arXiv subjects

Pascal Manuel

Publications and source records attributed to Pascal Manuel.

At least 55 records · Page 3Linked to original sources

arXiv2020

Neutron diffraction and symmetry analysis of the martensitic transformation in Co-doped Ni$_2$MnGa

Martensitic transformations are strain driven displacive transitions governing the mechanical and physical properties in intermetallic materials. This is the case in Ni$_2$MnGa, where the martensite transition is at the heart of the striking magnetic shape memory and magneto-caloric properties. Interestingly, the martensitic transformation is preceded by a pre-martensite phase, and the role of this precursor and its influence on the martensitic transition and properties is still a matter of debate. In this work, we report on the influence of Co doping (Ni$_{50-x}$Co$_x$Mn$_{25}$Ga$_{25}$ with x = 3 and 5) on the martensitic transformation path in stoichiometric Ni$_2$MnGa by neutron diffraction. The use of the superspace formalism to describe the crystal structure of the modulated martensitic phases, joined with a group theoretical analysis allows unfolding the different distortions featuring the structural transitions. Finally, a general Landau thermodynamic potential of the martensitic transformation, based on the symmetry analysis is outlined. The combined use of phenomenological and crystallographic studies highlights the close relationship between the lattice distortions at the core of the Ni$_2$MnGa physical properties and, more in general, on the properties of the martensitic transformations in the Ni-Mn based Heusler systems.

cond-mat.mtrl-sci↗

arXiv2020

Strong quantum fluctuations due to competition between magnetic phases in a pyrochlore iridate

We report neutron diffraction measurements of the magnetic structures in two pyrochlore iridates, Yb2Ir2O7 and Lu2Ir2O7. Both samples exhibit the all-in-all-out magnetic structure on the Ir4+ sites below TN~ 150,K, with a low temperature moment of around 0.45 muB/Ir. Below 2\,K, the Yb moments in Yb2Ir2O7 begin to order ferromagnetically. However, even at 40 mK the ordered moment is only 0.57(3)muB/Yb, well below the saturated moment of the ground state doublet of Yb3+ (1.9 muB/Yb), deduced from magnetization measurements and from a refined model of the crystal field environment, and also significantly smaller than the ordered moment of Yb in Yb2Ti2O7 (0.9 muB/Yb). A mean-field analysis shows that the reduced moment on Yb is a consequence of enhanced phase competition caused by coupling to the all-in-all-out magnetic order on the Ir sublattice.

cond-mat.str-el↗

arXiv2019

Large Easy Axis Anisotropy in the One-Dimensional Magnet BaMo(PO$_4$)$_2$

We present an extensive experimental and theoretical study on the low-temperature magnetic properties of the monoclinic anhydrous alum compound BaMo(PO$_4$)$_2$. The magnetic susceptibility reveals strong antiferromagnetic interactions $θ_{CW} = -167$~K and long-range magnetic order at $T_N=22$~K, in agreement with a recent report. Powder neutron diffraction furthermore shows that the order is collinear, with the moments near the $ac$ plane. Neutron spectroscopy reveals a large excitation gap $Δ= 15$~meV in the low-temperature ordered phase, suggesting a much larger easy-axis spin anisotropy than anticipated. However, the large anisotropy justifies the relatively high ordered moment, Néel temperature, and collinear order observed experimentally, and is furthermore reproduced in a first principles calculations using a new computational scheme. We therefore propose BaMo(PO$_4$)$_2$ to host $S=1$ antiferromagnetic chains with large easy-axis anisotropy, which has been theoretically predicted to realize novel excitation continua.

cond-mat.str-el↗

arXiv2019

Giant spontaneous exchange bias in an antiperovskite structure driven by a canted triangular magnetic structure

Exchange bias (EB) refers to a shift of the hysteresis loop along the field axis in materials consisting of ferromagnetic (FM) and antiferromagnetic (AFM) layers, generally after a cooling procedure in high magnetic field. This effect is highly desirable for technological applications ranging from spintronics to magnetic recording. Achieving giant EB effect near room temperature in a small cooling field is thus an on-going technologically relevant challenge for the materials science community. In this work, we present the experimental realization of such a fundamental goal by demonstrating the existence of giant EB after a zero field cooled (ZFC) procedure in antiperovskite Mn3.5Co0.5N below 256 K. We found that it exhibits an EB field of 0.28 T at 50 K after a ZFC procedure accompanied by a large vertical magnetization shift (VMS). Interestingly, this EB field can be elevated up to 1.2 T after a cooling procedure with a small applied field of just 500 Oe. Mn3:5Co0:5N bears the first intermetallic material showing a strong correlation between EB and VMS.We attribute the observed EB effect to a completely new canted triangular magnetic structure determined by neutron diffraction experiment. Finally, we discuss the striking effect of Co substitution on the physical properties of antiperovskite materials and put forward a new strategy for antiperovskite lattice to exploit new single phase materials showing large EB effect at room temperature.

cond-mat.str-el↗

arXiv2019

Colossal magnetoresistance in the insulating ferromagnetic double perovskites Tl$_2$NiMnO$_6$: A neutron diffraction study

In the family of double perovskites, colossal magnetoresistance (CMR) has been so far observed only in half-metallic ferrimagnets such as the known case Sr$_2$FeMoO$_6$ where it has been assigned to the tunneling MR at grain boundaries due to the half-metallic nature. Here we report a new material-Tl$_2$NiMnO$_6$, a relatively ordered double perovskite stablized by the high pressure and high temperature synthesis-showing CMR in the vicinity of its Curie temperature. We explain the origin of such effect with neutron diffraction experiment and electronic structure calculations that reveal the material is a ferromagnetic insulator. Hence the ordered Tl$_2$NiMnO$_6$ (~70% of Ni$^{2+}$/Mn$^{4+}$ cation ordering) represents the first realization of a ferromagnetic insulating double perovskite, showing CMR. The study of the relationship between structure and magnetic properties allows us to clarify the nature of spin glass behaviour in the disordered Tl$_2$NiMnO$_6$ (~31% of cation ordering), which is related to the clustering of antisite defects and associated with the short-range spin correlations. Our results highlight the key role of the cation ordering in establishing the long range magnetic ground state and lay out new avenues to exploit advanced magnetic materials in double perovskites.

cond-mat.str-el↗

arXiv2019

Determining the anisotropy and exchange parameters of polycrystalline spin-1 magnets

Although low-dimensional $S = 1$ antiferromagnets remain of great interest, difficulty in obtaining high-quality single crystals of the newest materials hinders experimental research in this area. Polycrystalline samples are more readily produced, but there are inherent problems in extracting the magnetic properties of anisotropic systems from powder data. Following a discussion of the effect of powder-averaging on various measurement techniques, we present a methodology to overcome this issue using thermodynamic measurements. In particular we focus on whether it is possible to characterise the magnetic properties of polycrystalline, anisotropic samples using readily available laboratory equipment. We test the efficacy of our method using the magnets [Ni(H$_{2}$O)$_{2}$(3,5-lutidine)$_{4}$](BF$_{4}$)$_{2}$ and Ni(H$_{2}$O)$_{2}$(acetate)$_{2}$(4-picoline)$_{2}$, which have negligible exchange interactions, as well as the antiferromagnet [Ni(H$_{2}$O)$_{2}$(pyrazine)$_{2}$](BF$_{4}$)$_{2}$, and show that we are able to extract the anisotropy parameters in each case. The results obtained from the thermodynamic measurements are checked against electron-spin resonance and neutron diffraction. We also present a density functional method, which incorporates spin-orbit coupling to estimate the size of the anisotropy in [Ni(H$_{2}$O)$_{2}$(pyrazine)$_{2}$](BF$_{4}$)$_{2}$.

cond-mat.str-el↗

arXiv2019

Magnetic frustration and spontaneous rotational symmetry breaking in PdCrO2

In the triangular layered magnet PdCrO2 the intralayer magnetic interactions are strong, however the lattice structure frustrates interlayer interactions. In spite of this, long-range, 120$^\circ$ antiferromagnetic order condenses at $T_N = 38$~K. We show here through neutron scattering measurements under in-plane uniaxial stress and in-plane magnetic field that this occurs through a spontaneous lifting of the three-fold rotational symmetry of the nonmagnetic lattice, which relieves the interlayer frustration. We also show through resistivity measurements that uniaxial stress can suppress thermal magnetic disorder within the antiferromagnetic phase.

cond-mat.str-el↗

arXiv2019

Anisotropy in the magnetization and magnetoelectric response of single crystalline Mn$_{4}$Ta$_{2}$O$_{9}$

We report temperature dependent magnetization and neutron diffraction measurements on the corundum related magnetoelectric antiferromagnet Mn$_{4}$Ta$_{2}$O$_{9}$. Measurements performed on a single crystalline specimen reveal that the magnetization is anisotropic, and a weak ferromagnetic component emerges well within the antiferromagnetically ordered state. Powder neutron diffraction measurements indicate that the magnetic structure comprises of antiferromagnetically coupled ferromagnetic chains of Mn$^{2+}$ spins aligned along the trigonal $c$ axis, in contrast to that reported in other isostructural members of this family. Magnetic measurements performed under a periodic electric field indicate that the magnetoelectric response is also anisotropic, with this coupling along the trigonal $c$ axis and that perpendicular to it having different signs.

cond-mat.str-el↗

arXiv2019

Rich magnetoelectric phase diagrams of multiferroic single-crystal alpha-NaFeO2

The magnetic and dielectric properties of the multiferroic triangular lattice magnet compound alpha-NaFeO2 were studied by magnetization, specific heat, dielectric permittivity, and pyroelectric current measurements and by neutron diffraction experiments using single crystals grown by a hydrothermal synthesis method. This work produced magnetic field (in the monoclinic ab-plane, B_ab, and along the c*-axis, B_c) versus temperature magnetic phase diagrams, including five and six magnetically ordered phases in B_ab and along B_c, respectively. Comparing the polarization direction to the magnetic structures in the different ferroelectric phases, we conclude that the extended inverse Dzyaloshinskii-Moriya mechanism expressed by the orthogonal components p1 ~ rij x (Si x Sj ) and p2 ~ Si x Sj can explain the polarization directions. Based on calculations incorporating exchange interactions up to fourth-nearest-neighbor (NN) couplings, we infer that competition among antiferromagnetic second NN interactions in the triangular lattice plane, as well as weak interplane antiferromagnetic interactions, are responsible for the rich phase diagrams of alpha-NaFeO2.

cond-mat.str-el↗

arXiv2019

Spin and orbital ordering in TlMnO3: Neutron diffraction study

Crystal and magnetic structures of the high-pressure stabilized perovskite phase of TlMnO3 have been studied by neutron powder diffraction. The crystal structure involves two types of primary structural distortions: a+b-b-octahedral tilting and antiferrodistortive type of orbital ordering, whose common action reduces the symmetry down to triclinic P -1. The orbital pattern and the way it is combined with the octahedral tilting are different from the family of LnMnO3 (Ln = lanthanide or Y) manganites who share with TlMnO3 the same tilting scheme. The experimentally determined magnetic structure with the k = (1/2,0,1/2) propagation vector and P_S-1 symmetry implies anisotropic exchange interactions with a ferromagnetic coupling within the (1,0,-1) planes and an antiferromagnetic one between them (A type). The spins in the primary magnetic mode were found to be confined close to the (1,0,-1) plane, which underlines the predominant role of the single ion anisotropy with the local easy axes of Mn3+ following the Jahn-Teller distortions of the octahedra. In spite of the same octahedral tilting scheme in the perovskite structures of both LnMnO3 and TlMnO3 manganites, a coupling of the secondary ferromagnetic component to the primary A-type spin configuration through antisymmetric exchange interaction is allowed in the former and forbidden in the latter cases.

cond-mat.str-el↗

arXiv2019

Magnetic ordering and ferroelectricity in multiferroic 2H-AgFeO2: Comparison between hexagonal and rhombohedral polytypes

Magnetic and dielectric properties of the hexagonal triangular lattice antiferromagnet 2H-AgFeO2 have been studied by neutron diffraction, magnetic susceptibility, specific heat, pyroelectric current, and dielectric constant measurements. The ferroelectric polarization, P ~ 5 μC/m2, has been found to appear below 11 K due to a polar nature of the magnetic ground state of the system. In the temperature range of 11 K < T < 18 K, an incommensurate spin density wave (ICM1) with the nonpolar magnetic point group mmm1' and the k1 = (0,q1_b,0; q1_b = 0.390-0.405)propagation vector takes place. Below 14 K, a proper screw ordering (ICM2) and k2 = (0,q2_b,0; q2_b = 0.385-0.396) appears as a minor phase which coexists with ICM1 and the ground state down to the lowestmeasured temperature 5.5 K. No ferroelectric polarization associated with the ICM2 phase was observed in agreement with its nonpolar point group 2221'. Finally, a spiral order with cycloid and proper screw components (ICM3), and k3 = (q3_a,q3_b,0; q3_a = 0.0467, q3_b = 0.349) emerges below 11 K as the ground state of the system. Based on the deduced magnetic point group 21', we conclude that the ferroelectric polarization in ICM3 is parallel to the c axis and is caused by the inverse Dzyloshinskii-Moriya effect with p1 ~ rij x (Si x Sj ). Unlike the rhombohedral 3R-AgFeO2 polytype, the additional contribution to the macroscopic polarization p2 ~ Si x Sj is not allowed in the present case due to the symmetry constraints imposed by the hexagonal lattice of 2H-AgFeO2.

cond-mat.str-el↗

arXiv2019

Magnetic ordering in pressure-induced phases with giant spin-driven ferroelectricity in multiferroic TbMnO3

In order to clarify the mechanism associated with pressure/magnetic-field-induced giant ferroelectric polarization in TbMnO3, this work investigated changes in magnetic ordering brought about by variations in temperature, magnetic field, and pressure. This was accomplished by means of neutron diffraction analyses under high pressures and high magnetic fields, employing a single crystal. The incommensurate magnetic ordering of a cycloid structure was found to be stable below the reported critical pressure of 4.5 GPa. In contrast, a commensurate E-type spin ordering of Mn spins and a noncollinear configuration of Tb spins with k=(0,1/2,0) appeared above 4.5 GPa. The application of a magnetic field along the a axis (H_{||a}) under pressure induces a k=(0,0,0)antiferromagnetic structure in the case of Tb spins above H_{||a}, enhancing the ferroelectric polarization, while the E-type ordering of Mn spins is stable even above the critical field. From the present experimental findings, we conclude that the E-type ordering of Mn spins induces giant ferroelectric polarization through an exchange striction mechanism. The H_{||a}-induced polarization enhancement can be understood by considering that the polarization, reduced by the polar ordering of Tb moments in a zero field, can be recovered through a field-induced change to nonpolar k=(0,0,0) ordering at H_{||a} ~ 2T.

cond-mat.str-el↗

arXiv2019

Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO$_2$

We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whereas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70\,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. This phase is gapless and shows a non-trivial evolution of the low-temperature specific heat. Our work demonstrates that NaYbO$_2$ practically gives the most direct experimental access to the spin-liquid physics of triangular antiferromagnets.

cond-mat.str-el↗

arXiv2018

Unravelling the complex magnetic structure of multiferroic pyroxene NaFeGe2O6: A combined experimental and theoretical study

Magnetic order and the underlying magnetic model of the multiferroic pyroxene NaFeGe2O6 are systematically investigated by neutron powder diffraction, thermodynamic measurements, density-functional bandstructure calculations, and Monte-Carlo simulations. Upon cooling, NaFeGe2O6 first reveals one-dimensional spin-spin correlations in the paramagnetic state below about 50 K, revealed by magnetic diffuse scattering. The sinusoidal spin-density wave with spins along the a-direction sets in at 13 K, followed by the cycloidal configuration with spins lying in the (ac) plane below 11.6 K. Microscopically, the strongest magnetic coupling runs along the structural chains, J1 ' 12 K, which is likely related to the one-dimensional spin-spin correlations. The interchain couplings J2 ' 3:8K and J3 ' 2:1K are energetically well balanced and compete, thus giving rise to the incommensurate order in sharp contrast to other transition-metal pyroxenes, where one type of the interchain couplings prevails. The magnetic model of NaFeGe2O6 is further completed by the weak single-ion anisotropy along the a-direction. Our results resolve the earlier controversies regarding the magnetic order in NaFeGe2O6 and establish relevant symmetries of the magnetic structures. These results, combined with symmetry analysis, enable us to identify the possible mechanisms of the magnetoelectric coupling in this compound. We also elucidate microscopic conditions for the formation of incommensurate magnetic order in pyroxenes.

cond-mat.str-el↗

arXiv2018

Spin Jahn-Teller antiferromagnetism in CoTi$_2$O$_5$

We have used neutron powder diffraction to solve the magnetic structure of orthorhombic CoTi$_2$O$_5$, showing that the long-range ordered state below 26 K identified in our muon-spin rotation experiments is antiferromagnetic with propagation vector ${\bf k}=(\pm \frac{1}{2}, \frac{1}{2}, 0)$ and moment of 2.72(1)$μ_{\rm B}$ per Co$^{2+}$ ion. This long range magnetic order is incompatible with the experimentally determined crystal structure because the imposed symmetry completely frustrates the exchange coupling. We conclude that the magnetic transition must therefore be associated with a spin Jahn-Teller effect which lowers the structural symmetry and thereby relieves the frustration. These results show that CoTi$_2$O$_5$ is a highly unusual low symmetry material exhibiting a purely spin-driven lattice distortion critical to the establishment of an ordered magnetic ground state.

cond-mat.str-el↗

arXiv2018

Investigating the magnetic ground state of the skyrmion host material Cu$_{2}$OSeO$_{3}$ using long-wavelength neutron diffraction

We present long-wavelength neutron diffraction data measured on both single crystal and polycrystalline samples of the skyrmion host material Cu$_{2}$OSeO$_{3}$. We observe magnetic satellites around the $(0\bar{1}1)$ diffraction peak not accessible to other techniques, and distinguish helical from conical spin textures in reciprocal space. We confirm successive transitions from helical to conical to field polarised ordered spin textures as the external magnetic field is increased. The formation of a skyrmion lattice with propagation vectors perpendicular to the field direction is observed in a region of the field-temperature phase diagram that is consistent with previous reports. Our measurements show that not only the field-polarised phase but also the helical ground state are made up of ferrimagnetic clusters instead of individual spins. These clusters are distorted Cu tetrahedra, where the spin on one Cu ion is anti-aligned with the spin on the three other Cu ions.

cond-mat.mtrl-sci↗

arXiv2018

Incommensurate atomic and magnetic modulations in the spin-frustrated β-NaMnO2 triangular lattice

The layered β-NaMnO2, a promising Na-ion energy-storage material has been investigated for its triangular lattice capability to promote complex magnetic configurations that may release symmetry restrictions for the coexistence of ferroelectric and magnetic orders. The complexity of the neutron powder diffraction patterns underlines that the routinely adopted commensurate structural models are inadequate. Instead, a single-phase superspace symmetry description is necessary, demonstrating that the material crystallizes in a compositionally modulated q= (0.077(1), 0, 0) structure. Here, Mn3+ Jahn-Teller distorted MnO6 octahedra form corrugated layer stacking sequences of the β-NaMnO2 type, which are interrupted by flat sheets of the α-like oxygen topology. Spontaneous long-range collinear antiferromagnetic order, defined by the propagation vector k= (1/2, 1/2, 1/2), appears below TN1= 200 K. Moreover, a second transition into a spatially modulated proper-screw magnetic state (k+-q) is established at TN2= 95 K, with an antiferromagnetic order parameter resembling that of a two-dimensional (2D) system. The evolution of 23Na NMR spin-lattice relaxation identifies a magnetically inhomogene-ous state in the intermediate T-region (TN2 <T< TN1), while its strong suppression below TN2 indicates that a spin-gap opens in the excitation spectrum. High-resolution neutron inelastic scattering confirms that the magnetic dynamics are indeed gapped (Δ~5 meV) in the low-temperature magnetic phase, while simulations on the basis of the single-mode approximation suggest that Mn-spins residing on ad-jacent antiferromagnetic chains, establish sizable 2D correlations. Our analysis points that novel struc-tural degrees of freedom promote, cooperative magnetism and emerging dielectric properties in this non-perovskite-type of manganite.

cond-mat.mtrl-sci↗

arXiv2018

Low-dimensional quantum magnetism in Cu(NCS)$_2$: A molecular framework material

Low-dimensional magnetic materials with spin-$\frac{1}{2}$ moments can host a range of exotic magnetic phenomena due to the intrinsic importance of quantum fluctuations to their behavior. Here, we report the structure, magnetic structure and magnetic properties of copper(II) thiocyanate, Cu(NCS)$_2$, a one-dimensional coordination polymer which displays low-dimensional quantum magnetism. Magnetic susceptibility, electron paramagnetic resonance (EPR) spectroscopy, $^{13}$C magic-angle spinning nuclear magnetic resonance (MASNMR) spectroscopy, and density functional theory (DFT) investigations indicate that Cu(NCS)$_2$ behaves as a two-dimensional array of weakly coupled antiferromagnetic spin chains ($J_2 = 133(1)$ K, $α= J_1/J_2 = 0.08$). Powder neutron-diffraction measurements confirm that Cu(NCS)$_2$ orders as a commensurate antiferromagnet below $T_\mathrm{N} = 12$ K, with a strongly reduced ordered moment (0.3 $μ_\mathrm{B}$) due to quantum fluctuations.

cond-mat.str-el↗