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Garlea, Vasile O

Publications and source records attributed to Garlea, Vasile O.

At least 19 records

Polarized neutron scattering on HYSPEC: the HYbrid SPECtrometer at SNS

Here, we describe some of the first polarized neutron scattering measurements performed at HYSPEC [1-4] spectrometer at the Spallation Neutron Source, Oak Ridge National Laboratory. Furthermore, we discuss details of the instrument setup and the experimental procedures in the mode with full polarization analysis. Examples of polarized neutron diffraction and polarized inelastic neutron data obtained on single crystal samples are presented.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Data processing workflow for time of flight polarized neutrons inelastic measurements

We discuss the data processing workflow for polarized neutron scattering measurements performed at HYSPEC spectrometer at the Spallation Neutron Source, Oak Ridge National Laboratory. The effects of the focusing Heusler crystal polarizer and the wide-angle supermirror transmission polarization analyzer are added to the data processing flow of the non-polarized case. The implementation is done using the Mantid software package.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source

The Spallation Neutron Source at Oak Ridge National Laboratory now hosts four direct geometry time-of-flight chopper spectrometers. These instruments cover a range of wave-vector and energy transfer space with varying degrees of neutron flux and resolution. The regions of reciprocal and energy space available to measure at these instruments are not exclusive and overlap significantly. We present a direct comparison of the capabilities of this instrumentation, conducted by data mining the instrument usage histories, and specific scanning regimes. In addition, one of the common science missions for these instruments is the study of magnetic excitations in condensed matter systems. We have measured the powder averaged spin wave spectra in one particular sample using each of these instruments, and use these data in our comparisons.

07 ISOTOPE AND RADIATION SOURCES↗

Synthesis, Structures, and Magnetic Properties of Rare-Earth Cobalt Arsenides, RCo2As2 (R = La, Ce, Pr, Nd)

Four rare-earth cobalt arsenides, RCo2As2 (R = La, Ce, Pr, Nd), were obtained by reactions of constituent elements in molten Bi. The use of Bi flux also allowed the growth of representative single crystals. All compounds are isostructural and belong to the ThCr2Si2 structure type (space group I4/mmm). The formation of Co vacancies is observed in all structures, while the structures of La- and Ce-containing compounds also show incorporation of minor Bi defects next to the R crystallographic site. Correspondingly, the general formula of these materials can be written as R1 xBixCo2 As2, with x/ = 0.03/0.1, 0.05/0.15, 0/0.2, and 0/0.3 for R = La, Ce, Pr, and Nd, respectively. All compounds exhibit high-temperature ferromagnetic ordering of Co magnetic moments in the range of 150-200 K. Electronic band structure calculations revealed a high peak in the density of states at the Fermi level, thus supporting the itinerant nature of magnetism in the Co sublattice. The magnetic ordering in the lanthanide sublattice takes place at lower temperatures, with the R moments aligning antiparallel to the Co moments to give a ferrimagnetic ground state. The measurements on oriented single crystals demonstrated significant magnetic anisotropy in the ferrimagnetic state, with the preferred moment alignment along the c axis of the tetragonal lattice. Neutron powder diffraction failed to reveal the structure of magnetically ordered states, but confirmed the presence of Co vacancies. X-ray absorption near-edge structure spectroscopy on Ce1.95Bi0.05Co1.85As2 showed the average oxidation state of Ce to be +3.06. Solid state NMR spectroscopy revealed a substantially reduced hyperfine field on the Co atoms in the vicinity of Bi defects.

Thompson, Corey↗

Partial Spin Ordering and Complex Magnetic Structure in BaYFeO4: A Neutron Diffraction and High Temperature Susceptibility Study

The novel iron-based compound, BaYFeO4, crystallizes in the Pnma space group with two distinct Fe3+ sites, that are alternately corner-shared [FeO5]7 square pyramids and [FeO6]9 octahedra, forming into [Fe4O18]24 rings, which propagate as columns along the b-axis. A recent report shows two discernible antiferromagnetic (AFM) transitions at 36 and 48 K in the susceptibility, yet heat capacity measurements reveal no magnetic phase transitions at these temperatures. An upturn in the magnetic susceptibility measurements up to 400 K suggests the presence of shortrange magnetic behavior at higher temperatures. In this Article, variable-temperature neutron powder diffraction and hightemperature magnetic susceptibility measurements were performed to clarify the magnetic behavior. Neutron powder diffraction confirmed that the two magnetic transitions observed at 36 and 48 K are due to long-range magnetic order. Below 48 K, the magnetic structure was determined as a spin-density wave (SDW) with a propagation vector, k = (0, 0, 1/3), and the moments along the b-axis, whereas the structure becomes an incommensurate cycloid [k = (0, 0, 0.35)] below 36 K with the moments within the bc-plane. However, for both cases the ordered moments on Fe3+ are only of the order 3.0 B, smaller than the expected values near 4.5 B, indicating that significant components of the Fe moments remain paramagnetic to the lowest temperature studied, 6 K. Moreover, new high-temperature magnetic susceptibility measurements revealed a peak maximum at 550 K indicative of short-range spin correlations. It is postulated that most of the magnetic entropy is thus removed at high temperatures which could explain the absence of heat capacity anomalies at the long-range ordering temperatures. Published spin dimer calculations, which appear to suggest a k = (0, 0, 0) magnetic structure, and allow for neither low dimensionality nor geometric frustration, are inadequate to explain the observed complex magnetic structure.

Thompson, Corey↗

Unconventional magnetism in ThCr2Si2-type phosphides, La1 xNdxCo2P2

Quaternary phases La1 xNdxCo2P2 (x = 0, 0.12, 0.25, 0.37, 0.50, 0.63, 0.75, 0.88, 1.0) have been synthesized from Sn flux to investigate the origins of drastic differences in properties between ferromagnetic LaCo2P2 and antiferromagnetic NdCo2P2. Powder and single-crystal X-ray diffraction indicate that all La1 xNdxCo2P2 samples are isostructural and crystallize in the ThCr2Si2 structure type. The unit cell parameters and volume change non-linearly with the Nd content (x), with the x < 0.50 10 samples being closer to LaCo2P2 and the ones with x > 0.50 being closer to NdCo2P2. These structural differences are also reflected in the magnetic behavior. The samples with lower Nd content are characterized by ferromagnetic ordering in the Co sublattice with the TC increasing from 132 K for x = 0 to 262 K for x = 0.50, while the samples with higher Nd content exhibit suppressed magnetization in the Co sublattice and canted antiferromagnetic ordering with TC ~ 270 K. Refinement of neutron powder 15 diffraction patterns for x = 0.50 and 0.75 reveals a gradual ordering of the Nd 4f moments under the influence of Co 3d moments below 100 K. At low temperatures and zero field, these samples exhibit antiferromagnetic ordering of both Nd and Co magnetic moments, but under applied field they demonstrate the stabilization of a ferrimagnetic state with antiparallel alignment of the 4f and 3d moments, as indicated by isothermal magnetization measurements. The re-entrant ferrimagnetic transition 20 is also observed in samples with x > 0.50 if the temperature is lowered below 5 K. The occurrence of this low-temperature magnetic transition was confirmed by alternating-current susceptibility measurements.

Thompson, Corey↗

Complex magnetic behavior of the sawtooth Fe chains in Rb2Fe2O(AsO4)2

Results of magnetic eld and temperature dependent neutron diraction and magnetization mea- surements on oxy-arsenate Rb2Fe2O(AsO4)2 are reported. The crystal structure of this compound contains pseudo-one-dimensional [Fe2O6] sawtooth-like chains, formed by corner sharing isosce- les triangles of Fe3+ ions occupying two nonequivalent crystallographic sites. The chains extend innitely along the crystallographic b-axis and are structurally conned from one another via dia- magnetic (AsO4)3- units along the a-axis, and Rb+ cations along the c-axis direction. Neutron diraction measurements indicate the onset of a long range antiferromagnetic order below approxi- mately 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 b-axis, while the second site bears a canted moment in the opposite direction. Exter- nally applied magnetic eld 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 mag- netic elds 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.

Garlea, Vasile O↗

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

Neutron diffraction, 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 contains two magnetically ordered phases and four structural phases below 420 K. The complicated transitions are 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.

Ma, Jie↗

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 FeV2O4, 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, MnV2O4. We were able to reproduce the essential elements of both the magnetic ordering pattern and the dispersion of the inelastic modes with semiclassical spin-wave calculations, using a minimal model that implies a sizable 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 VO6 octahedra, previously observed via neutron powder diffractionmeasurements. We further report on the spin gap, which is an order of magnitude larger than that observed in MnV2O4. 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 FeV2O4 and MnV2O4.

MacDougall, Prof. Gregory J.↗

LaSrVO4: a candidate for the spin-orbital liquid state

A layered perovskite LaSrVO4 was studied by neutron diraction, pair distribution function measurement using synchrotron x-ray, susceptibility and specific heat measurements, and first-principles calculation. The results show (i) a weak structural distortion around 100 K with the existence of orbital fluctuations both above and below it; (ii) the absence of the long range magnetic ordering down to 0.35 K but the appearance of a short range magnetic ordering around 11 K with a T2 behavior of the specic heat below it. Meanwhile, the calculation based on the density functional theory predicts a magnetic ordered ground state. All facts indicate a melting of the magnetic ordering due to the orbital fluctuations in LaSrVO4, which makes it a rare candidate for the spin-orbital liquid state related to t2g orbitals.

Dun, Z. L.↗

Interplay between Superconductivity and Magnetism in Fe1-xPdxTe

The love/hate relationship between superconductivity and magnetic ordering has fascinated the condensed matter physics community for a century. In the early days, magnetic impurities doped into a superconductor were found to quickly suppress superconductivity. Later, a variety of systems, such as cuprates, heavy fermions and Fe pnictides, show superconductivity in a narrow region near the border to antiferromagnetism (AFM) as a function of pressure or doping. On the other hand, the coexistence of superconductivity and ferromagnetic (FM) or AFM ordering is found in a few compounds (RRh4B4 (R = Nd, Sm, Tm, Er), R'Mo6X8 (R' = Tb, Dy, Er, Ho, and X = S, Se), UMGe (M = Ge, Rh, Co), CeCoIn5, EuFe2(As1-xPx)2 etc.), providing evidence for their compatibility. Here, we present a third situation, where superconductivity coexists with FM and near the border of AFM in Fe1-xPdxTe. The doping of Pd for Fe gradually suppresses the first-order AFM ordering at temperature TN/S, and turns into short-range (SR) AFM correlation with a characteristic peak in magnetic susceptibility at T'N. Superconductivity sets in when T'N reaches zero. However, there is a gigantic ferromagnetic dome imposed in the superconducting-AFM (SR) crossover regime. Such a system is ideal for studying the interplay between superconductivity and two types of magnetic interactions (FM and AFM).

Karki, A B↗

Inhomogeneous magnetism in the doped kagome lattice of LaCuO2.66

The hole-doped kagome lattice of Cu2+ ions in LaCuO2.66 was investigated by nuclear quadrupole resonance (NQR), electron spin resonance (ESR), electrical resistivity, bulk magnetization and specific heat measurements. For temperatures above 180 K, the spin and charge properties show an activated behavior suggestive of a narrow-gap semiconductor. At lower temperatures, the results indicate an insulating ground state which may or may not be charge ordered. While the frustrated spins in remaining patches of the original kagome lattice might not be directly detected here, the observation of coexisting non-magnetic sites, free spins and frozen moments reveals an intrinsically inhomogeneous magnetism. Numerical simulations of a 1/3-diluted kagome lattice rationalize this magnetic state in terms of a heterogeneous distribution of cluster sizes and morphologies near the site-percolation threshold.

Julien, M. -H.↗

Local moments and suppression of antiferromagnetism in correlated Zr4Fe4Si7

We report magnetic, transport, and neutron diffraction measurements as well as a doping study of the V-phase compound Zr4Fe4Si7. This compound exhibits collinear antiferromagnetic order below TN = 98 1 K with a staggered moment of 0.57(3) B/Fe as T 0. The magnetic order can be quenched with Co substitution to the Fe site, but even then a 1.5 B/Fe paramagnetic moment remains. The resistivity and heat capacity of Zr4Fe4Si7 are Fermi-liquid-like below 16 and 7 K, respectively, and reveal correlations on the scale of those observed in superconducting Fe pnictides and chalcogenides. Electronic structure calculations overestimate the ordered moment, suggesting the importance of dynamical effects. The existence of magnetic order, electronic correlations, and spin fluctuations make Zr4Fe4Si7 distinct from the majority of Fe-Si compounds, fostering comparison instead with the parent compounds of Fe-based superconductors.

Simonson, Jack↗