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1.
Phys Rev B ; 103(17)2021 May.
Article in English | MEDLINE | ID: mdl-37588030

ABSTRACT

We report the magnetic ordering and structural distortion in PrFeAsO crystals, the basis compound for one of the oxypnictide superconductors, using high-resolution x-ray diffraction, neutron diffraction, and x-ray resonant magnetic scattering (XRMS). We find the structural tetragonal-to-orthorhombic phase transition at TS=147K, the AFM phase transition of the Fe moments at TFe=72K, and the Pr AFM phase transition at TPr=21K. Combined high-resolution neutron diffraction and XRMS show unambiguously that the Pr moments point parallel to the longer orthorhombic a axis and order antiferromagnetically along the a axis but ferromagnetically along the b and c directions in the stripelike AFM order. The temperature-dependent magnetic order parameter of the Pr moments shows no evidence for a reorientation of moments.

2.
Phys Rev B ; 101(21)2020 Jun.
Article in English | MEDLINE | ID: mdl-34141976

ABSTRACT

We report the electronic and magnetic properties of stoichiometric CeAuBi2 single crystals. At ambient pressure, CeAuBi2 orders antiferromagnetically below a Néel temperature (TN ) of 19 K. Neutron diffraction experiments revealed an antiferromagnetic propagation vector τ ^ = [ 0 , 0 , 1 ∕ 2 ] , which doubles the paramagnetic unit cell along the c axis. At low temperatures several metamagnetic transitions are induced by the application of fields parallel to the c axis, suggesting that the magnetic structure of CeAuBi2 changes as a function of field. At low temperatures, a linear positive magnetoresistance may indicate the presence of band crossings near the Fermi level. Finally, the application of external pressure favors the antiferromagnetic state, indicating that the 4f electrons become more localized.

3.
Phys Rev B ; 102(19)2020 Nov.
Article in English | MEDLINE | ID: mdl-37720206

ABSTRACT

We report the evolution of the magnetic properties of Ce2Rh1-xIrxIn8-yCdy single crystals. In particular, for Ce2Rh0.5Ir0.5In8 (TN=2.0K) and Ce2Rh0.5Ir0.5In7.79Cd0.21 (TN=4.2K), we have solved the magnetic structure of these compounds using single-crystal neutron magnetic diffraction experiments. Taking the magnetic structure of the Ce2RhIn8 heavy-fermion antiferromagnet as a reference, we have identified no changes in the q=12,12,0 magnetic wave vector; however, the direction of the ordered Ce3+ moments rotates toward the ab plane, under the influence of both dopants. By constraining the analysis of the crystalline electric field (CEF) with the experimental ordered moment's direction and high-temperature magnetic-susceptibility data, we have used a mean-field model with tetragonal CEF and exchange interactions to gain insight into the CEF scheme and anisotropy of the CEF ground-state wave function when Cd and Ir are introduced into Ce2RhIn8. Consistent with previous work, we find that Cd doping in Ce2RhIn8 tends to rotate the magnetic moment toward the ab plane and lower the energy of the CEF excited states' levels. Interestingly, the presence of Ir also rotates the magnetic moment towards the ab plane although its connection to the CEF overall splitting evolution for the y = 0 samples may not be straightforward. These findings may shed light on the origin of the disordered spin-glass phase on the Ir-rich side of the phase diagram and also indicate that the Ce2MIn8 compounds may not follow exactly the same Rh-Ir CEF effects trend established for the Ce2MIn5 compounds.

4.
Phys Rev Mater ; 3(9)2019.
Article in English | MEDLINE | ID: mdl-33062913

ABSTRACT

The acoustic phonons in the organic-inorganic lead halide perovskites have been reported to have anomalously short lifetimes over a large part of the Brillouin zone. The resulting shortened mean free paths of the phonons have been implicated as the origin of the low thermal conductivity. We apply neutron spectroscopy to show that the same acoustic phonon energy linewidth broadening (corresponding to shortened lifetimes) occurs in the fully inorganic CsPbBr3 by comparing the results on the organic-inorganic CH3NH3PbCl3. We investigate the critical dynamics near the three zone boundaries of the cubic P m 3 ¯ m Brillouin zone of CsPbBr3 and find energy and momentum broadened dynamics at momentum points where the Cs-site (A-site) motions contribute to the cross section. Neutron diffraction is used to confirm that both the Cs and Br sites have unusually large thermal displacements with an anisotropy that mirrors the low temperature structural distortions. The presence of an organic molecule is not necessary to disrupt the low-energy acoustic phonons at momentum transfers located away from the zone center in the lead halide perovskites and such damping may be driven by the large displacements or possibly disorder on the A site.

5.
Phys Rev B ; 1002019.
Article in English | MEDLINE | ID: mdl-33123651

ABSTRACT

The pressure evolution of the magnetic properties of the Ce2RhIn7.79Cd0.21 heavy fermion compound was investigated by single crystal neutron magnetic diffraction and electrical resistivity experiments under applied pressure. From the neutron magnetic diffraction data, up to P = 0.6 GPa, we found no changes in the magnetic structure or in the ordering temperature T N = 4.8 K. However, the increase of pressure induces an interesting spin rotation of the ordered antiferromagnetic moment of Ce2RhIn7.79Cd0.21 into the ab tetragonal plane. From the electrical resistivity measurements under pressure, we have mapped the evolution of T N and the maximum of the temperature dependent electrical resistivity (T MAX) as a function of the pressure (P ≲ 3.6 GPa). To gain some insight into the microscopic origin of the observed spin rotation as a function of pressure, we have also analyzed some macroscopic magnetic susceptibility data at ambient pressure for pure and Cd-doped Ce2RhIn8 using a mean-field model including tetragonal crystalline electric field (CEF). The analysis indicates that these compounds have a Kramers doublet Γ 7 - -type ground state, followed by a Γ 7 + first excited state at Δ1 ∼ 80 K and a Γ6 second excited state at Δ2 ∼ 270 K for Ce2RhIn8 and Δ2 ∼ 250 K for Ce2RhIn7.79Cd0.21. The evolution of the magnetic properties of Ce2RhIn8 as a function of Cd doping and the rotation of the direction of the ordered moment for the Ce2RhIn7.79Cd0.21 compound under pressure suggest important changes of the single ion anisotropy of Ce3+ induced by applying pressure and Cd doping in these systems. These changes are reflected in modifications in the CEF scheme that will ultimately affect the actual ground state of these compounds.

6.
Article in English | MEDLINE | ID: mdl-38915817

ABSTRACT

Here we report on the microstructural factors influencing the formation of the interfacial exchange bias effect in three-dimensional transition-metal-based nanocomposite systems, with relevance to permanent magnet applications. Bulk phase-separated nanocomposites consisting of the ferromagnetic α -Fe and metastable antiferromagnetic γ - Fe 70 Mn 30 phases exhibit a notable low-temperature exchange bias and substantial coercivity ( H ex = 24.6 kA / m , H C = 95.7 kA / m ) as well as a near room-temperature blocking temperature. Structural investigation by synchrotron X-ray diffraction, neutron scattering, and transmission electron microscopy confirm that the ferromagnetic α -Fe phase nucleates as small precipitates ( d ≈ 50 nm ) at the grain boundaries of the antiferromagnetic γ - Fe 70 Mn 30 grains ( d = 360 - 740 nm ) and grows anisotropically upon heat treatment, resulting in an elliptical geometry. These results indicate that optimization of the exchange bias effect in bulk nanocomposite systems may be achieved through maximizing the surface-to-volume ratio of ferromagnetic precipitates in an antiferromagnetic matrix, enhancing the magnetocrystalline anisotropy of the antiferromagnetic phase to facilitate interfacial pinning and ensuring a balanced distribution of the ferromagnetic and antiferromagnetic phases. This work further clarifies critical factors influencing the formation of an exchange bias in an inexpensive transition-metal-based bulk nanocomposite system with potential for scalable production.

7.
Phys Rev Mater ; 2(12)2018 Dec.
Article in English | MEDLINE | ID: mdl-38915935

ABSTRACT

Lead halide hybrid perovskites consist of an inorganic framework hosting a molecular cation located in the interstitial space. These compounds have been extensively studied as they have been identified as promising materials for photovoltaic applications with the interaction between the molecular cation and the inorganic framework implicated as influential for the electronic properties. CH3NH3PbCl3 undergoes two structural transitions from a high temperature cubic unit cell to a tetragonal phase at 177 K and then a subsequent orthorhombic transition at 170 K. We have measured the low-frequency lattice dynamics using neutron spectroscopy and observe an energy broadening in the acoustic phonon linewidth towards the high-symmetry point Q X = ( 2 , 1 2 , 0 ) when approaching the transitions. Concomitant with these zone boundary anomalies is a hardening of the entire acoustic phonon branch measured in the q → 0 limit near the (2, 0, 0) Bragg position with decreasing temperature. Measurements of the elastic scattering at the Brillouin zone edges Q X = ( 2 , 1 2 , 0 ) , Q M = ( 3 2 , 1 2 , 0 ) , and Q R = ( 3 2 , 3 2 , 5 2 ) show Bragg peaks appearing below these structural transitions. Based on selection rules of neutron scattering, we suggest that the higher 177 K transition is displacive with a distortion of the local octahedral environment and the lower transition is a rigid tilt transition of the octahedra. We do not observe any critical broadening in energy or momentum, beyond resolution, of these peaks near the transitions. We compare these results to the critical properties reported near the structural transitions in other perovskites and particularly CsPbCl3 [Y. Fujii, S. Hoshino, Y. Yamada, and G. Shirane, Phys. Rev. B 9, 4549 (1974)]. We suggest that the simultaneous onset of static resolution-limited Bragg peaks at the zone boundaries and the changes in acoustic phonon energies near the zone center is evidence of a coupling between the inorganic framework and the molecular cation. The results also highlight the importance of displacive transitions in organic-inorganic hybrid perovskites.

8.
Sci Rep ; 5: 17771, 2015 Dec 08.
Article in English | MEDLINE | ID: mdl-26644220

ABSTRACT

We report on the intriguing evolution of the dynamical spin correlations of the frustrated spinel ZnMn2O4. Inelastic neutron scattering and magnetization studies reveal that the dynamical correlations at high temperatures are 1D. At lower temperature, these dynamical correlations become 2D. Surprisingly, the dynamical correlations condense into a quasi 2D Ising-like ordered state, making this a rare observation of two dimensional order on the spinel lattice. Remarkably, 3D ordering is not observed down to temperatures as low as 300 mK. This unprecedented dimensional crossover stems from frustrated exchange couplings due to the huge Jahn-Teller distortions around Mn(3+) ions on the spinel lattice.

9.
Article in English | MEDLINE | ID: mdl-26900514

ABSTRACT

The new thermal triple-axis spectrometer at the NIST Center for Neutron Research (NCNR) is located at the BT-7 beam port. The 165 mm diameter reactor beam is equipped with a selection of Söller collimators, beam-limiters, and a pyrolytic graphite (PG) filter to tailor the beam for the dual 20×20 cm(2) double-focusing monochromator system that provides monochromatic fluxes exceeding 10(8) n/cm(2)/s onto the sample. The two monochromators installed are PG(002) and Cu(220), which provide incident energies from 5 meV to above 500 meV. The computer controlled analyzer system offers six standard modes of operation, including a diffraction detector, a position-sensitive detector (PSD) in diffraction mode, horizontal energy focusing analyzer with detector, a Q-E mode employing a flat analyzer and PSD, a constant-E mode with the analyzer crystal system and PSD, and a conventional mode with a selection of Söller collimators and detector. Additional configurations for specific measurement needs are also available. This paper discusses the capabilities and performance for this new state-of-the-art neutron spectrometer.

10.
Phys Rev Lett ; 107(20): 207206, 2011 Nov 11.
Article in English | MEDLINE | ID: mdl-22181767

ABSTRACT

Polarized small-angle neutron scattering studies of single-crystalline multiferroic BiFeO(3) reveal a long-wavelength spin density wave generated by ∼1° spin canting of the spins out of the rotation plane of the antiferromagnetic cycloidal order. This signifies weak ferromagnetism within mesoscopic regions of dimension 0.03 microns along [110], to several microns along [111], confirming a long-standing theoretical prediction. The average local magnetization is 0.06 µ(B)/Fe. Our results provide an indication of the intrinsic macroscopic magnetization to be expected in ferroelectric BiFeO(3) thin films under strain, where the magnetic cycloid is suppressed.

11.
Phys Rev Lett ; 107(6): 067203, 2011 Aug 05.
Article in English | MEDLINE | ID: mdl-21902365

ABSTRACT

Neutron diffraction is used to show that small (∼7 MPa, or 70 bar) uniaxial pressure produces significant changes in the populations of magnetic domains in a single crystal of 2% Nd-doped bismuth ferrite. The magnetic easy plane of the domains converted by the pressure is rotated 60° relative to its original position. These results demonstrate extreme sensitivity of the magnetic properties of multiferroic bismuth ferrite to tiny (less than 10(-4)) elastic strain, as well as weakness of the forces pinning the domain walls between the cycloidal magnetic domains in this material.

12.
Phys Rev Lett ; 103(3): 037201, 2009 Jul 17.
Article in English | MEDLINE | ID: mdl-19659312

ABSTRACT

Using synchrotron x-ray and neutron diffraction, we disentangle spin-lattice order in highly frustrated ZnCr2O4 where magnetic chromium ions occupy the vertices of regular tetrahedra. Upon cooling below 12.5 K the quandary of antialigning spins surrounding the triangular faces of tetrahedra is resolved by establishing weak interactions on each triangle through an intricate lattice distortion. However, the resulting spin order is not simply a Néel state on strong bonds, but rather a complex coplanar spin structure, indicating that antisymmetric and/or further neighbor exchange interactions also play a role as ZnCr2O4 resolves conflicting magnetic interactions.

13.
Phys Rev Lett ; 102(18): 187202, 2009 May 08.
Article in English | MEDLINE | ID: mdl-19518906

ABSTRACT

Ising chain compound Ca3Co2-xMnxO6 exhibits up-up-down-down long-range magnetic order (LRO) in a broad range of 0.75

14.
J Phys Condens Matter ; 21(45): 456008, 2009 Nov 11.
Article in English | MEDLINE | ID: mdl-21694028

ABSTRACT

The conical spin order of multiferroic CoCr(2)O(4) has been studied by a neutron diffraction to investigate its magnetic phase transitions at temperatures below 40 K. Magnetic order of a spiral spin component with an incommensurate propagation vector of (0.63, 0.63, 0) was observed at 26 K, while at 14.5 K, the incommensurate conical spin order showed a transition into the fixed commensurate propagation vector of (2/3,2/3,0). In addition, two satellite peaks with propagation vectors of (0.035, 0, 0) and (0, 0.035, 0) from the commensurate vector were observed. The widths of these peaks indicate a long-range magnetic order. This new magnetic configuration below 14.5 K may lead to a new model of multiferroic behavior differing from the well-known spin-current model for magnetic ferroelectricity.

15.
Phys Rev Lett ; 101(16): 167203, 2008 Oct 17.
Article in English | MEDLINE | ID: mdl-18999708

ABSTRACT

We report inelastic neutron scattering studies of magnetic excitations in antiferromagnetically ordered SrFe2As2 (T_{N}=200-220 K), the parent compound of the FeAs-based superconductors. At low temperatures (T=7 K), the magnetic spectrum S(Q,Planck's omega) consists of a Bragg peak at the elastic position (Planck's omega=0 meV), a spin gap (Delta< or =6.5 meV), and sharp spin-wave excitations at higher energies. Based on the observed dispersion relation, we estimate the effective magnetic exchange coupling using a Heisenberg model. On warming across T_{N}, the low-temperature spin gap rapidly closes, with weak critical scattering and spin-spin correlations in the paramagnetic state. The antiferromagnetic order in SrFe2As2 is therefore consistent with a first order phase transition, similar to the structural lattice distortion.

16.
Phys Rev Lett ; 101(13): 135703, 2008 Sep 26.
Article in English | MEDLINE | ID: mdl-18851463

ABSTRACT

Elastic neutron-scattering, inelastic x-ray scattering, specific-heat, and pressure-dependent electrical transport measurements have been made on single crystals of AuZn and Au0.52Zn0.48. Elastic neutron scattering detects new commensurate Bragg peaks (modulation) appearing at Q =(1.33,0.67,0) at temperatures corresponding to each sample's transition temperature (TM = 64 and 45 K, respectively). Although the new Bragg peaks appear in a discontinuous manner in the Au0.52Zn0.48 sample, they appear in a continuous manner in AuZn. Surprising us, the temperature dependence of the AuZn Bragg peak intensity and the specific-heat jump near TM are in favorable accord with a continuous transition. A fit to the pressure dependence of TM suggests the presence of a critical end point in the AuZn phase diagram located at TM* = 2.7 K and p* = 3.1 GPa.


Subject(s)
Gold Alloys/chemistry , Zinc/chemistry , Biocompatible Materials/chemistry , Neutron Diffraction , Temperature , Thermodynamics , X-Ray Diffraction
17.
Phys Rev Lett ; 101(13): 137203, 2008 Sep 26.
Article in English | MEDLINE | ID: mdl-18851488

ABSTRACT

We have studied quasi-two-dimensional multiferroic LuFe2O4 with strong charge-spin-lattice coupling, in which low-temperature coercivity approaches an extraordinary value of 9 T in single crystals. The enhancement of the coercivity is connected to the collective freezing of nanoscale pancakelike ferrimagnetic domains with large uniaxial magnetic anisotropy ("Ising pancakes"). Our results suggest that collective freezing in low-dimensional magnets with large uniaxial anisotropy provides an effective mechanism to achieve enhanced coercivity. This observation may help identify novel approaches for synthesis of magnets with enhanced properties.

18.
Nature ; 453(7197): 899-902, 2008 Jun 12.
Article in English | MEDLINE | ID: mdl-18509333

ABSTRACT

Following the discovery of long-range antiferromagnetic order in the parent compounds of high-transition-temperature (high-T(c)) copper oxides, there have been efforts to understand the role of magnetism in the superconductivity that occurs when mobile 'electrons' or 'holes' are doped into the antiferromagnetic parent compounds. Superconductivity in the newly discovered rare-earth iron-based oxide systems ROFeAs (R, rare-earth metal) also arises from either electron or hole doping of their non-superconducting parent compounds. The parent material LaOFeAs is metallic but shows anomalies near 150 K in both resistivity and d.c. magnetic susceptibility. Although optical conductivity and theoretical calculations suggest that LaOFeAs exhibits a spin-density-wave (SDW) instability that is suppressed by doping with electrons to induce superconductivity, there has been no direct evidence of SDW order. Here we report neutron-scattering experiments that demonstrate that LaOFeAs undergoes an abrupt structural distortion below 155 K, changing the symmetry from tetragonal (space group P4/nmm) to monoclinic (space group P112/n) at low temperatures, and then, at approximately 137 K, develops long-range SDW-type antiferromagnetic order with a small moment but simple magnetic structure. Doping the system with fluorine suppresses both the magnetic order and the structural distortion in favour of superconductivity. Therefore, like high-T(c) copper oxides, the superconducting regime in these iron-based materials occurs in close proximity to a long-range-ordered antiferromagnetic ground state.

19.
Phys Rev Lett ; 94(13): 137202, 2005 Apr 08.
Article in English | MEDLINE | ID: mdl-15904023

ABSTRACT

The spin-lattice coupling plays an important role in strongly frustrated magnets. In ZnCr2O4, an excellent realization of the Heisenberg antiferromagnet on the pyrochlore network, a lattice distortion relieves the geometrical frustration through a spin-Peierls-like phase transition at T(c)=12.5 K. Conversely, spin correlations strongly influence the elastic properties of a frustrated magnet. By using infrared spectroscopy and published data on magnetic specific heat, we demonstrate that the frequency of an optical phonon triplet in ZnCr2O4 tracks the nearest-neighbor spin correlations above T(c). The splitting of the phonon triplet below T(c) provides a way to measure the spin-Peierls order parameter.

20.
Phys Rev Lett ; 92(5): 056402, 2004 Feb 06.
Article in English | MEDLINE | ID: mdl-14995323

ABSTRACT

The transition-metal spinel MgTi2O4 undergoes a metal-insulator (M-I) 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 MgTi2O4, 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, MgTi2O4 is an orbitally ordered band insulator.

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