arXiv subjects

V. Hardy

Publications and source records attributed to V. Hardy.

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↗

arXiv2018

Fermi- to non-Fermi-liquid crossover and Kondo transition in two-dimensional Cu$_{2/3}$V$_{1/3}$V$_2$S$_4$

By means of a specific heat ($C$) and electrical resistivity ($\varrho$) study, we give evidence of a pronounced Fermi liquid (FL) behavior with sizable mass renormalization, $m^{\ast}/m = 30$, up to unusually high temperatures $\sim$70 K in the layered system Cu$_{2/3}$V$_{1/3}$V$_2$S$_4$. At low temperature, a marked upturn of both $C$ and $\varrho$ is suppressed by magnetic field, which suggests a picture of Kondo coupling between conduction electrons in the VS$_2$ layers and impurity spins of the V$^{3+}$ ions located between layers. This picture opens the possibility of controlling electronic correlations and the FL to non-FL crossover in simple layered materials. For instance, we envisage that the coupling between layers provided by the impurity spins may realize a two-channel Kondo state.

cond-mat.str-el↗

arXiv2014

Impact of the various spin and orbital ordering processes on multiferroic properties of orthovanadate DyVO3

The orthovanadate DyVO3 crystal, known to exhibit multiple structural, spin and orbital ordering transitions, is presently investigated on the basis of magnetization, heat capacity, resistivity, dielectric and polarization measurements. Our main result is experimental evidence for the existence of multiferroicity below a high TC of 108 K over a wide temperature range including different spin-orbital ordered states. The onset of ferroelectricity is found to coincide with the antiferromagnetic C-type spin ordering transition taking place at 108 K, which indicates that DyVO3 belongs to type II multiferroics exhibiting a coupling between magnetism and ferroelectricity. Some anomalies detected on the temperature dependence of electric polarization are discussed with respect to the nature of the spin-orbital ordered states of the V sublattice and the degree of spin alignment in the Dy sublattice. The orthovanadates RVO3 (R = rare earth or Y) form an important new category for searching for high-TC multiferroics.

cond-mat.str-el↗

arXiv2013

Cobalt spin state above the valence and spin-state transition in (Pr0.7Sm0.3)0.7Ca0.3CoO3

(Pr0.7Sm0.3)0.7Ca0.3CoO3 belongs to a class of cobalt oxides undergoing a first-order transition (T* close to 90 K) associated to a coupled change in the valence and spin-state degrees of freedom. The Curie-Weiss regime present around room temperature (T >> T*) was analysed in detail to address the controversial issue of the cobalt spin states above the transition. This magnetic investigation indicates that the Co4+ are in an intermediate spin-state, while the Co3+ are in a mixed state combining low-spin and high-spin states. These results are discussed with respect to the literature on related compounds and recent results of x-ray absorption spectroscopy.

cond-mat.str-el↗

arXiv2013

Jumps in entropy and magnetic susceptibility at the valence and spin-state transition in a cobalt oxide

A wide family of cobalt oxides of formulation (Pr,Ln,Ca)CoO3 (Ln being a lanthanide) exhibits a coupled valence and spin-state transition (VSST) at a temperature T*, which involves two concomitant modifications: (i) a change in the spin state of Co3+ from low-spin (T < T*) to a higher spin-state (T > T*), and (ii) a change in the valence state of Pr, from a mixed Pr4+/Pr3+ state (T < T*) to a purely trivalent state (T > T*), accompanied by an equivalent charge transfer within the Co3+/Co4+ subsystem. In the present paper, the VSST taking place in (Pr0.7Sm0.3)0.7Ca0.3CoO3 at T* = about 90 K is investigated by magnetization and heat capacity measurements. First, we quantitatively characterized the jumps in magnetic susceptibility (khi) and entropy (S) around T*. Then, these values were compared to those calculated as a function of the variations in the population of the different cationic species involved in the VSST. X-ray absorption spectroscopy experiments recently showed that the higher spin state above T* should be regarded as an inhomogeneous mixture between low-spin (LS) and high-spin (HS) states. In the frame of this description, we demonstrate that the jumps in both khi and S can be associated to the same change in the Co3+ HS content around T*. This result lends further support to the relevance of the LS/HS picture for the VSST, challenging the currently dominant interpretation based on the occurrence of an intermediate-spin (IS) state of Co3+ above T*.

cond-mat.str-el↗

arXiv2013

Coupled valence and spin state transition in (Pr0.7Sm0.3)0.7Ca0.3CoO3

The coupled valence and spin state transition (VSST) taking place in (Pr0.7Sm0.3)0.7Ca0.3CoO3 was investigated by soft x-ray absorption spectroscopy (XAS) experiments carried out at the Pr-M4,5, Co-L2,3, and O-1s edges. This VSST is found to be composed of a sharp Pr/Co valence and Co spin state transition centered at T*=89.3 K, followed by a smoother Co spin-state evolution at higher temperatures. At T < T*, we found that the praseodymium displays a mixed valence Pr3+/Pr4+ with about 0.13 Pr4+/f.u., while all the Co3+ is in the low-spin (LS) state. At T around T*, the sharp valence transition converts all the Pr4+ to Pr3+ with a corresponding Co3+ to Co4+ compensation. This is accompanied by an equally sharp spin state transition of the Co3+ from the low to an incoherent mixture of low and high spin (HS) states. An involvement of the intermediate spin (IS) state can be discarded for the Co3+. While above T* and at high temperatures the system shares rather similar properties as Sr-doped LaCoO3, at low temperatures it behaves much more like EuCoO3 with its highly stable LS configuration for the Co3+. Apparently, the mechanism responsible for the formation of Pr4+ at low temperatures also helps to stabilize the Co3+ in the LS configuration despite the presence of Co4+ ions. We also found out that that the Co4+ is in an IS state over the entire temperature range investigated in this study (10-290 K). The presence of Co3+ HS and Co4+ IS at elevated temperatures facilitates the conductivity of the material.

cond-mat.str-el↗

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↗

arXiv2010

On the derivation of the magnetocaloric properties in ferrimagnetic spinel Mn3O4

Large magnetocaloric effect has been observed in Mn3O4 around its ferrimagnetic transition at TN = 42.75 K. Field-induced isothermal entropy changes (\DeltaS) were derived from both magnetic and calorimetric techniques. The maximum |\DeltaS| and adiabatic temperature change (ΔTad) at TN are 11 J kg-1 K-1 and 1.9 K, respectively, for a magnetic field change of 20 kOe. Moreover, it is found that the complex magnetic phase transitions taking place below TN produce additional -but smaller- features on \DeltaS(T).

cond-mat.mtrl-sci↗

arXiv2010

Magnetocaloric effect and improved relative cooling power in (La0.7Sr0.3MnO3/SrRuO3) superlattices

Magnetic properties of a series of (La0.7Sr0.3MnO3/SrRuO3) superlattices, where the SrRuO3 layer thickness is varying, are examined. A room-temperature magnetocaloric effect is obtained owing to the finite size effect which reduces the TC of La0.7Sr0.3MnO3 layers. While the working temperature ranges are enlarged,, -DeltaSmax values remains similar to the values in polycrystalline La0.7Sr0.3MnO3. Consequently, the relative cooling powers are significantly improved, the microscopic mechanism of which is related to the effect of the interfaces at La0.7Sr0.3MnO3/SrRuO3 and higher nanostructural disorder. This study indicates that artificial oxide superlattices/multilayers might provide an alternative pathway in searching for efficient room-temperature magnetic refrigerators for (nano)microscale systems.

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↗

arXiv2006

Valence, spin, and orbital state of the Co ions in the one-dimensional Ca3Co2O6: an x-ray absorption and magnetic circular dichroism study

We have investigated the valence, spin, and orbital state of the Co ions in the one-dimensional cobaltate Ca3Co2O6 using x-ray absorption and x-ray magnetic circular dichroism at the Co-L2,3 edges. The Co ions at both the octahedral Co_oct and trigonal Co_trig sites are found to be in a 3+ state. From the analysis of the dichroism we established a low-spin state for the Co_oct and a high-spin state with an anomalously large orbital moment of 1.7 muB at the Co3+ trig ions. This large orbital moment along the c-axis chain and the unusually large magnetocrystalline anisotropy can be traced back to the double occupancy of the d2 orbital in trigonal crystal field.

cond-mat.str-el↗

arXiv2006

Scaling behavior in thermoelectric misfit cobalt oxides

We investigate both thermoelectric and thermodynamic properties of the misfit cobalt oxide [Bi$_{1.7}$Co$_{0.3}$Ca$_{2}$O$_{4}$]$^{RS}_{0.6}$CoO$_{2}$. A large negative magnetothermopower is found to scale with both magnetic field and temperature revealing a significant spin entropy contribution to thermoelectric properties giving rise to a constant S$_0\approx$ 60 $μ$V K$^{-1}$ equal to the high temperature asymptotic value of the spin 1/2 entropy. Low temperature specific heat measurements allow us to determine an enhanced electronic part with $γ\approx$ 50 mJ (mol K$^{2}$)$^{-1}$ attesting of strong correlations. Thereby, a critical comparison between [Bi$_{1.7}$Co$_{0.3}$Ca$_{2}$O$_{4}$]$^{RS}_{0.6}$CoO$_{2}$, other cobaltites as well as other materials reveals a universal behavior of the thermopower low temperature slope as a function of $γ$ testifying thus a purely electronic origin. This potentially generic scaling behavior suggests here that the high room temperature value of the thermopower in misfit cobalt oxides results from the addition of a spin entropy contribution to an enlarged electronic one.

cond-mat.str-el↗

arXiv2006

High and low-temperature crystal and magnetic structures of epsilon-Fe2O3 and their correlation to its magnetic properties

The crystal and magnetic structures of the orthorhombic e-Fe2O3 have been studied by simultaneous Rietveld refinement of X-ray and neutron powder diffraction data in combination with Mossbauer spectroscopy, as well as magnetisation and heat capacity measurements. It has been found that above 150 K the e-Fe2O3 polymorph is a collinear ferrimagnet with the magnetic moments directed along the a axis, while the magnetic ordering below 80 K is characterised by a square-wave incommensurate structure. The transformation between these two states is a second order phase transition and involves subtle structural changes mostly affecting the coordination of the tetrahedral and one of the octahedral Fe sites. The temperature dependence of the e-Fe2O3 magnetic properties is discussed in the light of these results.

cond-mat.mtrl-sci↗

arXiv2005

Voltage noise and surface current fluctuations in the superconducting surface sheath

We report the first measurements of the voltage noise in the surface superconductivity state of a type-II superconductor. We present strong evidences that surface vortices generates surface current fluctuations whose magnitude can be modified by the pinning ability of the surface. Simple two-stage mechanism governed by current conservation appears to describe the data. We conclude that large voltage fluctuations induced by surface vortices exist while the bulk is metallic. Furthermore, this experiment shows that sole surface current fluctuations can account for the noise observed even in the presence of vortices in the bulk.

cond-mat.supr-con↗

arXiv2005

Strongly correlated properties of the thermoelectric cobalt oxide Ca3Co4O9

We have performed both in-plane resistivity, Hall effect and specific heat measurements on the thermoelectric cobalt oxide Ca$_{3}$Co$_{4}$O$_{9}$. Four distinct transport regimes are found as a function of temperature, corresponding to a low temperature insulating one up to $T_{min}\approx $63 K, a strongly correlated Fermi liquid up to $T^*\approx $140 K, with $ρ=ρ_0+AT^2$ and $A\approx 3.63$ $10^{-2} μΩcm/K^{2}$, followed by an incoherent metal with $k_Fl\leq 1$ and a high temperature insulator above T$^{**}\approx $510 K . Specific heat Sommerfeld coefficient $γ= 93$ mJ/(mol.K$^{2}$) confirms a rather large value of the electronic effective mass and fulfils the Kadowaki-Woods ratio $A/γ^2 \approx 0.45$ 10$^{-5}$ $μΩcm.K^2/(mJ^2mol^{-2})$. Resistivity measurements under pressure reveal a decrease of the Fermi liquid transport coefficient A with an increase of $T^*$ as a function of pressure while the product $A(T^*)^2/a$ remains constant and of order $h/e^2$. Both thermodynamic and transport properties suggest a strong renormalization of the quasiparticles coherence scale of order $T^*$ that seems to govern also thermopower.

cond-mat.str-el↗

arXiv2004

Investigation of the field-treated magnetic state in Gd5Ge4

At low temperatures, the intermetallic compound Gd$_5$Ge$_4$ shows a sharp field-induced transition into a ferromagnetic state around 25 kOe of applied field. The material remains in the field treated ferromagnetic state even when the magnetic field is removed. We have investigated the character of this field-treated state by magnetization and heat capacity measurements. The nature of the magnetization and the heat capacity are found to be different above and below a charactersitic temperature Tirr = 25 K.

cond-mat.str-el↗

arXiv2004

Quantum Tunneling of the Magnetization in the Ising Chain Compound Ca3Co2O6

The magnetic behavior of the Ca3Co2O6 spin chain compound is characterized by a large Ising-like character of its ferromagnetic chains, set on triangular lattice, that are antiferromagnetically coupled. At low temperature, T < 7K, the 3D antiferromagnetic state evolves towards a spin frozen state. In this temperature range, magnetic field driven magnetization of single crystals (H//chains) exhibits stepped variations. The occurrence of these steps at regular intervals of the applied magnetic field, Hstep=1.2T, is reminiscent of the quantum tunneling of the magnetization (QTM) of molecular based magnets. Magnetization relaxation experiments also strongly support the occurrence of this quantum phenomenon. This first observation of QTM in a magnetic oxide belonging to the large family of the A3BBO6 compounds opens new opportunities to study a quantum effect in a very different class of materials from molecular magnets.

cond-mat.str-el↗

arXiv2004

Magnetic susceptibility and heat capacity investigations of the unconventional spin-chain compound Sr3CuPtO6

The Heisenberg spin chain compound Sr3CuPtO6 is investigated by magnetic susceptibility and heat capacity measurements. Sr3CuPtO6 has an unconventional chain structure in the sense that i) the spin half copper atoms are arranged in a zigzag chain structure, and ii) neighboring Cu atoms along the chains are separated by spin zero platinum atoms. We report that this compound shows broad features in the temperature dependence of both the magnetic contribution to the heat capacity and the magnetic susceptibility. Despite the unconventional nature of the spin chain structure, this set of data exhibits good agreement with theoretical models for a classical S = 1/2 Heisenberg spin chain compound. The values of the intra-chain coupling constant, obtained by different techniques, are found to be very close to each other. The low temperature heat capacity data (below ~ 6 K) exhibit a deviation from the theoretically expected behavior, which could be related to a small energy gap in the spin excitation spectrum.

cond-mat.str-el↗