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Martin Meven

Publications and source records attributed to Martin Meven.

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Magnetic excitation spectrum and hierarchy of magnetic interactions in ErFeO3

We report a comprehensive investigation of the excitation spectrum of ErFeO$_3$ orthoferrite by means of time-of-flight neutron spectroscopy. The spectrum consists of two distinct components: strongly dispersive spin wave excitations of the Fe$^{3+}$ sublattice spanning $\approx$~9 - 65 meV, and crystal electric field (CEF) excitations of Er$^{3+}$ ions below 36 meV. The observed spin wave dispersions and spectral weight are well captured within linear spin wave theory, enabling extraction of the key Fe-Fe exchange parameters. Low-energy incident neutrons with their enhanced energy resolution, further revealed the dispersive character and splitting of Kramers-degenerate CEF levels. We show that the dispersion is caused by the exchange coupling between Er$^{3+}$ ions, while the degeneracy is lifted by interactions between the Er$^{3+}$ and Fe$^{3+}$ sublattices. We further explore the influence of dipolar and antisymmetric exchange interactions with the focus on the magnetic ground state of ErFeO$_3$, with particular attention to the low-temperature spin arrangement. Taken together, our results provide a detailed account of the spin dynamics in ErFeO$_3$ and reveal a hierarchy of interactions scales characteristic for orthoferrites.

cond-mat.str-el

Tilted and Twisted Magnetic Moments in the Kitaev Magnet $\alpha$-RuCl$_3$

The layered honeycomb magnet $\alpha$-RuCl$_3$ has attracted intense scrutiny as a prime candidate for realizing the Kitaev quantum spin liquid, yet a consensus on its microscopic Hamiltonian remains elusive due to the material's extreme sensitivity to structural details. Here, we report a comprehensive reexamination of the low-temperature crystallographic and magnetic structures of high-quality $\alpha$-RuCl$_3$ single crystals using unpolarized and polarized neutron diffraction. We confirm a sharp, first-order structural phase transition to the rhombohedral $R\bar{3}$ space group with a pronounced thermal hysteresis. Crucially, using both spherical and longitudinal neutron polarization analysis, we determine the 3D orientation of the ordered magnetic moment without the ambiguity typically arising from domain distributions. We find that the Ru$^{3+}$ magnetic moments in the zigzag phase are tilted by $15.7^\circ$ out of the hexagonal plane and, remarkably, exhibit an additional in-plane twist of $-13.8^\circ$. This "tilted and twisted" geometry differentiates the ground state from the previously reported models based on unpolarized neutron diffraction or resonant elastic X-ray scattering (REXS) analysis.

cond-mat.str-el

Phonons reflect dynamic spin-state order in LaCoO$_3$

We investigate lattice dynamics in LaCoO$_3$ using inelastic neutron and x-ray scattering over $T = 2\mbox{-}650\,\mathrm{K}$, spanning the spin-state crossover at $T_{1} \approx 100\,\mathrm{K}$ and the insulator--metal transition at $T_{2} \approx 550\,\mathrm{K}$. Comparison with quasi-harmonic $ab-initio$ lattice-dynamical calculations helps reveal anomalous softening of a $\approx 10\,\mathrm{meV}$ oxygen phonon, confined to the temperature interval $T_{1} \leq T \leq T_{2}$ and localized in momentum space at $\boldsymbol{q}_{\mathrm{SSO}} = \left( \frac{1}{2},\frac{1}{2},\frac{1}{2} \right)_{c}$. This wave vector corresponds to the spin-state ordering originally proposed by Goodenough [J. Phys. Chem. Solids 6, 287-297 (1958)]. Our results therefore provide momentum-resolved evidence for dynamic correlations of high-spin and low-spin Co$^{3+}$ states in LaCoO$_{3}$, linking spin-state fluctuations to anomalous phonon renormalization.

cond-mat.str-el

Flat band-engineered spin-density wave and the emergent multi-$k$ magnetic state in the topological kagome metal Mn$_{3}$Sn

Magnetic kagome metals, in which topologically non-trivial band structures and electronic correlation are intertwined, have recently emerged as an exciting platform to explore exotic correlated topological phases, that are usually not found in weakly interacting materials described within the semi-classical picture of electrons. Here, via a comprehensive single-crystal neutron diffraction and first-principles density functional theory study of the archetypical topological kagome metal Mn$_3$Sn, which is also a magnetic Weyl fermion material and a promising chiral magnet for antiferromagnetic spintronics, we report the realisation of an emergent spin-density wave (SDW) order, a hallmark correlated many-body phenomenon, that is engineered by the Fermi surface nesting of topological flat bands. We further reveal that the phase transition, from the well-known high-temperature coplanar and non-collinear k = 0 inverse triangular antiferromagnetic order to a double-$k$ non-coplanar modulated incommensurate magnetic structure below $T_1$ = 280 K, is primarily driven by the SDW instability. The double-$k$ nature of this complex low-temperature magnetic order, which can be regarded as an intriguing superposition of a longitudinal SDW with a modulation wavevector k$_L$ and a transverse incommensurate helical magnetic order with a modulation wavevector k$_T$, is unambiguously confirmed by our observation of the inter-modulation high-order harmonics of the type of 2k$_L$+k$_T$. This discovery not only solves a long-standing puzzle concerning the nature of the phase transition at $T_1$, but also provides an extraordinary example on the intrinsic engineering of correlated many-body phenomena in topological matter. The identified multi-$k$ magnetic state can be further exploited for the engineering of the new modes of magnetization and chirality switching in antiferromagnetic spintronics.

cond-mat.str-el

Unconventional magneto-resistance, and electronic transition in Mn$_3$Ge Weyl semimetal

Weyl semimetals are well known for their anomalous transport effects caused by a large fictitious magnetic field generated by the non-zero Berry curvature. We performed the analysis of the electrical transport measurements of the magnetic Weyl semimetal Mn$_{3}$Ge in the a-b and a-c plane. We have observed negative longitudinal magneto-resistance (LMR) at a low magnetic field ($B<1.5$ T) along all the axes. The high field LMR shows different behavior along x and z axes. A similar trend has been observed in the case of planar Hall effect (PHE) measurements as well. The nature of high field LMR along the x axis changes near 200 K. Dominant carrier concentration type, and metallic to semimetallic transition also occur near 200 K. These observations suggest two main conclusions: (i) The high field LMR in Mn$_3$Ge is driven by the metallic - semimetallic nature of the compound. (ii) Mn$_3$Ge compound goes through an electronic band topological transition near 200 K. Single crystal neutron diffraction does not show any change in the magnetic structure below 300 K. However, the in-plane lattice parameter (a) shows a maximum near 230 K. Therefore, it is possible that the change in electronic band structure near 200 K is driven by the a lattice parameter of the compound.

cond-mat.str-el

Crystal Symmetry of Stripe Ordered La1.88Sr0.12CuO4

We present a combined x-ray and neutron diffraction study of the stripe ordered superconductor \lscox{0.12}. The average crystal structure is consistent with the orthorhombic $Bmab$ space group as commonly reported in the literature. This structure however is not symmetry compatible with a second order phase transition into the stripe order phase, and, as we report here numerous Bragg peaks forbidden in the $Bmab$ space group are observed. We have studied and analysed these $Bmab$-forbidden Bragg reflections. Fitting of the diffraction intensities yields monoclinic lattice distortions that are symmetry consistent with charge stripe order.

cond-mat.supr-con

Compositional Studies of Metals with Complex Order by means of the Optical Floating-Zone Technique

The availability of large high-quality single crystals is an important prerequisite for many studies in solid-state research. The optical floating-zone technique is an elegant method to grow such crystals, offering potential to prepare samples that may be hardly accessible with other techniques. As elaborated in this report, examples include single crystals with intentional compositional gradients, deliberate off-stoichiometry, or complex metallurgy. For the cubic chiral magnets Mn$_{1-x}$Fe$_{x}$Si and Fe$_{1-x}$Co$_{x}$Si, we prepared single crystals in which the composition was varied during growth from $x = 0 - 0.15$ and from $x = 0.1 - 0.3$, respectively. Such samples allowed us to efficiently study the evolution of the magnetic properties as a function of composition, as demonstrated by means of neutron scattering. For the archetypical chiral magnet MnSi and the itinerant antiferromagnet CrB$_{2}$, we grew single crystals with varying initial manganese (0.99 to 1.04) and boron (1.95 to 2.1) content. Measurements of the low-temperature properties addressed the correlation between magnetic transition temperature and sample quality. Furthermore, we prepared single crystals of the diborides ErB$_{2}$, MnB$_{2}$, and VB$_{2}$. In addition to high vapor pressures, these materials suffer from peritectic formation, potential decomposition, and high melting temperature, respectively.

cond-mat.str-el

Structural disorder and magnetic correlations driven by oxygen doping in Nd2NiO4+d (d ~ 0.11)

We investigated the influence of oxygen over-stoichiometry on apical oxygen disorder and magnetic correlations in Nd2NiO4+d (d~0.11) in the temperature range of 2-300 K by means of synchrotron x-ray powder diffraction, neutron single crystal and powder diffraction studies, combined with macroscopic magnetic measurements. In the investigated temperature range, the compound crystalizes in a tetragonal commensurate structure with the P42/ncm space group with excess oxygen atoms occupy the 4b (3/4 1/4 1/4) interstitial sites, coordinated by four apical oxygen atoms. Large and anisotropic thermal displacement parameters are found for equatorial and apical oxygen atoms, which are strongly reduced on an absolute scale compared to the Nd2NiO4.23 phase. Maximum Entropy analysis of the neutron single crystal diffraction data uncovered anharmonic contributions to the displacement parameters of the apical oxygen atoms, toward the nearest vacant 4b interstitial site, related to the phonon assisted oxygen diffusion mechanism. Macroscopic magnetization measurements and neutron powder diffraction studies reveal long-range antiferromagnetic ordering of the Ni-sublattice at TN ~ 53 K with a weak ferromagnetic component along the c-axis, while the long-range magnetic ordering of the Nd-sublattice occurs below 10 K. Temperature dependent neutron diffraction patterns show the appearance of a commensurate magnetic order at TN with the propagation vector k = (100) and the emergence of an additional incommensurate phase below 30 K, while both phases coexist at 2 K. The commensurate magnetic structure is best described by the P42/nc`m` Shubnikov space group. Refined magnetic moments of the Ni and Nd-sites at 2 K are 1.144(76) muB and 1.632(52) muB respectively. A possible origin of the incommensurate phase is discussed and a tentative magnetic phase diagram is proposed.

cond-mat.mtrl-sci

Interdependent scaling of long-range oxygen and magnetic ordering in non-stoichiometric Nd${}_2$NiO${}_{4.10}$

Hole doping in Nd${}_{2}$NiO${}_{4.00}$ can be either achieved by substituting the trivalent Nd atoms by bivalent alkaline earth metals or by oxygen doping, yielding Nd${}_{2}$NiO${}_{4+\delta}$. In this study, we investigated the interplay between oxygen and spin ordering for a low oxygen doping concentration i.e. Nd${}_{2}$NiO${}_{4.10}$. Although the extra oxygen doping level remains rather modest with only one out of 20 possible interstitial tetrahedral lattice sites occupied, we observed by single crystal neutron diffraction the presence of a complex 3D modulated structure related to oxygen ordering already at ambient, the modulation vectors being $\pm$2/13\textit{\textbf{a*}}$\pm$3/13\textit{\textbf{b*}}, $\pm$3/13\textit{\textbf{b*}}$\pm$2/13\textit{\textbf{b*}} and $\pm$1/5\textit{\textbf{a*}}$\pm$1/2\textit{\textbf{c*}} and satellite reflections up to fourth order. Temperature dependent neutron diffraction studies indicate the coexistence of oxygen and magnetic ordering below T${}_{N}$ $\simeq$ 48 K, the wave vector of the Ni sublattice being \textbf{\textit{k}}=(100). In addition, magnetic satellite reflections adapt exactly the same modulation vectors as found for the oxygen ordering, evidencing a unique coexistence of 3D modulated ordering for spin and oxygen ordering in Nd${}_{2}$NiO${}_{4.10}$. Temperature dependent measurements of magnetic intensities suggest two magnetic phase transitions below 48 K and 20 K, indicating two distinct onsets of magnetic ordering for the Ni and Nd sublattice, respectively.

physics.app-ph

Magnetic structures, spin-flop transition and coupling of Eu and Mn magnetism in the Dirac semimetal EuMnBi$_2$

We report here a comprehensive study of the AFM structures of the Eu and Mn magnetic sublattices as well as the interplay between Eu and Mn magnetism in this compound by using both polarized and non-polarized single-crystal neutron diffraction. Magnetic susceptibility, specific heat capacity measurements and the temperature dependence of magnetic diffractions suggest that the AFM ordering temperature of the Eu and Mn moments is at 22 and 337 K, respectively. The magnetic moments of both Eu and Mn ions are oriented along the crystallographic $c$ axis, and the respective magnetic propagation vector is $\textbf{k}_{Eu} = (0,0,1)$ and $\textbf{k}_{Mn}=(0,0,0)$. With proper neutron absorption correction, the ordered moments are refined at 3 K as 7.7(1) $\mu_B$ and 4.1(1) $\mu_B$ for the Eu and Mn ions, respectively. In addition, a spin-flop (SF) phase transition of the Eu moments in an applied magnetic field along the $c$ axis was confirmed to take place at a critical field of B$_c$ $\sim$ 5.3 T. The evolution of the Eu magnetic moment direction as a function of the applied magnetic field in the SF phase was also determined. Clear kinks in both field and temperature dependence of the magnetic reflections ($\pm1$, 0, 1) of Mn were observed at the onset of the SF phase transition and the AFM order of the Eu moments, respectively. This unambiguously indicates the existence of a strong coupling between Eu and Mn magnetism. The interplay between two magnetic sublattices could bring new possibilities to tune Dirac fermions via changing magnetic structures by applied fields in this class of magnetic topological semimetals.

cond-mat.str-el

Magnetoelectric coupling in the mixed erythrosiderite [(NH$_4$)$_{1-x}$K$_x$]$_2$[FeCl$_5$(H$_2$O)]

We present a study of the dielectric, structural, and magnetic properties of the multiferroic or linear magnetoelectric substitution series [(NH$_4$)$_{1-x}$K$_x$]$_2$[FeCl$_5$(H$_2$O)]. Pyroelectric currents, magnetic susceptibilities, and thermodynamic properties were examined on large single crystals of the erythrosiderite compounds and detailed magnetic-field versus temperature phase diagrams are derived for three different substitution levels. With increasing potassium concentration the material is tuned from a multiferroic ($x \le 0.06$) to a linear magnetoelectric ($x \ge 0.15$) ground state. In contrast to the respective pure parent compounds with $x=0$ or 1, however, the ferroelectric or linear magnetoelectric polarization in none of the substituted samples is switchable by external electric fields, because these samples exhibit a significant electric polarization already above the magnetic ordering transition. The polarization arises at a higher-lying structural phase transition that is examined by THz spectroscopy and, on a deuterated pure single crystal, by comprehensive neutron-diffraction experiments. The structural phase transition is attributed to an ordering of NH$_4^+$ tetrahedra but does not break inversion symmetry in the pure material, while a finite K content causes pyroelectricity.

cond-mat.str-el

Ultra-high vacuum compatible induction-heated rod casting furnace

We report the design of a radio-frequency induction-heated rod casting furnace that permits the preparation of polycrystalline ingots of intermetallic compounds under ultra-high vacuum compatible conditions. The central part of the system is a bespoke water-cooled Hukin crucible supporting a casting mold. Depending on the choice of mold, typical rods have a diameter between 6 mm and 10 mm and a length up to 90 mm, suitable for single-crystal growth by means of float-zoning. The setup is all-metal sealed and may be baked out. We find that the resulting ultra-high vacuum represents an important precondition for processing compounds with high vapor pressures under a high-purity argon atmosphere up to 3 bar. Using the rod casting furnace, we succeeded to prepare large high-quality single crystals of two half-Heusler compounds, namely the itinerant antiferromagnet CuMnSb and the half-metallic ferromagnet NiMnSb.

physics.ins-det

Origin of forbidden reflections in multiferroic Ba$_2$CoGe$_2$O$_7$ by neutron diffraction: Symmetry lowering or Renninger effect?

For a symmetry consistent theoretical description of the multiferroic phase of Ba$_2$CoGe$_2$O$_7$ a precise knowledge of its crystal structure is a prerequisite. In our previous synchrotron X-ray diffraction experiment on multiferroic Ba$_2$CoGe$_2$O$_7$ at room temperature we found forbidden reflections that favour the tetragonal-to-orthorhombic symmetry lowering of the titled compound. Here, we report the results of room-temperature single-crystal diffraction studies with both hot and cold neutrons to differentiate between the real symmetry lowering and multiple diffraction (the Renninger effect). A comparison of the experimental multiple diffraction patterns with simulated ones rules out the symmetry lowering. Thus, the structural model based on the tetragonal space group $P\bar{4}2_1m$ was selected to describe the Ba$_2$CoGe$_2$O$_7$ symmetry at room temperature. The precise structural parameters from neutron diffraction at 300K are presented and compared with the previous X-ray diffraction results.

cond-mat.str-el

Low-temperature properties of single-crystal CrB$_{2}$

We report the low-temperature properties of $^{11}$B-enriched single-crystal CrB$_{2}$ as prepared from high-purity Cr and B powder by a solid-state reaction and optical float zoning. The electrical resistivity, $ρ_{\rm xx}$, Hall effect, $ρ_{\rm xy}$, and specific heat, $C$, are characteristic of an exchange-enhanced Fermi liquid ground state, which develops a slightly anisotropic spin gap $Δ\approx 220\,{\rm K}$ below $T_{\rm N}=88\,{\rm K}$. This observation is corroborated by the absence of a Curie dependence in the magnetization for $T\to0$ reported in the literature. Comparison of $C$ with $dρ_{\rm xx}/dT$, where we infer lattice contributions from measurements of VB$_2$, reveals strong antiferromagnetic spin fluctuations with a characteristic spin fluctuation temperature $T_{\rm sf}\approx 257\,{\rm K}$ in the paramagnetic state, followed by a pronounced second-order mean-field transition at $T_{\rm N}$, and unusual excitations around $\approx T_{\rm N}/2$. The pronounced anisotropy of $ρ_{\rm xx}$ above $T_{\rm N}$ is characteristic of an easy-plane anisotropy of the spin fluctuations consistent with the magnetization. The ratio of the Curie-Weiss to the N$\acute{\rm{e}}$el temperatures, $f=-Θ_{\rm CW}/T_{\rm N}\approx 8.5$, inferred from the magnetization, implies strong geometric frustration. All physical properties are remarkably invariant under applied magnetic fields up to $14\,\,{\rm T}$, the highest field studied. In contrast to earlier suggestions of local-moment magnetism our study identifies CrB$_{2}$ as a weak itinerant antiferromagnet par excellence with strong geometric frustration.

cond-mat.str-el

Low-temperature structural investigations of the frustrated quantum antiferromagnets Cs2CuCl(4-x)Br(x)

Powder X-ray diffraction (PXRD) and single-crystal neutron scattering were used to study in detail the structural properties of the Cs2CuCl(4-x)Br(x) series, good realizations of layered triangular antiferromagnets. Detailed temperature-dependent PXRD reveal a pronounced anisotropy of the thermal expansion for the three different crystal directions of the orthorhombic structure without any structural phase transition down to 20 K. Remarkably, the anisotropy of the thermal expansion varies for different $x$, leading to distinct changes of the geometry of the local Cu environment as a function of temperature and composition. The refinement of the atomic positions confirms that for x=1 and 2, the Br atoms occupy distinct halogen sites in the [CuX4]-tetrahedra (X = Cl, Br). The precise structure data are used to calculate the magnetic exchange couplings using density functional methods for x=0. We observe a pronounced temperature dependence of the calculated magnetic exchange couplings, reflected in the strong sensitivity of the magnetic exchange couplings on structural details. These calculations are in good agreement with the experimentally established values for Cs2CuCl4 if one takes the low-temperature structure data as a starting point.

cond-mat.str-el

Optical floating zone growth of high-quality Cu2MnAl single crystals

We report the growth of large single-crystals of Cu2MnAl, a ferromagnetic Heusler compound suitable for polarizing neutron monochromators, by means of optical floating zone under ultra-high vacuum compatible conditions. Unlike Bridgman or Czochralsky grown Cu2MnAl, our floating zone grown single-crystals show highly reproducible magnetic properties and an excellent crystal quality with a narrow and homogeneous mosaic spread as examined by neutron diffraction. An investigation of the polarizing properties in neutron scattering suggests a high polarization efficiency, limited by the relatively small sample dimensions studied. Our study identifies optical floating zone under ultra-high vacuum compatible conditions as a highly reproducible method to grow high-quality single-crystals of Cu2MnAl.

cond-mat.mtrl-sci