetic ordering in Fe-doped Sr$_2$RuO$_4$

Sr$_2$RuO$_4$, an unconventional superconductor, is known to possess an incommensurate spin density wave instability driven by Fermi surface nesting. Here we report a static spin density wave ordering with a commensurate propagation vector $q_c$ = (0.25 0.25 0) in Fe-doped Sr$_2$RuO$_4$, despite the magnetic fluctuations persisting at the incommensurate wave vectors $q_{ic}$ = (0.3 0.3 L) as in the parent compound. The latter feature is corroborated by the first principles calculations, which show that Fe substitution barely changes the nesting vector of the Fermi surface. These results suggest that in addition to the known incommensurate magnetic instability, Sr$_2$RuO$_4$ is also in proximity to a commensurate magnetic tendency that can be stabilized via Fe doping.

cond-mat.str-el↗

Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6

The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.

cond-mat.str-el↗

Unusual UUDD magnetic chain structure of the spin-1/2 tetragonally distorted spinel GeCu2O4

GeCu2O4 exhibits a tetragonal spinel structure due to the strong Jahn-Teller distortion associated with Cu2+ ions. We show that its magnetic structure can be described as slabs composed of a pair of layers with orthogonally oriented spin 1/2 Cu chains in the basal ab plane. The spins between the two layers within a slab are collinearly aligned while the spin directions of neighboring slabs are perpendicular to each other. Interestingly, we find that spins along each chain form an unusual up-up-down-down (UUDD) pattern, suggesting a non-negligible nearest-neighbor biquadratic exchange interaction in the effective classical spin Hamiltonian. We hypothesize that spin-orbit coupling and orbital mixing of Cu2+ ions in this system is non-negligible, which calls for future calculations using perturbation theory with extended Hilbert (spin and orbital) space and calculations based on density functional theory including spin-orbit coupling and looking at the global stability of the UUDD state.

cond-mat.mtrl-sci↗

Spin-lattice coupling mediated multiferroicity in (ND4)2FeCl5D2O

We report a neutron diffraction study of the multiferroic mechanism in (ND4)2FeCl5D2O, a molecular compound that exhibits magnetically induced ferroelectricity. This material exhibits two successive magnetic transitions on cooling: a long-range order transition to an incommensurate (IC) collinear sinusoidal spin state at TN=7.3 K, followed by a second transition to an IC cycloidal spin state at TFE=6.8 K, the later of which is accompanied by spontaneous ferroelectric polarization. The cycloid structure is strongly distorted by spin-lattice coupling as evidenced by the observations of both odd and even higher-order harmonics associated with the cycloid wave vector, and a weak commensurate phase that coexists with the IC phase. The appearance of the 2nd-order harmonic coincides with the onset of the electric polarization, thereby providing unambiguous evidence that the induced electric polarization is mediated by the spin-lattice interaction. Our results for this system, in which the orbital angular momentum is expected to be quenched, are remarkably similar to those of the prototypical TbMnO3, in which the magnetoelectric effect is attributed to spin-orbit coupling.

cond-mat.str-el↗

Two-dimensional Dirac fermions in YbMnBi2 antiferromagnet

We report two-dimensional quantum transport and Dirac fermions in YbMnBi2 single crystals. YbMnBi2 is a layered material with anisotropic conductivity and magnetic order below 290 K. Magnetotransport properties, nonzero Berry phase and small cyclotron mass indicate the presence of quasi two dimensional Dirac fermions. Quantum oscillations in Hall resistivity suggest the presence of both electron and hole parts of the Fermi surface whereas the Berry phase suggests spin-orbit coupling.

cond-mat.mes-hall↗

Anisotropic exchange within decoupled tetrahedra in the quantum breathing pyrochlore Ba3Yb2Zn5O11

The low energy spin excitation spectrum of the breathing pyrochlore Ba3Yb2Zn5O11 has been investigated with inelastic neutron scattering. Several nearly resolution limited modes with no observable dispersion are observed at 250 mK while, at elevated temperatures, transitions between excited levels become visible. To gain deeper insight, a theoretical model of isolated Yb3+ tetrahedra parametrized by four anisotropic exchange constants is constructed. The model reproduces the inelastic neutron scattering data, specific heat, and magnetic susceptibility with high fidelity. The fitted exchange parameters reveal a Heisenberg antiferromagnet with a very large Dzyaloshinskii-Moriya interaction. Using this model, we predict the appearance of an unusual octupolar paramagnet at low temperatures and speculate on the development of inter-tetrahedron correlations.

cond-mat.str-el↗

Canted Magnetic Ground State of Quarter-Doped Manganites $R_{0.75}$Ca$_{0.25}$MnO$_3$ ($R$ = Y, Tb, Dy, Ho, and Er)

Polycrystalline samples of the quarter-doped manganites $R_{0.75}$Ca$_{0.25}$MnO$_3$ ($R$ = Y, Tb, Dy, Ho, and Er) were studied by X-ray diffraction and AC/DC susceptibility measurements. All five samples are orthorhombic and exhibit similar magnetic properties: enhanced ferromagnetism below $T_1$ ($\sim80$ K) and a spin glass (SG) state below $T_{SG}$ ($\sim30$ K). With increasing $R^{3+}$ ionic size, both $T_1$ and $T_{SG}$ generally increase. The single crystal neutron diffraction results on Tb$_{0.75}$Ca$_{0.25}$MnO$_3$ revealed that the SG state is mainly composed of a short-range ordered version of a novel canted (i.e. noncollinear) antiferromagnetic spin state. Furthermore, calculations based on the double exchange model for quarter-doped manganites reveal that this new magnetic phase provides a transition state between the ferromagnetic state and the theoretically predicted spin-orthogonal stripe phase.

cond-mat.mtrl-sci↗

Structural transition and orbital glass physics in near itinerant CoV2O4

The ferrimagnetic spinel $\mathrm{CoV_2O_4}$ has been a topic of intense recent interest, both as a frustrated insulator with unquenched orbital degeneracy and as a near-itinerant magnet which can be driven metallic with moderate applied pressure. Here, we report on our recent neutron diffraction and inelastic scattering measurements on powders with minimal cation site disorder. Our main new result is the identification of a weak ($\frac{Δa}{a} \sim 10^{-4}$), first order structural phase transition at $T^*$ = 90 K, the same temperature where spin canting was seen in recent single crystal measurements. This transition is characterized by a short-range distortion of oxygen octahedral positions, and inelastic data further establish a weak $Δ\sim 1.25 meV$ spin gap at low temperature. Together, these findings provide strong support for the local orbital picture and the existence of an orbital glass state at temperatures below $T^*$.

cond-mat.str-el↗

Structural and Magnetic Phase Transitions in CeCu$_{6-x}T_x$ ($T$ = Ag, Pd)

The structural and the magnetic properties of CeCu$_{6-x}$Ag$_x$ (0 $\leq$ $x$ $\leq$ 0.85) and CeCu$_{6-x}$Pd$_x$ (0 $\leq$ $x$ $\leq$ 0.4) have been studied using neutron diffraction, resonant ultrasound spectroscopy (RUS), heat capacity, x-ray diffraction measurements and first principles calculations. The structural and magnetic phase diagrams of CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$ as a function of Ag/Pd composition are reported. The end member, CeCu$_6$, undergoes a structural phase transition from an orthorhombic ($Pnma$) to a monoclinic ($P2_1/c$) phase at 240 K. In CeCu$_{6-x}$Ag$_x$, the structural phase transition temperature (${T_{s}}$) decreases linearly with Ag concentration and extrapolates to zero at $x_{S}$ $\approx$ 0.1. The structural transition in CeCu$_{6-x}$Pd$_x$ remains unperturbed with Pd substitution within the range of our study. The lattice constant $b$ slightly decreases with Ag/Pd doping, whereas, $a$ and $c$ increase with an overall increase in the unit cell volume. Both systems, CeCu$_{6-x}$Ag$_x$ and CeCu$_{6-x}$Pd$_x$, exhibit a magnetic quantum critical point (QCP), at $x$ $\approx$ 0.2 and $x$ $\approx$ 0.05 respectively. Near the QCP, long range antiferromagnetic ordering takes place at an incommensurate wave vector ($δ_1$ 0 $δ_2$) where $δ_1 \sim 0.62$, $δ_2 \sim 0.25$, $x$ = 0.125 for CeCu$_{6-x}$Pd$_x$ and $δ_1 \sim 0.64$, $δ_2 \sim 0.3$, $x$ = 0.3 for CeCu$_{6-x}$Ag$_x$. The magnetic structure consists of an amplitude modulation of the Ce-moments which are aligned along the $c$-axis of the orthorhombic unit cell.

cond-mat.str-el↗

Disorder from order among anisotropic next-nearest-neighbor Ising spin chains in SrHo$_2$O$_4$

We describe why Ising spin chains with competing interactions in $\rm SrHo_2O_4$ segregate into ordered and disordered ensembles at low temperatures ($T$). Using elastic neutron scattering, magnetization, and specific heat measurements, the two distinct spin chains are inferred to have Néel ($\uparrow\downarrow\uparrow\downarrow$) and double-Néel ($\uparrow\uparrow\downarrow\downarrow$) ground states respectively. Below $T_\mathrm{N}=0.68(2)$~K, the Néel chains develop three dimensional (3D) long range order (LRO), which arrests further thermal equilibration of the double-Néel chains so they remain in a disordered incommensurate state for $T$ below $T_\mathrm{S}= 0.52(2)$~K. $\rm SrHo_2O_4$ distills an important feature of incommensurate low dimensional magnetism: kinetically trapped topological defects in a quasi$-d-$dimensional spin system can preclude order in $d+1$ dimensions.

cond-mat.str-el↗

Spin liquid ground state in the frustrated J1-J2 zigzag chain system BaTb2O4

We have investigated polycrystalline samples of the zigzag chain system BaTb$_2$O$_4$ with a combination of magnetic susceptibility, heat capacity, neutron powder diffraction, and muon spin relaxation measurements. Despite the onset of Tb$^{3+}$ short-range antiferromagnetic correlations at $|θ_{CW}|$ $=$ 18.5 K and a very large effective moment, our combined measurements indicate that BaTb$_2$O$_4$ remains paramagnetic down to 0.095 K. The magnetic properties of this material show striking similarities to the pyrochlore antiferromagnet Tb$_2$Ti$_2$O$_7$, and therefore we propose that BaTb$_2$O$_4$ is a new large moment spin liquid candidate.

cond-mat.str-el↗

Superconductivity in Noncentrosymmetric Iridium Silicide Li2IrSi3

The effects of lithium absorption on the crystal structure and electronic properties of IrSi3, a binary silicide with a noncentrosymmetric crystal structure, were studied. X-ray and neutron diffraction experiments revealed that hexagonal IrSi3 (space group P6_3mc) transforms into trigonal Li2IrSi3 (space group P31c) upon lithium absorption. The structure of Li2IrSi3 is found to consist of a planar kagome network of silicon atoms with Li and Ir spaced at unequal distances between the kagome layers, resulting in a polar structure along the c-axis. Li2IrSi3 exhibited type-II superconductivity with a transition temperature Tc of 3.8 K, displaying a structure type that no previous superconductors have been reported to have.

cond-mat.supr-con↗

Magnetic ordering in the frustrated J1-J2 Ising chain candidate BaNd2O4

The AR$_2$O$_4$ family (R = rare earth) have recently been attracting interest as a new series of frustrated magnets, with the magnetic R atoms forming zigzag chains running along the $c$-axis. We have investigated polycrystalline BaNd$_2$O$_4$ with a combination of magnetization, heat capacity, and neutron powder diffraction (NPD) measurements. Magnetic Bragg peaks are observed below $T_N$ $=$ 1.7 K, and they can be indexed with a propagation vector of $\vec{k}$ $=$ (0 1/2 1/2). The signal from magnetic diffraction is well described by long-range ordering from only one of the two types of Nd zigzag chains, with collinear up-up-down-down intrachain spin configurations. Furthermore, low temperature magnetization and heat capacity measurements reveal two field-induced spin transitions at 2.5 T and 4 T for $T$ $=$ 0.46 K. The high field phase is paramagnetic, while the intermediate field state may arise from a spin transition of the long-range ordered Nd chains, resulting in an up-up-down intrachain spin configuration. The proposed intermediate field state is consistent with the magnetic structure determined in zero field for these chains by NPD, as both phases are predicted for the classical Ising chain model with nearest neighbor and next nearest neighbor interactions.

cond-mat.str-el↗

Magnons and a two-component spin gap in FeV2O4

The spinel vanadates have become a model family for exploring orbital order on the frustrated pyrochlore lattice, and recent debate has focused on the symmetry of local crystal fields at the cation sites. Here, we present neutron scattering measurements of the magnetic excitation spectrum in $\mathrm{FeV_2O_4}$, a recent example of a ferrimagnetic spinel vanadate which is available in single crystal form. We report the existence of two emergent magnon modes at low temperatures, which draw strong parallels with the closely related material, $\mathrm{MnV_2O_4}$. We were able to reproduce the essential elements of both the magnetic ordering pattern and the dispersion of the inelastic modes with semi- classical spin wave calculations, using a minimal model that implies a sizeable single-ion anisotropy on the vanadium sublattice. Taking into account the direction of ordered spins, we associate this anisotropy with the large trigonal distortion of $\mathrm{VO_6}$ octahedra, previously observed via neutron powder diffraction measurements. We further report on the spin gap, which is an order-of-magnitude larger than that observed in $\mathrm{MnV_2O_4}$. By looking at the overall temperature dependence, we were able to show that the gap magnitude is largely associated with the ferro-orbital order known to exist on the iron sublattice, but the contribution to the gap from the vanadium sublattice is in fact comparable to what is reported in the Mn compound. This reinforces the conclusion that the spin canting transition is associated with the ordering of vanadium orbitals in this system, and closer analysis indicates closely related physics underlying orbital transitions in $\mathrm{FeV_2O_4}$ and $\mathrm{MnV_2O_4}$.

cond-mat.str-el↗

Magnetic and Structural Phase Transitions in the Spinel Compound Fe1+xCr2-xO4

Neutron and X-ray diffraction, magnetic susceptibility, and specific heat measurements have been used to investigate the magnetic and structural phase transitions of the spinel system Fe1+xCr2-xO4(0.0<=x<=1.0). The temperature versus Fe concentration (x) phase diagram features two magnetically ordered states and four structural states below 420 K. The complexity of the phase diagram is closely related to the change in the spin and orbital degrees of freedom induced by substitution of Fe ions for Cr ions. The systematic change in the crystal structure is explained by the combined effects of Jahn-Teller distortion, spin-lattice interaction, Fe2+-Fe3+ hopping, and disorder among Fe2+, Fe3+, and Cr3+ ions.

cond-mat.mtrl-sci↗

Complex magnetic behavior of the sawtooth Fe chains in Rb$_{2}$Fe$_{2}$O(AsO$_{4}$)$_{2}$

Results of magnetic field and temperature dependent neutron diffraction and magnetization measurements on oxy-arsenate Rb$_{2}$Fe$_{2}$O(AsO$_{4}$)$_{2}$ are reported. The crystal structure of this compound contains pseudo-one-dimensional [Fe$_{2}$O$_{6}$]$^\infty$ sawtooth-like chains, formed by corner sharing isosceles triangles of $Fe^{3+}$ ions occupying two nonequivalent crystallographic sites. The chains extend infinitely along the crystallographic $b$-axis and are structurally confined from one another via diamagnetic (AsO$_{4}$)$^{3-}$ units along the $a$-axis, and Rb$^+$ cations along the $c$-axis direction. Neutron diffraction measurements indicate the onset of a long range antiferromagnetic order below approximately 25 K. The magnetic structure consists of ferrimagnetic chains which are antiferromagnetically coupled with each other. Within each chain, one of the two Fe sites carries a moment which lies along the \emph{b}-axis, while the second site bears a canted moment in the opposite direction. Externally applied magnetic field induces a transition to a ferrimagnetic state, in which the coupling between the sawtooth chains becomes ferromagnetic. Magnetization measurements performed on optically-aligned single crystals reveal evidence for an uncompensated magnetization at low magnetic fields that could emerge from to a phase-segregated state with ferrimagnetic inclusions or from antiferromagnetic domain walls. The observed magnetic states and the competition between them is expected to arise from strongly frustrated interactions within the sawtooth chains and relatively weak coupling between them.

cond-mat.str-el↗