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A. Llobet

Publications and source records attributed to A. Llobet.

18 recordsLinked to original sources
arXiv2018

Lattice distortion in the spin-orbital entangled state in RVO3 perovskites

We report a thorough study of Y$_{0.7}$La$_{0.3}$VO$_3$ single crystals by measuring magnetic properties, specific heat, thermal conductivity, x-ray and neutron diffraction with the motivation of revealing the lattice response to the spin-orbital entanglement in \textit{R}VO$_3$. Upon cooling from room temperature, the orbitally disordered paramagnetic state changes around T*$\sim$220\,K to spin-orbital entangled state which is then followed by a transition at T$_N$=116\,K to C-type orbital ordered (OO) and G-type antiferromagnetic ordered (AF) ground state. In the temperature interval T$_N<T<T^*$, the VO$_{6/2}$ octahedra have two comparable in-plane V-O bonds which are longer than the out-of-plane V-O1 bond. This local structural distortion supports the spin-orbital entanglement of partially filled and degenerate yz/zx orbitals. However, this distortion is incompatible with the steric octahedral site distortion intrinsic to orthorhombic perovskites. Their competition induces a second order transition from the spin-orbital entangled state to C-OO/G-AF ground state where the long range OO suppresses the spin-orbital entanglement. Our analysis suggests that the spin-orbital entangled state and G-OO are comparable in energy and compete with each other. Rare earth site disorder favors the spin-orbital entanglement rather than a cooperative Jahn-Teller distortion. The results also indicate for LaVO$_3$ a C-OO/G-AF state in T$_t$\,$\leq$\,T\,$\leq$T$_N$ and an orbital flipping transition at T$_t$.

cond-mat.str-el↗
arXiv2016

Defect-induced magnetic structure of CuMnSb

Ab initio total energy calculations show that the antiferromagnetic (111) order is not the ground state for the ideal CuMnSb Heusler alloy in contrast to the results of neutron diffraction experiments. It is known, that Heusler alloys usually contain various defects depending on the sample preparation. We have therefore investigated magnetic phases of CuMnSb assuming the most common defects which exist in real experimental conditions. The full-potential supercell approach and a Heisenberg model approach using the coherent potential approximation are adopted. The results of the total energy supercell calculations indicate that defects that bring Mn atoms close together promote the antiferromagnetic (111) structure already for a low critical defect concentrations ($\approx$ 3%). A detailed study of exchange interactions between Mn-moments further supports the above stabilization mechanism. Finally, the stability of the antiferromagnetic (111) order is enhanced by inclusion of electron correlations in narrow Mn-bands. The present refinement structure analysis of neutron scattering experiment supports theoretical conclusions.

cond-mat.mtrl-sci↗
arXiv2015

Structural evolution of bismuth sodium titanate induced by A-site non-stoichiometry: Neutron powder diffraction studies

We performed neutron powder diffraction measurements on (Bi$_{0.5}$Na$_{0.5+x}$)TiO$_3$ and (Bi$_{0.5+y}$Na$_{0.5}$)TiO$_3$ to study structural evolution induced by the non-stoichiometry. Despite the non-stoichiometry, the local structure ($r$$\leq$ 3.5 Å) from the pair distribution function analysis is barely affected by the sodium deficit of up to -5 mol%. With increasing pair distance, however, the atomic pair correlations weaken due to the disorder caused by the sodium deficiency. Although the sodium and the bismuth share the same crystallographic site, their non-stoichiometry have rather opposite effects as revealed from a distinctive distortion of the Bragg peaks. In addition, Rietveld refinement demonstrates that the octahedral tilting is continually suppressed by the sodium deficit of up to -5 mol%. This is contrary to the effect of the bismuth deficiency, which enhances the octahedral tilting.

cond-mat.mtrl-sci↗
arXiv2012

Electronic thermoelectric power factor and metal-insulator transition in FeSb2

We show that synthesis-induced Metal -Insulator transition (MIT) for electronic transport along the orthorombic c axis of FeSb$_{2}$ single crystals has greatly enhanced electrical conductivity while keeping the thermopower at a relatively high level. By this means, the thermoelectric power factor is enhanced to a new record high S$^{2}$$σ$ $\sim$ 8000 $μ$WK$^{-2}$cm$^{-1}$ at 28 K. We find that the large thermopower in FeSb$_{2}$ can be rationalized within the correlated electron model with two bands having large quasiparaticle disparity, whereas MIT is induced by subtle structural differences. The results in this work testify that correlated electrons can produce extreme power factor values.

cond-mat.str-el↗
arXiv2012

Magnetism in La2O3(Fe1-xMnx)2Se2 tuned by Fe/Mn ratio

We report the evolution of structural and magnetic properties in La2O3(Fe1-xMnx)2Se2. Heat capacity and bulk magnetization indicate an increased ferromagnetic component of the long-range magnetic order and possible increased degree of frustration. Atomic disorder on Fe(Mn) sites suppresses the temperature of the long-range order whereas intermediate alloys show a rich magnetic phase diagram.

cond-mat.str-el↗
arXiv2012

Iron Displacements and Magnetoelastic Coupling in the Spin-Ladder Compound BaFe2Se3

We report long-range ordered antiferromagnetism concomitant with local iron displacements in the spin-ladder compound BaFe$_2$Se$_3$. Short-range magnetic correlations, present at room temperature, develop into long-range antiferromagnetic order below T$_N$ = 256 K, with no superconductivity down to 1.8 K. Built of ferromagnetic Fe$_4$ plaquettes, the magnetic ground state correlates with local displacements of the Fe atoms. These iron displacements imply significant magnetoelastic coupling in FeX$_4$-based materials, an ingredient hypothesized to be important in the emergence of superconductivity. This result also suggests that knowledge of these local displacements is essential for properly understanding the electronic structure of these systems. As with the copper oxide superconductors two decades ago, our results highlight the importance of reduced dimensionality spin ladder compounds in the study of the coupling of spin, charge, and atom positions in superconducting materials.

cond-mat.supr-con↗
arXiv2012

Orbital Selective Magnetism in the Spin-Ladder Iron Selenides Ba$_{1-x}$K$_{x}$Fe$_2$Se$_3$

Here we show that the 2.80(8) μB/Fe block antiferromagnetic order of BaFe2Se3 transforms into stripe antiferromagnetic order in KFe2Se3 with a decrease in moment to 2.1(1) μB/Fe. This reduction is larger than expected from the change in electron count from Ba$^{2+}$ to K$^{+}$, and occurs with the loss of the displacements of Fe atoms from ideal positions in the ladders, as found by neutron pair distribution function analysis. Intermediate compositions remain insulating, and magnetic susceptibility measurements show a suppression of magnetic order and probable formation of a spin-glass. Together, these results imply an orbital-dependent selection of magnetic versus bonded behavior, driven by relative bandwidths and fillings.

cond-mat.supr-con↗
arXiv2011

Crystal fields, disorder, and antiferromagnetic short-range order in Yb0.24Sn0.76Ru

We report extensive measurements on a new compound (Yb0.24Sn0.76)Ru that crystallizes in the cubic CsCl structure. Valence band photoemission and L3 x-ray absorption show no divalent component in the 4f configuration of Yb. Inelastic neutron scattering (INS) indicates that the eight-fold degenerate J-multiplet of Yb3+ is split by the crystalline electric field (CEF) into a Γ7 doublet ground state and a Γ8 quartet at an excitation energy 20 meV. The magnetic susceptibility can be fit very well by this CEF scheme under the assumption that a Γ6 excited state resides at 32 meV; however, the Γ8/Γ6 transition expected at 12 meV was not observed in the INS. The resistivity follows a Bloch- Grüneisen law shunted by a parallel resistor, as is typical of systems subject to phonon scattering with no apparent magnetic scattering. All of these properties can be understood as representing simple local moment behavior of the trivalent Yb ion. At 1 K, there is a peak in specific heat that is too broad to represent a magnetic phase transition, consistent with absence of magnetic reflections in neutron diffraction. On the other hand, this peak also is too narrow to represent the Kondo effect in the Γ7 ground state doublet. On the basis of the field-dependence of the specific heat, we argue that antiferromagnetic shortrange order (possibly co-existing with Kondo physics) occurs at low temperatures. The long-range magnetic order is suppressed because the Yb site occupancy is below the percolation threshold for this disordered compound.

cond-mat.str-el↗
arXiv2011

Role of Magnetic Exchange Energy on Charge Ordering in RSFO (R=La, Pr, and Nd)

Inelastic neutron scattering is applied to study the role of magnetism in stabilizing the charge ordered state in \emph{R}$_{1/3}$Sr$_{2/3}$FeO$_{3}$ (\emph{R}SFO) (\emph{R} = La, Pr, and Nd). The ratio of the ferromagnetic exchange energy (J$_F$) and antiferromagnetic exchange energy (J$_{AF}$), |J$_F$ /J$_{AF}|, is a key indicator of the stability of the charge ordered and antiferromagnetic ordered state. This ratio is obtained from the spin wave spectrum by inelastic neutron scattering and is sufficiently large to suggest that the magnetic exchange energy alone can stabilize the charge ordered state in La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ and Pr$_{1/3}$Sr$_{2/3}$FeO$_{3}$. The exchange ratio decreases from La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ to Nd1$_{1/3}$Sr$_{2/3}$FeO$_{3}$ which indicates a gradual destabilization of the magnetic exchange mechanism for charge ordering in correspondence with the observed reduction in the ordering temperature.

cond-mat.str-el↗
arXiv2011

Lattice dynamical origin of peak thermoelectric performance in AgPbmSbTe2+m observed by inelastic neutron scattering

Phonon densities of states (DOS) for the high performing thermoelectric material, AgPbmSbTe2+m (LAST-m, m = 16, 18, and 20), were extracted from time-of-flight inelastic neutron scattering measurements. The phonon DOS of LAST-18 differs remarkably from LAST-16 and LAST-20 by exhibiting a dramatic broadening of its acoustic modes that increases on heating. This broadening coincides with a minimum in the thermal conductivity, a maximum in the electrical conductivity and Seebeck coefficient, and a related peak in thermoelectric performance. We argue that the anomalous broadening originates with scattering enhanced by modifications to Te-Ag(Sb) bonds caused by their resonant electronic states falling near the Fermi energy for m = 18.

cond-mat.mtrl-sci↗
arXiv2010

Atomic displacements in the "charge-ice" pyrochlore Bi2Ti2O7 studied by neutron total scattering

The oxide pyrochlore Bi$_2$Ti$_2$O$_6$O$^\prime$ is known to be associated with large displacements of Bi and O$^\prime$ atoms from their ideal crystallographic positions. Neutron total scattering, analyzed in both reciprocal and real space, is employed here to understand the nature of these displacements. Rietveld analysis and maximum entropy methods are used to produce an average picture of the structural non-ideality. Local structure is modeled via large-box reverse Monte Carlo simulations constrained simultaneously by the Bragg profile and real-space pair distribution function. Direct visualization and statistical analyses of these models show the precise nature of the static Bi and O$^\prime$ displacements. Correlations between neighboring Bi displacements are analyzed using coordinates from the large-box simulations. The framework of continuous symmetry measures has been applied to distributions of O$^\prime$Bi$_4$ tetrahedra to examine deviations from ideality. Bi displacements from ideal positions appear correlated over local length scales. The results are consistent with the idea that these nonmagnetic lone-pair containing pyrochlore compounds can be regarded as highly structurally frustrated systems.

cond-mat.mtrl-sci↗
arXiv2009

Intrinsic Localized Modes Observed in the High Temperature Vibrational Spectrum of NaI

Inelastic neutron measurements of the high-temperature lattice excitations in NaI show that in thermal equilibrium at 555 K an intrinsic mode, localized in three dimensions, occurs at a single frequency near the center of the spectral phonon gap, polarized along [111]. At higher temperatures the intrinsic localized mode gains intensity. Higher energy inelastic neutron and x-ray scattering measurements on a room-temperature NaI crystal indicate that the creation energy of the ground state of the intrinsic localized mode is 299 meV.

cond-mat.str-el↗
arXiv2005

Novel Coexistence of Superconductivity with Two Distinct Magnetic Orders

The heavy fermion Ce(Rh,Ir)In5 system exhibits properties that range from an incommensurate antiferromagnet on the Rh-rich end to an exotic superconductor on the Ir-rich end of the phase diagram. At intermediate composition where antiferromagnetism coexists with superconductivity, two types of magnetic order are observed: the incommensurate one of CeRhIn5 and a new, commensurate antiferromagnetism that orders separately. The coexistence of f-electron superconductivity with two distinct f-electron magnetic orders is unique among unconventional superconductors, adding a new variety to the usual coexistence found in magnetic superconductors.

cond-mat.supr-con↗
arXiv2004

Neutron diffraction study of average and local structure in La0.5Ca0.5MnO3

We used neutron powder diffraction to obtain the local and long-range structure of La0.5Ca0.5MnO3 at room temperature and 20K. By combining Rietveld and pair distribution function analysis of the total neutron scattering data, we have analyzed the structure of the compound using two competing models describing the low temperature phase: first the charge ordered/orbital ordered model and second the Mn-Mn dimer model. These structural models fit the 20K neutron powder diffraction pattern equally well using Rietveld analysis. Therefore, pair distribution function analysis is used to probe the local and medium-range structure revealing a system with two distinctly distorted Mn octahedra and Mn ions with non-integral valence states. The distorted octahedra differ with the structural model for the Zener polaron type Mn-Mn dimer picture proposed for Pr0.6Ca0.4MnO3 and order in a similar checkerboard configuration associated with the CE-type anti-ferromagnetic structure. Therefore, locally the charge difference and structural ordering between the two Mn is appreciable enough to describe the system at 20K as "partially charge ordered".

cond-mat.str-el↗
arXiv2004

YbGaGe: normal thermal expansion

We report evidence of the absence of zero thermal expansion in well-characterized high-quality polycrystalline samples of YbGaGe. High-quality samples of YbGaGe were produced from high-purity starting elements and were extensively characterized using x-ray powder diffraction, differential thermal analysis, atomic emission spectroscopy, magnetization, and neutron powder diffraction at various temperatures. Our sample melts congruently at 920 C. A small amount of Yb2O3 was found in our sample, which explains the behavior of the magnetic susceptibility. These observations rule out the scenario of electronic valence driven thermal expansion in YbGaGe. Our studies indicate that the thermal expansion of YbGaGe is comparable to that of Cu.

cond-mat.mtrl-sci↗
arXiv2003

Magnetic structure of CeRhIn_5 as a function of pressure and temperature

We report magnetic neutron-diffraction and electrical resistivity studies on single crystals of the heavy-fermion antiferromagnet CeRhIn$_{5}$ at pressures up to 2.3 GPa. These experiments show that the staggered moment of Ce and the incommensurate magnetic structure change weakly with applied pressure up to 1.63 GPa, where resistivity, specific heat and NQR measurements confirm the presence of bulk superconductivity. This work places new constraints on an interpretation of the relationship between antiferromagnetism and unconventional superconductivity in CeRhIn$_{5}$.

cond-mat.str-el↗
arXiv2002

Selective Spin-State Switch and Metal-Insulator Transition in \boldmath $\rm GdBaCo_2O_{5.5}$

Ultra-high resolution synchrotron diffraction data for $\rm GdBaCo_2O_{5.5}$ throw new light on the metal-insulator transition of Co$^{3+}$ Ba-cobaltites. An anomalous expansion of CoO$_6$ octahedra is observed at the phase transition on heating, while CoO$_5$ pyramids show the normal shrinking at the closing of the gap. The insulator-to-metal transition is attributed to a sudden excitation of some electrons in the octahedra ($t_{2g}^6$ state) into the Co $e_g$ band (final $t_{2g}^4e_g^2$ state). The $t_{2g}^5e_g^1$ state in the pyramids does not change and the structural study also rules out a $d_{3x^2-r^2}/d_{3y^2-r^2}$ orbital ordering at $T_{MI}$.

cond-mat.mtrl-sci↗