arXiv subjects

O. Fabelo

Publications and source records attributed to O. Fabelo.

14 recordsLinked to original sources

arXiv2026

Water, vacancies, and competing exchange interactions in Prussian blue analogues: a neutron diffraction study of field and dehydration-driven magnetic transitions

We report a neutron diffraction study of the structural and magnetic properties of a family of ferro- and ferrimagnetic Prussian blue analogues (PBAs), $A_4$[Fe(CN)$_6$]$_{2.7}$ ($A$ = Co, Mn, Ni), Rb$_2$Ni$_4$[Fe(CN)$_6$]$_{3.3}$, and Mn$_4$[Cr(CN)$_6$]$_{2.7}$, as a function of temperature (2--450~K) and applied magnetic field. All bimetallic compounds of the Fm$\overline{3}$m family exhibit a broad diffuse feature at low scattering angle, which we identify, through comparison with the cation-stabilized Rb$_2$NiFe framework, as an intrinsic signature of correlated vacancies and their associated interstitial water. High-temperature diffraction reveals a continuous crossover from positive to negative thermal expansion in CoFe and MnFe upon dehydration, while NiFe remains structurally robust up to 450~K. At low temperature, all compounds order in a collinear ferrimagnetic state with propagation vector $\mathbf{k}=(0,0,0)$, except MnFe, which adopts a partially frustrated magnetic structure with $\mathbf{k}=(1,0,0)$. A moderate magnetic field of $B_c = 1.3$~T drives a spin reorientation in MnFe toward the collinear $\mathbf{k}=(0,0,0)$ ferrimagnetic state common to the other compounds; the same transition is independently induced by dehydration. A minimal Heisenberg model shows that this transition results from a near-compensation between antiferromagnetic Mn--Fe coupling and a geometrically frustrated antiferromagnetic Mn--Mn interaction on the face-centered-cubic Mn sublattice, placing MnFe in the vicinity of a magnetic compensation point. These results resolve a longstanding ambiguity in the interpretation of the Fe $K$-edge XMCD response of MnFe-based PBAs, and establish water content as a key parameter controlling both the structural and magnetic stability of this family of materials, with direct relevance to their use as battery electrodes.

cond-mat.mtrl-sci↗

arXiv2026

Thermal expansion of FeWO$_4$ (Ferberite) and FeWO$_4$:Fe$_2$WO$_6$ (7:1): a comparative X-ray and neutron diffraction study

The thermal expansion of natural FeWO$_4$ (ferberite) and synthetic FeWO$_4$:Fe$_2$WO$_6$ (7:1) was investigated over the 2-1123 K temperature range combining single-crystal and powder X-ray diffraction together with neutron powder diffraction. High-precision lattice parameters were obtained for both samples. The temperature dependence of the unit-cell volume was analysed using physically based thermodynamic models, including the Kroll and Berman approaches as implemented in EoSFit7. All datasets are well reproduced within their respective temperature intervals. However, significant differences are observed between the behavior of ferberite and FeWO$_4$:Fe$_2$WO$_6$, which has a \~40% smaller thermal expansion coefficient and a reduced reference volume. Possible origins, including microstructural and phase-coexistence effects, are discussed. The results provide a comprehensive description of the thermal expansion behavior of FeWO$_4$ across a wide temperature range.

cond-mat.mtrl-sci↗

arXiv2026

Structural studies on $A_2$ReCl$_6$ ($A$=K, Rb, Cs): absence of Jahn-Teller distortion

K$_2$ReCl$_6$ belongs to the antifluorite family and exhibits a sequence of structural transitions above the onset of magnetic order at $T_N$ = 12 K. Because of its 5d3 electronic configuration in an octahedral coordination, the ground state is a pure spin state without orbital degeneracy within the LS coupling scheme, but it can become Jahn-Teller active in the strong spin-orbit coupling limit described by the $jj$ coupling [S. Streltsov and D. I. Khomskii, Phys. Rev. X 10, 031043 (2020)]. While the structural transitions in K$_2$ReCl$_6$ are understood in terms of octahedral rotation and tilting, the possible impact of a Jahn-Teller distortion remains an open issue. We report on comprehensive crystalstructure studies by means of powder neutron and single-crystal x-ray diffraction on K$_2$ReCl$_6$ and on K$_2$SnCl$_6$. The latter material is used as a reference, because it exhibits the same sequence of structural transitions as K$_2$ReCl$_6$, but possesses a filled 4d shell ruling out a Jahn-Teller distortion. While the ReCl$_6$ octahedron in K$_2$ReCl$_6$ presents sizable distortions at intermediate temperatures, there is no such distortion persisting to low temperatures excluding a sizable Jahn-Teller effect. Studies on polycrystalline samples of Rb$_2$ReCl$_6$ and Cs$_2$ReCl$_6$, in which the structural transitions are suppressed due to the larger alkaline ionic radius, also do not find any indications for a Jahn-Teller distortion.

cond-mat.str-el↗

arXiv2025

New insight on the phase diagram of the superconducting iron spin ladder BaFe$_2$S$_3$

BaFe$_2$S$_3$ and BaFe$_2$Se$_3$ are the only two quasi-one-dimensional iron-based compounds that become superconductors under pressure. Interestingly, these two compounds exhibit different symmetries and properties. While more detailed and recent studies on BaFe$_2$Se$_3$ using single crystals have advanced the filed towards a more universal description of this family, such a study is still lacking for the compound BaFe$_2$S$_3$. Here, we present a detailed study of the crystalline and magnetic structure performed on single crystals using X-ray and neutron diffraction. We demonstrate a polar structure at room temperature within the $Cm2m$ space group, followed by a structural transition at 130 K to the polar $Pb2_1m$ space group. This space group remains unchanged across the magnetic transition at $T_N =95$ K, revealing multiferroic characteristics with a weak magnetoelastic coupling. The determined magnetic structure is monoclinic ($P_am$), with non-collinear magnetic moments, displaying a significant angle of 18$^\circ$ relative to the $a$-axis in the $(a, c)$ plane. This reexamination of the temperature-dependent properties of BaFe$_2$S$_3$ provides new insights into the physics of this system from multiple key perspectives.

cond-mat.str-el↗

arXiv2025

Duality of Wave Modulation and Nanotwinning in Ni-Mn-Ga Martensite via Long-Period Commensurate States

Structural modulation is a key ingredient behind the extraordinary (magneto)elastic response of Ni-Mn-Ga martensite, yet its link to fine microstructural features and twin-boundary supermobility remains unresolved. Here we analyse martensitic single crystals of Ni50.0Mn27.7Ga22.3 and Ni50.0Mn28.1Ga21.9. Neutron and X-ray diffraction reveal an anharmonic five-layer structural modulation, evidenced by high-order satellite reflections, that evolves from commensurate (q = 2/5) to incommensurate (2/5 < q < 5/12) upon cooling. Interpreting the refined modulation displacements as a basal-plane stacking sequence links the wave description to the microstructural evolution on cooling. In this view, evolving incommensurability produces periodic nanodomains interpreted as emerging a/b-nanotwins with a characteristic size of approximately 20 nm at approximately 290 K. With further cooling, the modulation can lock into long-period commensurate (LP-C) states, such as 34O (q = 7/17), 24O (q = 5/12), and 14O (q = 3/7), whose orthorhombic unit cells can be viewed as a/b-nanotwins. Ab initio calculations show that LP-C structures are energetically competitive with the initial commensurate state, supporting a shallow martensitic energy landscape. We propose a physical picture in which the martensitic transformation selects a commensurate state with q = 2/5 in the Mn-rich compositions studied here, while subsequent cooling drives relaxation within the martensitic landscape toward LP-C states, particularly 24O in the present alloys. The resulting structure is neither purely wave-like nor purely nanotwinned; rather, it reflects coupling between a coherent modulation wave and local accommodation via NM-like tetragonal distortions, nanotwinning, and LP-C lock-ins, providing a structural basis for the wave-nanotwin duality in Ni-Mn-Ga martensite.

cond-mat.mtrl-sci↗

arXiv2024

Resolving the local distortions of Ising-like moments in magnetoelectric Ho-doped langasite

The magnetic properties of Ho-doped langasites (La:Ho)$_3$Ga$_5$SiO$_{14}$ are dominated by the Ising-like magnetic moments of the Ho$^{3+}$ ions. In their saturated regime, the induced magnetic state breaks both time and space inversion symmetries, leading to a novel linear magnetoelectric effect. However, due to distortions induced by a shared Ga/Si occupancy of the 2d sites, resolving the microscopic nature of the magnetic configuration remains a difficult task. Here we combine polarized neutron diffraction and angular dependent magnetization experiments to determine the local distortions of the Ho$^{3+}$ magnetic moments in doped langasites (La$_{1-x}$Ho$_x$)$_3$Ga$_5$SiO$_{14}$ with $x \approx 0.015$ and $x \approx 0.045$. We propose a model for a field-induced magnetic configuration with arbitrary orientations of the local Ising axis of Ho$^{3+}$ in distorted positions. The operations of broken local $C_2$ symmetry and rotations around the trigonal $C_3$ axis connect different sites, restoring the global P321 symmetry of the crystal and simplifying the description of the magnetic properties. The superposition of two distorted Ho$^{3+}$ positions connected by $C_2$ symmetry determines the local magnetic susceptibility tensor, which no longer appears Ising-like at low fields.

cond-mat.mtrl-sci↗

arXiv2024

Anharmonic Incommensurate Structure Modulation in Ni-Mn-Ga Martensite Exhibiting Highly Mobile Twin Boundaries

Understanding the crystal structure of magnetic shape memory alloys is crucial for insights into their unique properties, such as the high mobility of twin boundaries and magnetic field functionality. The complex neutron diffraction patterns betweeen 10-300 K indicate an incommensurate and simultaneously anharmonic modulation function (AMF) in Ni50.0Mn27.7Ga22.3 10M martensite. Our identification of the dominant Fourier components in the AMF allowed for a comparison between calculated diffraction patterns and experiments. The AMF explains the appearance of peculiar small-intensity diffraction peaks when nearly commensurate AMF at 300 K turns to incommensurate AMF upon cooling. Further analysis reveals that divergent periodicity between the incommensurate modulation and the lattice leads to the formation of additional nanodomains. Interpreting the modulation displacements within the nanodomains in the terms of the (2-3)2 stacking sequence of basal (110) planes enables to understand that these nanodomains are emerging a/b nanotwins. The nanotwinning interlinked with incommensurate modulation also explains the transition from the tetragonal to the orthorhombic symmetry upon cooling. We identify specific low-temperature orthorhombic structures, like 34O, 24O, 14O, which are significant as their unit cell simultaneously represents an a/b-nanotwin. The ab initio calculations confirm the stability and low and comparable energy of all found nanotwinned structures. Based on the presumed stability of the nanotwinned state and literature comparisons, we propose that the low temperature state of the martensite nominally marked as five-layered modulated, 5M or 10M, is one of the specific a/b-nanotwinned configurations such as 34O, 24O, 14O. The exact choice depends on the composition, but 14O resulting from q = 3/7 is the ultimate limit with a corresponding smallest twin domain size of 3.5 nm.

cond-mat.mtrl-sci↗

arXiv2022

Strain control of a bandwidth-driven spin reorientation in Ca$_{3}$Ru$_{2}$O$_{7}$

The layered-ruthenate family of materials possess an intricate interplay of structural, electronic and magnetic degrees of freedom that yields a plethora of delicately balanced ground states. This is exemplified by Ca$_{3}$Ru$_{2}$O$_{7}$, which hosts a coupled transition in which the lattice parameters jump, the Fermi surface partially gaps and the spins undergo a $90^{\circ}$ in-plane reorientation. Here, we show how the transition is driven by a lattice strain that tunes the electronic bandwidth. We apply uniaxial stress to single crystals of Ca$_{3}$Ru$_{2}$O$_{7}$, using neutron and resonant x-ray scattering to simultaneously probe the structural and magnetic responses. These measurements demonstrate that the transition can be driven by externally induced strain, stimulating the development of a theoretical model in which an internal strain is generated self-consistently to lower the electronic energy. We understand the strain to act by modifying tilts and rotations of the RuO$_{6}$ octahedra, which directly influences the nearest-neighbour hopping. Our results offer a blueprint for uncovering the driving force behind coupled phase transitions, as well as a route to controlling them.

cond-mat.str-el↗

arXiv2022

Neutron diffraction in MnSb2O6: Magnetic and structural domains in a helicoidal polar magnet with coupled chiralities

MnSb$_{2}$O$_{6}$ is based on the structural chiral $P$321 space group #150 where the magnetic Mn$^{2+}$ moments ($S=5/2$, $L\approx 0$) order antiferromagnetically at $T_\mathrm{N}=12$ K. Unlike the related iron based langasite (Ba$_3$NbFe$_3$Si$_2$O$_{14}$) where the low temperature magnetism is based on a proper helix characterized by a time-even pseudoscalar `magnetic' chirality, the Mn$^{2+}$ ions in MnSb$_{2}$O$_{6}$ order with a cycloidal structure at low temperatures, described instead by a time-even vector `magnetic' polarity. A tilted cycloidal structure has been found [M. Kinoshita et al. Phys. Rev. Lett. 117, 047201 (2016)] to facilitate ferroelectric switching under an applied magnetic field. In this work, we apply polarized and unpolarized neutron diffraction analyzing the magnetic and nuclear structures in MnSb$_{2}$O$_{6}$ with the aim of understanding this magnetoelectric coupling. We find no evidence for a helicoidal magnetic structure with one of the spin envelope axes tilted away from the cycloidal $c$-axis. However, on application of a magnetic field $\parallel$ $\vec{c}$ the spin rotation plane can be tilted, giving rise to a cycloid-helix admixture that evolves towards a distorted helix (zero cycloidal component) for fields great than $\approx$ 2 T. We propose a mechanism for the previously reported ferroelectric switching based on coupled structural and magnetic chiralities requiring only an imbalance of structural chiral domains.

cond-mat.str-el↗

arXiv2021

Tuning the tilting of the spiral plane by Mn doping in YBaCuFeO5 multiferroic

The layered perovskite YBaCuFeO5 (YBCFO) is considered one of the best candidates to high-temperature chiral multiferroics with strong magnetoelectric coupling. In RBaCuFeO5 perovskites (R: rare-earth or Y) A-site cations are fully ordered whereas their magnetic properties strongly depend on the preparation process. They exhibit partial cationic disorder at the B-site that generates a magnetic spiral stabilized through directionally assisted long range coupling between canted locally frustrated spins. Moreover the orientation of its magnetic spiral can be critical for the magnetoelectric response of this chiral magnetic oxide. We have synthesized and studied YBaCuFe1-xMnxO5 samples doped with Mn, with the aim of increasing spin-orbit coupling effects, and found that the overall Fe/Cu cation disorder at the B-sites can be increased by doping without changing the sample preparation process. In YBaCuFe1-xMnxO5 samples prepared under the same conditions, the T-x magnetic phase diagram have been constructed in the range 10K-500K combining magnetometry, X-ray and neutron powder diffraction measurements. The tilting angles of the spins in the collinear, θcol , and spiral phases, θspiral, barely vary with temperature. In the collinear phase θcol is also independent of the Mn content. In contrast, the presence of Mn produces a progressive reorientation of the plane of the magnetic helix in the incommensurate phase, capable to transform the helicoidal spin ordering into a cycloidal one, which may critically determine the ferroelectric and magnetoelectric behavior in these compounds. Some of the observations are of interest for engineering and developing this family of potential high-temperature multiferroics.

cond-mat.mtrl-sci↗

arXiv2020

High temperature tetragonal crystal structure of UPt$_2$Si$_2$

High temperature crystal structure of UPt$_2$Si$_2$ determined using single-crystal neutron diffraction at 400 K is reported. It is found that the crystal structure remains of the primitive tetragonal CaBe$_2$Ge$_2$ type with the space group P4/$n m m. Anisotropic displacement factors of the Pt atoms at the 2a (3/4 1/4 0) and Si atoms at the 2c (1/4 1/4 z) Wyckoff sites are found to be anomalously large.

cond-mat.str-el↗

arXiv2019

Natural ferroelectric order near ambient temperature in HoFeO3: A member of RFeO3 orthoferrites

Current scenario in multiferroics demands a breakthrough discovery of promising materials after BiFeO3. Recently, the controversial discovery of room temperature ferroelectricity (FE) in SmFeO3 [PRL 107, 117201 (2011); 113, 217203 (2014)] inspires the investigation of HoFeO3. Here, we report a natural ferroelectric order below 210 K (TFE) along c-axis with reasonably large polarization and low-field strong magnetoelectric coupling. Synchrotron and neutron diffraction results confirm that a shift of O atoms along c-axis of polar Pbn21 structure causes FE in HoFeO3. The exchange striction mechanism is suggested to elucidate the ferroelectric order. The results create a renewed attention for searching promising candidates with a natural ferroelectric order and higher TFE in the rest of the RFeO3 series.

cond-mat.mtrl-sci↗

arXiv2019

A Unique Crystal Structure of Ca$_2$RuO$_4$ in the Current Stabilized Semi-Metallic State

The electric-current stabilized semi-metallic state in the quasi-two-dimensional Mott insulator Ca$_2$RuO$_4$ exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and X-ray diffraction, we show that this non-equilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high pressure and epitaxial strain, which in turn leads to a distinct electronic band structure. Dynamical mean field theory calculations based on the crystallographically refined atomic coordinates and realistic Coulomb repulsion parameters indicate a semi-metallic state with partially gapped Fermi surface. Our neutron diffraction data show that the non-equilibrium behavior is homogeneous, with antiferromagnetic long-range order completely suppressed. These results provide a new basis for theoretical work on the origin of the unusual non-equilibrium diamagnetism in Ca$_2$RuO$_4$.

cond-mat.str-el↗

arXiv2017

Magnetic and dielectric order in the kagome-like francisite Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl

We report a single-crystal neutron diffraction and inelastic neutron scattering study on the spin 1/2 cuprate Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl, complemented by dielectric and electric polarization measurements. The study clarifies a number of open issues concerning this complex material, whose frustrated interactions on a kagome-like lattice, combined with Dzyaloshinskii-Moriya interactions, are expected to stabilize an exotic canted antiferromagnetic order. In particular, we determine the nature of the structural transition occurring at 115 K, the magnetic structure below 25 K resolved in the updated space group, and the microscopic ingredients at the origin of this magnetic arrangement. This was achieved by an analysis of the measured gapped spin waves, which signifies the need of an unexpected and significant anisotropic exchange beyond the proposed Dzyaloshinskii-Moriya interactions. Finally, we discuss the mutliferroic properties of this material with respect to the space group symmetries.

cond-mat.mtrl-sci↗