arXiv subjects

V. Caignaert

Publications and source records attributed to V. Caignaert.

At least 19 recordsLinked to original sources

arXiv2026

Microscopic investigation of spin dynamics in the single-chain magnet Sr4Mn2CoO9

One-dimensional single-chain magnets offer a unique platform for studying the interplay of crystal-field effects, exchange interactions, and lattice dynamics. Here, we investigate spin excitations in Sr4Mn2CoO9 using inelastic neutron scattering (INS) and theoretical modelling. INS reveals two low-energy magnetic excitations at 4 and 7 meV from Mn-Co-Mn spin chains, alongside higher-energy crystal-electric-field (CEF) excitations from two crystallographically inequivalent Co2+ sites. Interestingly, these spin excitations persist at room temperature, demonstrating dynamic magnetic correlations in the absence of long-range order. Furthermore, the crystal-field modelling, based on Stevens operator formalism, reproduces well the CEF spectra, establishing Ising-like Kramers ground-state doublets with strong uniaxial magnetic anisotropy for both Co2+ ions. In addition, the spin wave simulation using SpinW reproduces the spin excitation spectrum and reveals microscopic exchange interactions in two non-interacting Mn-Co-Mn spin chains. Finally, machine-learning lattice-dynamics calculations confirm the phonon spectrum and spin-phonon coupling. By projecting the exchange Hamiltonian onto CEF ground-state doublets, we estimate exchange-induced splittings matching the observed excitations. Thus, our results elucidate low-energy spin dynamics arising from combined crystal-field anisotropy and exchange interactions, with the persistent low-energy excitation providing a microscopic pathway for thermally activated spin relaxation. Furthermore, this work delivers a unified microscopic understanding of the interplay between crystal-field effects, magnetic exchange, and lattice dynamics in Sr4Mn2CoO9, advancing insights into spin dynamics in low-dimensional transition-metal oxides.

cond-mat.mtrl-sci↗

arXiv2023

Origin of spin-driven ferroelectricity and effect of external pressure on the complex magnetism of 6H-perovskite Ba3HoRu2O9

The compound Ba3HoRu2O9 magnetically orders at 50 K (TN1) followed by another complex magnetic ordering at 10.2 K (TN2). The 2nd magnetic phase transition was characterized by the co-existence of two competing magnetic ground states associated with two different magnetic wave vectors (K1=1/2 0 0 and K2=1/4 1/4 0). Here, we have discussed the origin of spin-driven ferroelectricity, which is not known yet. We demonstrate through time-of-flight Neutron diffraction and theoretical calculation that the non-collinear structure involving two different magnetic ions, Ru(4d) and Ho(4f), break the spatial inversion symmetry via inverse Dzyaloshinskii-Moriya (D-M) interaction through strong 4d-4f magnetic correlation, which shifts the oxygen atoms and results in non-zero polarization. Such an observation of inverse D-M interaction from two different magnetic ions which caused ferroelectricity is rarely observed. We have systematically studied the spin and dipolar dynamics, which exhibit intriguing behavior with shorter coherence lengths of 2nd magnetic phase associated with the k2-wave vector. The results manifest the development of finite-size magnetoelectric domains instead of true long-range ordering which justifies the experimentally obtained low value of ferroelectric polarization. The synchrotron XRD analysis predicts a non-centrosymmetric space group P-62c. Furthermore, we have investigated the effect of external pressure on this complex magnetism. The result reveals an enhancement of ordering temperature by the application of external pressure (1.6 K/GPa). The external pressure might favor stabilizing the magnetic ground state associated with 2nd magnetic phase. Our study shows an unconventional mechanism of spin-driven ferroelectricity.

cond-mat.str-el↗

arXiv2020

Cooperative Ru(4d)-Ho(4f) magnetic orderings and phase coexistence in the 6H-perovskite multiferroic Ba3HoRu2O9

We report cooperative magnetic orderings in a 6H-perovskite multiferroic system, Ba3HoRu2O9, via comprehensive neutron powder diffraction measurements. This system undergoes long-range antiferromagnetic ordering at TN1 ~ 50 K with a propagation wave vector of K1 = (0.5 0 0), a transition temperature much higher than the previously reported one at ~10 K (TN2). Both Ru and Ho-moments order simultaneously below TN1, followed by spin-reorientations at lower temperatures, demonstrating strong Ru(4d)-Ho(4f) magnetic correlation. Below TN1 another magnetic phase with a propagation wave vector K2 = (0.25 0.25 0) emerges and coexists with the one associated with K1, which is rarely observed and suggests complex magnetism due to phase competition in the magnetic ground state. We argue that the exchange-striction arising from the up-up-down-down spin structure associated with K2-wave vector below TN2 may be responsible for the small ferroelectric polarization reported previously in this compound.

cond-mat.str-el↗

arXiv2013

Gigantic magnetic field polarization and magnetoelectric coupling in a ferrimagnetic oxide CaBaCo4O7

The single crystal study of CaBaCo4O7, a non collinear ferrimagnet (TC=64K), with a polar orthorhombic space group (Pbn21) between 4 K and 293 K, shows the appearance below TC of a large electric polarization along its c axis, reaching 17mC.m-2 at 10K. At 62.5K, a magnetic field driven giant variation of polarization, P(9T)-P(0T)=8mC.m-2, is observed. Moreover, the present magnetoelectric measurements, are fully consistent with the m'm2' magnetic point group, strongly supporting that this oxide is also ferrotoroidic. This ferrimagnetic oxide, which belongs to the '114' structural family, opens an avenue for the search of new magnetoelectrics.

cond-mat.mtrl-sci↗

arXiv2012

Geometric and disorder -- type magnetic frustration in ferrimagnetic "114" Ferrites: Role of diamagnetic Li+ and Zn2+ cation substitution

The comparative study of the substitution of zinc and lithium for iron in the "114" ferrites, YBaFe4O7 and CaBaFe4O7, shows that these diamagnetic cations play a major role in tuning the competition between ferrimagnetism and magnetic frustration in these oxides. The substitution of Li or Zn for Fe in the cubic phase YBaFe4O7 leads to a structural transition to a hexagonal phase YBaFe4-xMxO7, for M = Li (0.30 < x < 0.75) and for M = Zn (0.40 < x < 1.50). It is seen that for low doping values i.e. x = 0.30 (for Li) and x = 0.40 (for Zn), these diamagnetic cations induce a strong ferrimagnetic component in the samples, in contrast to the spin glass behaviour of the cubic phase. In all the hexagonal phases, YBaFe4-xMxO7 and CaBaFe4-xMxO7 with M = Li and Zn, it is seen that in the low doping regime (x ~ 0.3 to 0.5), the competition between ferrimagnetism and 2 D magnetic frustration is dominated by the average valency of iron. In contrast, in the high doping regime (x ~ 1.5), the emergence of a spin glass is controlled by the high degree of cationic disorder, irrespective of the iron valency.

cond-mat.mtrl-sci↗

arXiv2012

Gallium Substituted "114" YBaFe4O7: From a ferrimagnetic cluster glass to a cationic disordered spin glass

The study of the ferrites YBaFe4-xGaxO7 shows that the substitution of Ga for Fe in YBaFe4O7 stabilizes the hexagonal symmetry for 0.40 < x < 0.70, at the expense of the cubic one. Using combined measurements of a. c. and d. c. magnetization, we establish that Ga substitution for Fe in YBaFe4O7 leads to an evolution from a geometrically frustrated spin glass (for x = 0) to a cationic disorder induced spin glass (x = 0.70). We also find an intermediate narrow range of doping where the samples are clearly phase separated having small ferrimagnetic clusters embedded in a spin glass matrix. The origin of the ferrimagnetic clusters lies in the change in symmetry of the samples from cubic to hexagonal (and a consequent lifting of the geometrical frustration) as a result of Ga doping. We also show the presence of exchange bias and domain wall pinning in these samples. The cause of both these effects can be traced back to the inherent phase separation present in the samples.

cond-mat.mtrl-sci↗

arXiv2012

Ordering process and ferroelectricity in a spinel derived from FeV2O4

The spinel FeV2O4 is known to exhibit peculiar physical properties, which is generally ascribed to the unusual presence of two cations showing a pronounced interplay between spin, orbital and lattice degrees of freedom (Fe2+ and V3+ on the tetrahedral and octahedral sites, respectively). The present work reports on an experimental re-investigation of this material based on a broad combination of techniques, including x-ray diffraction, energy dispersive and Mössbauer spectroscopies, as well as magnetization, heat capacity, dielectric and polarization measurements. Special attention was firstly paid to establish the exact cationic composition of the investigated samples, which was found to be Fe1.18V1.82O4. All the physical properties were found to point out a complex ordering process with a structural transition at TS = 138 K, followed by two successive magnetostructural transitions at TN1 = 111 K and TN2 = 56 K. This latter transition marking the appearance of electric polarization, magnetization data were analysed in details to discuss the nature of the magnetic state at T< TN2. An overall interpretation of the sequence of transitions was proposed, taking into account two spin couplings, as well as the Jahn-Teller effects and the mechanism of spin-orbit stabilization. Finally, the origin of ferroelectricity in Fe1.18V1.82O4 is discussed on the basis of recent models.

cond-mat.mtrl-sci↗

arXiv2011

Oxygen hyperstoichiometric hexagonal ferrite CaBaFe4O7+δ(δ\approx 0.14) : coexistence of ferrimagnetism and spin glass behavior

An oxygen hyperstoichiometric ferrite CaBaFe4O7+δ(δ\approx 0.14) has been synthesized using "soft" reduction of CaBaFe4O8. Like the oxygen stoichiometric ferrimagnet CaBaFe4O7, this oxide also keeps the hexagonal symmetry (space group: P63mc), and exhibits the same high Curie temperature of 270 K. However, the introduction of extra oxygen into the system weakens the ferrimagnetic interaction significantly at the cost of increased magnetic frustration at low temperature. Moreover, this canonical spin glass (Tg ~ 166 K) exhibits an intriguing cross-over from de Almeida-Thouless type to Gabay-Toulouse type critical line in the field temperature plane above a certain field strength, which can be identified as the anisotropy field. Domain wall pinning is also observed below 110 K. These results are interpreted on the basis of cationic disordering on the iron sites.

cond-mat.str-el↗

arXiv2010

Hysteretic "Magnetic-Transport-Structural" Transition in "114" Cobaltites: Size Mismatch Effect

The triple "magnetic-transport-structural" transition versus temperature in three series of "114" cobaltites - Y1-xYbxBaCo4O7, Y1-xCaxBaCo4O7 and Yb1-xCaxBaCo4O7 - has been studied using magnetic, transport and differential scanning calorimetric measurements. The effect of the size mismatch σ2, due to cationic disordering at the Ln sites upon such a transition is shown for the first time in a triangular lattice. We show that increasing has an effect of increasing TS dramatically, while the size mismatch σ2 at the Ln sites decreases TS substantially. Moreover, the cationic mismatch at the Ln sites modifies the nature of the hysteretic transition by turning the sharp first order transition seen in the undoped samples into an intermix of first and second order transitions. These results are discussed on the basis of the particular nature of the high temperature form which exhibits a hexagonal close packed structure (space group: P63mc) with respect to the low temperature orthorhombic form (space group: Pbn21), the latter corresponding to a distortion of the former due to a puckering of the kagomé layers.

cond-mat.mtrl-sci↗

arXiv2010

Magnetic and Electronic properties of Eu0.9Ca0.1BaCo2O5.5+? with the disparity of Oxygen Stoichiometry

The effect of oxygen content on the magnetic and transport properties of the ferromagnetic Eu0.9Ca0.1BaCo2O5.5+δ has been carried out. Unlike the increase in TC with calcium content, paradoxally the TC value decreases with the increase in oxygen (Co4+) content as observed in the undoped phase. This result unveils the hidden generic magnetic feature of the LnBaCo2O5.5 system in the calcium doped phase. This behaviour supports strongly the appearance of Co3+ disproportion action into Co4+ and Co2+ and the magnetic phase separation scenario of ferromagnetic domains embedded in an antiferromagnetic matrix. All the samples covering a wide range of oxygen content, exhibit a p-type conductivity.

cond-mat.mtrl-sci↗

arXiv2010

Competition between Ferrimagnetism and Magnetic Frustration in Zinc Substituted YBaFe4O7

The substitution of zinc for iron in YBaFe4O7 has allowed the oxide series YBaFe4-xZnxO7, with 0.40 < x < 1.50, belonging to the "114" structural family to be synthesized. These oxides crystallize in the hexagonal symmetry (P63mc), as opposed to the cubic symmetry (F-43m) of YBaFe4O7. Importantly, the d.c. magnetization shows that the zinc substitution induces ferrimagnetism, in contrast to the spin glass behaviour of YBaFe4O7. Moreover, a.c. susceptibility measurements demonstrate that concomitantly these oxides exhibit a spin glass or a cluster glass behaviour, which increases at the expense of ferrimagnetism, as the zinc content is increased. This competition between ferrimagnetism and magnetic frustration is interpreted in terms of lifting of the geometric frustration, inducing the magnetic ordering, and of cationic disordering, which favours the glassy state.

cond-mat.mtrl-sci↗

arXiv2010

Magnetic and Electrical Properties of Ordered 112-type Perovskite LnBaCoMnO5+δ(Ln = Nd, Eu)

Investigation of the oxygen-deficient 112-type ordered oxides of the type LnBaCoMnO5+δ(Ln = Nd, Eu) evidences certain unusual magnetic behavior at low temperatures, compared to the LnBaCo2O5+δcobaltites. One observes that the substitution of manganese for cobalt suppresses the ferromagnetic state and induces strong antiferromagnetic interactions. Importantly, NdBaCoMnO5.9 depicts a clear paramagnetic to antiferromagnetic type transition around 220 K, whereas for EuBaCoMnO5.7 one observes an unusual magnetic behavior below 177 K which consists of ferromagnetic regions embedded in an antiferromagnetic matrix. The existence of two sorts of crystallographic sites for Co/Mn and their mixed valence states favor the ferromagnetic interaction whereas antiferromagnetism originates from the Co3+-O-Co3+ and Mn4+-O-Mn4+ interactions. Unlike the parent compounds, the present Mn-substituted phases do not exhibit prominent magnetoresistance effects in the temperature range 75-400K.

cond-mat.mtrl-sci↗

arXiv2010

Magnetic Structure of CaBaCo4O7: Lifting of Geometrical Frustration towards Ferrimagnetism

CaBaCo4O7 represents a new class of ferrimagnets whose structure is built up of CoO4 tetrahedra only, similarly to other members LnBaCo4O7 of the 114 series, forming an alternate stacking of kagome and triangular layers. Neutron powder diffraction reveals, that this compound exhibits the largest distortion within the 114 series, characterized by a strong buckling of the kagome layers. Differently from all other members it shows charge ordering, with Co2+ sitting on two sites (Co2, Co3) and mixed valent cobalt Co3+/Co2+L sitting on two other sites (Co1, Co4). The unique ferrimagnetic structure of this cobaltite at 4 K can be described as the assemblage of ferrimagnetic triple chains (Co1 Co2 Co3) running perpendicular to the kagome layers, ferromagnetically coupled within the layers, and antiferromagnetically coupled with a fourth cobalt species Co4. The lifting of the geometrical frustration towards ferrimagnetism, which appears in spite of the triangular topology of the cobalt lattice, is explained by the very large structural distortion, charge ordering phenomena and large cobalt valence compared to other LnBaCo4O7 oxides.

cond-mat.mtrl-sci↗

arXiv2008

Magneto-transport and Magneto-dielectric effect in Bi-based Perovskite Manganites

The effect of cobalt and nickel substitutions for manganese on the physical properties of the perovskite manganite La1.2Bi0.8Mn2-x(Ni/Co)xO6+d, with x = 0.0-0.8, has been investigated. It is observed that the ferromagnetism is enhanced, TC being increased from 103 K for the parent compound (x = 0.0) to 178 K for Ni-phase, and to 181 K for the Co-phase (x = 0.8). Moreover, the systems remain insulating and depict relatively large values of magnetoresistance effect at low temperatures (up to 67 % at 90K and 70 kOe, for x = 0.0 phase). These phenomena are interpreted by means of electronic phase separation, where the ferromagnetic Mn4+/Ni2+ and Mn4+/Co2+ interactions reinforce the Mn3+/Mn4+ interactions by super-exchange interaction. The dielectric measurements below the magnetic transition temperatures exhibit weak magneto-dielectric effect of around 0.25% at 80K, which may be due to spin-lattice interaction.

cond-mat.mtrl-sci↗

arXiv2008

A Multiferroic Ceramic with Perovskite Structure: La0.5Bi0.5Mn0.5Fe0.5O3.09

ABO3 perovskite multiferroic La0.5Bi0.5Mn0.5Fe0.5O3.09 where the B-site cations is responsible for the magnetic properties and the A-site cation with lone pair electron is responsible for the ferroelectric properties was synthesized at normal conditions. This oxide exhibits a ferromagnetic transition around 240 K with a well defined hysteresis loop, and a significant reversible remnant polarization below 67K similar to ferroelectric behavior. The magnetic interaction is interpreted by the ferromagnetic Fe3+-O-Mn3+ and antiferromagnetic Fe3+(Mn3+)-O-Fe3+(Mn3+) interactions competed each other, whereas the ferroelectricity is predominantly due to the polar nature introduced by the 6s2 lone pair of Bi3+ cations

cond-mat.mtrl-sci↗

arXiv2008

Electron transport and thermoelectric properties of layered perovskite LaBaCo2O5.5

We have investigated the systematic transport properties of the layered 112-type cobaltite LaBaCo2O5.5 by means of electrical resistivity, magnetoresistance, electroresistance and thermoelectric measurements in various conditions. In order to understand the complex conduction mechanism of LaBaCo2O5.5, the transport data have been analyzed using different theoretical models. The system shows semiconductor-semiconductor like transition (TSC) around 326K, corresponding to ferromagnetic transition and in the low temperature region resistivity data follows the Motts variable range hopping model. Interestingly, near and below the room temperature this compound depicts significant change in electro- and magnetoresistance behavior, the latter one is noteworthy near the magnetic phase boundary. The temperature dependence of thermopower, S(T), exhibits p-type polaronic conductivity in the temperature range of 60-320K and reaches a maximum value of 303 uV/K (at 120K). In the low temperature AFM region, the unusual S(T) behavior, generally observed for the cobaltite series LnBaCo2O5.5 (Ln = Rare Earth), is explained by the electron magnon scattering mechanism as previously described for perovskite manganites.

cond-mat.mtrl-sci↗

arXiv2008

Enhancement of ferromagnetism by Co and Ni substitution in the perovskite LaBiMn2O6+d

The substitution of cobalt and nickel for manganese in the perovskite manganate LaBiMn2O6+d; has been realized, leading to the perovskites LaBiMn2-x(M)xO6+d, with M = Co, Ni and x =0-2/3. In contrast to the literature those phases are found to be orthorhombic with Pnma symmetry. More importantly, it is shown that ferromagnetism is enhanced, TC being increased from 80 K for the parent compound (x = 0) to 97 K for Ni-phase, and to 130 K for the Co-phase. Moreover, a strong competition between ferromagnetism and a glassy-ferromagnetic state in the case of nickel or a spin-glass behaviour in the case of cobalt is observed. These phenomena are interpreted in the frame of a phase separation scenario, where the ferromagnetic Mn4+/Ni2+ and Mn4+/Co2+ interactions reinforce the Mn3+/Mn4+ interactions. These compounds are found to be insulating with a relatively large positive value of thermoelectric power.

cond-mat.mtrl-sci↗

arXiv2007

Transport and magnetic properties in YBaCo2O5.45: Focus on the high-temperature transition

The electronic transport properties and the magnetic susceptibility were measured in detail in $YBaCo_2O_{5.45}$. Close to the so-called metal-insulator transition, strong effects of resistance relaxation, a clear thermal hysteresis and a sudden increase of the resistance noise are observed. This is likely due to the first order character of the transition and to the underlying phases coexistence. Despite these out of equilibrium features, a positive and linear magneto-resistance is also observed, possibly linked to the heterogeneity of the state. From a magnetic point of view, the paramagnetic to ordered magnetic state transition is observed using non linear susceptibilty. This transition shows the characteristics of a continuous transition, and time dependent effects can be linked with the dynamics of magnetic domains in presence of disorder. Thus, when focusing on the order of the transitions, the electronic one and the magnetic one can not be directly associated.

cond-mat.mtrl-sci↗