arXiv subjects

W. Prellier

Publications and source records attributed to W. Prellier.

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↗

arXiv2025

Tailoring non-collinear magnetism and 3d $-$ 4f exchange interactions in RVO$_3$ epitaxial thin films

In orthorhombic perovskite oxides (RMO$_3$), substituting R$^{3+}$ rare-earth cations tailors the spin, orbital, and charge degrees of freedom of the central M$^{3+}$ transition metal cations through lattice distortions. In turn, these modify also the surrounding environment of R$^{3+}$. When both R$^{3+}$ and M$^{3+}$ exhibit magnetic properties, phenomena such as spin reorientation and magnetization reversal can occur. In fact, the underlying exchange interactions between M-$3d$ spins and R-$4f$ magnetic moments enrich the multifunctional character of RMO$_3$, particularly when combined with structural distortions. They play a crucial role in achieving appealing properties such as robust magnetoelectricity with non-collinear magnetic orders. Here, we explore the exchange coupling in epitaxial PrVO$_3$ thin films, selectively probing the magnetism of cation sublattices, and uncovering simultaneous V$^{3+}$ $3d$ spin reorientation and Pr$^{3+}$ $4f$ magnetization reversal using spectroscopy techniques. By strain engineering, we manipulate the lattice distortions to rationalize their role in coupling $3d$ spins and $4f$ magnetic moments. Theorectical calculations show that octahedral rotations and Jahn-Teller distortions act as tuning mechanisms, promoting competition between orbital and spin orders. The observed coupling between magnetic cations and lattice distortions can be extended to other orthorhombic RMO$_3$ systems, advancing the understanding of controlling spins in engineered perovskite heterostructures and superlattices.

cond-mat.mtrl-sci↗

arXiv2025

Nanoscale characterization of atomic positions in orthorhombic perovskite thin films

The crystal structure determines many of the physical properties of oxide perovskites (ABO$_3$) and only a tiny modification of the lattice structure causes major changes in the functional properties through the interplay among spin, orbital and charge orders. The determination of characteristic distortions and symmetries is a valuable asset for understanding the structure-properties relationship and guiding the design of epitaxial oxide heterostructures, where electron degrees of freedom and correlated electronic states can be tailored. Even until new phases, otherwise absent in bulk materials, may appear. Here, we report on the in-depth structural characterization of 50~nm-LaVO$_3$ thin film grown onto (110)-oriented DyScO$_3$ by molecular beam epitaxy. We have investigated the heterostructure by means of x-ray diffraction, high-resolution and scanning transmission electron microscopies, scanning precession electron diffraction tomography and first-principle calculations. LaVO$_3$ crystallizes in the orthorhombic $Pbnm$ space group and is constrained by the substrate, which imposes a growth along the $[110]$ orthorhombic direction, over the 140 deposited unit cells. The mapping of the reciprocal space allows determining the orientation of the film and refining the lattice parameters. Using scanning transmission electron microscopy, we analyzed the structure of LaVO$_3$, focusing on the determination of the antipolar displacement of the rare earth. Additionally, 3D electron diffraction enabled to resolve the atomic positions of all species within the film.

cond-mat.mtrl-sci↗

arXiv2023

Artificial ageing of thin films of the indium-free transparent conducting oxide SrVO3

SrVO3 (SVO) is a prospective candidate to replace the conventional indium-tin-oxide (ITO) among the new transparent conducting oxide (TCO) generation. In this study, the structural, electrical, and optical properties of SVO thin films, both epitaxial and polycrystalline, are determined during and after heat treatments in the 150-250 {\deg}C range and under ambient environment in order to explore the chemical stability of this material. The use of these relatively low temperatures speeds up the natural ageing of the films, and allows to follow the evolution of their related properties. The combination of techniques rather sensitive to the film surface and of techniques sampling the film volume will emphasize the presence of a surface oxidation evolving in time at low annealing temperatures, whereas the perovskite phase is destroyed throughout the film for treatments above 200 {\deg}C. The present study is designed to understand the thermal degradation and long-term stability issues of vanadate-based TCOs, and to identify technologically viable solutions for the application of this group as new TCOs.

cond-mat.mtrl-sci↗

arXiv2020

Engineering the magnetic and magnetocaloric properties of PrVO3 epitaxial oxide thin films by strain effects

Combining multiple degrees of freedom in strongly-correlated materials such as transition-metal oxides would lead to fascinating magnetic and magnetocaloric features. Herein, the strain effects are used to markedly tailor the magnetic and magnetocaloric properties of PrVO3 thin films. The selection of appropriate thickness and substrate enables us to dramatically decrease the coercive magnetic field from 2.4 T previously observed in sintered PVO3 bulk to 0.05 T for compressive thin films making from the PrVO3 compound a nearly soft magnet. This is associated with a marked enhancement of the magnetic moment and the magnetocaloric effect that reach unusual maximum values of roughly 4.86 uB and 56.8 J/kg K in the magnetic field change of 6 T applied in the sample plane at the cryogenic temperature range (3 K), respectively. This work strongly suggests that taking advantage of different degrees of freedom and the exploitation of multiple instabilities in a nanoscale regime is a promising strategy for unveiling unexpected phases accompanied by a large magnetocaloric effect in oxides.

cond-mat.mtrl-sci↗

arXiv2015

Preferential Orientation Relationships in Ca$_2$MnO$_4$ Ruddlesden-Popper thin films

A high-throughput investigation of local epitaxy (called combinatorial substrate epitaxy) was carried out on Ca$_2$MnO$_4$ Ruddlesden-Popper thin films of six thicknesses (from 20 to 400 nm), all deposited on isostructural polycrystalline Sr$_2$TiO$_4$ substrates. Electron backscatter diffraction revealed grain-over-grain local epitaxial growth for all films, resulting in a single orientation relationship ($OR$) for each substrate-film grain pair. Two preferred epitaxial $ORs$ accounted for more than 90 \% of all ORs on 300 different microcrystals, based on analyzing 50 grain pairs for each thickness. The unit cell over unit cell $OR$ ([100][001]$_{film}$ $\parallel$ [100][001]$_{substrate}$, or $OR1$) accounted for approximately 30 \% of each film. The $OR$ that accounted for 60 \% of each film ([100][001]$_{film}$ $\parallel$ [100][010]$_{substrate}$, or $OR2$) corresponds to a rotation from $OR1$ by 90$^{\circ}$ about the a-axis. $OR2$ is strongly favored for substrate orientations in the center of the stereographic triangle, and $OR1$ is observed for orientations very close to (001) or to those near the edge connecting (100) and (110). While $OR1$ should be lower in energy, the majority observation of $OR2$ implies kinetic hindrances decrease the frequency of $OR1$. Persistent grain over grain growth and the absence of variations of the $OR$ frequencies with thickness implies that the growth competition is finished within the first few \si{\nano\meter}, and local epitaxy persists thereafter during growth.

cond-mat.mtrl-sci↗

arXiv2014

Growth of Ca$_2$MnO$_4$ Ruddlesden-Popper structured thin films using Combinatorial Substrate Epitaxy

The local epitaxial growth of pulsed laser deposited Ca$_2$MnO$_4$ films on polycrystalline spark plasma sintered Sr$_2$TiO$_4$ substrates was investigated to determine phase formation and preferred epitaxial orientation relationships ($ORs$) for isostructural Ruddlesden-Popper (RP) heteroepitaxy, further developing the high-throughput synthetic approach called Combinatorial Substrate Epitaxy (CSE). Both grazing incidence X-ray diffraction and electron backscatter diffraction (EBSD) patterns of the film and substrate were indexable as single-phase RP-structured compounds. The optimal growth temperature (between 650 $^{\circ}$C and 800 $^{\circ}$C) was found to be 750 $^{\circ}$C using the maximum value of the average image quality (IQ) of the backscattered diffraction patterns. Films grew in a grain-over-grain pattern such that each Ca$_2$MnO$_4$ grain had a single $OR$ with the Sr$_2$TiO$_4$ grain on which it grew. Three primary $ORs$ described 47 out of 49 grain pairs that covered nearly all of RP orientation space. The first $OR$, found for 20 of the 49, was the expected RP unit-cell over RP unit-cell $OR$, expressed as [100][001]$_{film}$||[100][001]$_{sub}$. The other two $ORs$ were essentially rotated from the first by 90$^{\circ}$, with one (observed for 17 of 49 pairs) being rotated about the [100] and the other (observed for 10 of 49 pairs) being rotated about the [110] (and not exactly by 90$^{\circ}$). These results indicate that only a small number of $ORs$ are needed to describe isostructural RP heteroepitaxy and further demonstrate the potential of CSE in the design and growth of a wide range of complex functional oxides.

cond-mat.mtrl-sci↗

arXiv2014

Structural analysis of strained LaVO$_3$ thin films

While structure refinement is routinely achieved for simple bulk materials, the accurate structural determination still poses challenges for thin films due on the one hand to the small amount of material deposited on the thicker substrate and, on the other hand, to the intricate epitaxial relationships that substantially complicate standard X-ray diffraction analysis. Using a combined approach, we analyze the crystal structure of epitaxial LaVO$_3$ thin films grown on (100)-oriented SrTiO$_3$. Transmission electron microscopy study reveals that the thin films are epitaxially grown on SrTiO$_3$ and points to the presence of 90$^{\circ}$ oriented domains. The mapping of the reciprocal space obtained by high resolution X-ray diffraction permits refinement of the lattice parameters. We finally deduce that strain accommodation imposes a monoclinic structure onto the LaVO$_3$ film. The reciprocal space maps are numerically processed and the extracted data computed to refine the atomic positions, which are compared to those obtained using precession electron diffraction tomography. We discuss the obtained results and our methodological approach as a promising thin film structure determination for complex systems.

cond-mat.mtrl-sci↗

arXiv2014

Structural characterization of PrVO3 epitaxial thin films

Rare earth perovskite oxides constitute a wide family of materials presenting functional proper- ties strongly coupled to their crystalline structure. Here, we report on the experimental results on epitaxial PrVO3 deposited on SrTiO3 single crystal substrates by pulsed laser deposition. By com- bining advanced structural characterization tools, we have observed that the PVO unrelaxed film structure grown on STO, is characterized by two kinds of oriented domains whose epitaxial relations are: (i) PrVO3[110]o//SrTiO3[001]c and PrVO3[001]o//SrTiO3[100]c, (ii) PrVO3[110]o//SrTiO3[001]c and PrVO3[001]o//SrTiO3[010]c. We have also measured reciprocal space maps. From these results, we have determined that the PVO film epitaxy on STO imposes a lowering of the PVO structure symmetry from orthorhombic (Pbnm) to monoclinic (P21/m). We show, the nominal strain induced by the substrate being constant, that the obtained film structure depends on both growth oxygen and temperature. Thus, by finely controlling the deposition conditions, we could tune the strain experienced by PrVO3 thin film. These results show an alternative to substrate mismatch as a path to control the strain and structure of PVO films.

physics.chem-ph↗

arXiv2014

BiFeO3/La0.7Sr0.3MnO3 heterostructures deposited on Spark Plasma Sintered LaAlO3 Substrates

Multiferroic BiFeO3 (BFO) / La0.7Sr0.3MnO3 heterostructured thin films were grown by pulsed laser deposition on polished spark plasma sintered LaAlO3 (LAO) polycrystalline substrates. Both polycrystalline LAO substrates and BFO films were locally characterized using electron backscattering diffraction (EBSD), which confirmed the high-quality local epitaxial growth on each substrate grain. Piezoforce microscopy was used to image and switch the piezo-domains, and the results are consistent with the relative orientation of the ferroelectric variants with the surface normal. This high-throughput synthesis process opens the routes towards wide survey of electronic properties as a function of crystalline orientation in complex oxide thin film synthesis.

cond-mat.mtrl-sci↗

arXiv2013

High-throughput synthesis of thermoelectric Ca$_3$Co$_4$O$_9$ films

Properties of complex oxide thin films can be tuned over a range of values as a function of mismatch, composition, orientation, and structure. Here, we report a strategy for growing structured epitaxial thermoelectric thin films leading to improved Seebeck coefficient. Instead of using single-crystal sapphire substrates to support epitaxial growth, Ca$_3$Co$_4$O$_9$ films are deposited, using the Pulsed Laser Deposition technique, onto Al$_2$O$_3$ polycrystalline substrates textured by Spark Plasma Sintering. The structural quality of the 2000 Åthin film was investigated by Transmission Electron Microscopy, while the crystallographic orientation of the grains and the epitaxial relationships were determined by Electron Back Scatter Diffraction. The use of a polycrystalline ceramic template leads to structured films that are in good local epitaxial registry. The Seebeck coefficient is about 170 $μ$V/K at 300 K, a typical value of misfit material with low carrier density. This high-throughput process, called combinatorial substrate epitaxy, appears to facilitate the rational tuning of functional oxide films, opening a route to the epitaxial synthesis of high quality complex oxides.

cond-mat.mtrl-sci↗

arXiv2013

Growth and texture of Spark Plasma Sintered Al2O3 ceramics: a combined analysis of X-rays and Electron Back Scatter Diffraction

Textured alumina ceramics were obtained by Spark Plasma Sintering (SPS) of undoped commercial a-Al2O3 powders. Various parameters (density, grain growth, grain size distribution) of the alumina ceramics, sintered at two typical temperatures 1400°C and 1700°C, are investigated. Quantitative textural and structural analysis, carried out using a combination of Electron Back Scattering Diffraction (EBSD) and X-ray diffraction (XRD), are represented in the form of mapping, and pole figures. The mechanical properties of these textured alumina ceramics include high elastic modulus and hardness value with high anisotropic nature, opening the door for a large range of applications

cond-mat.mtrl-sci↗

arXiv2012

Charge localization at the interface between La1-xSrxMnO3 and the infinite layers cuprate CaCuO2

(CaCuO2)m/(La0.7Sr0.3MnO3)n superlattices, consisting of the infinite layers cuprate CaCuO2 and the optimally doped manganite La1-xSrxMnO3, were grown by pulsed laser deposition. The transport properties are dominated by the manganite block. X-Ray Absorption spectroscopy measurements show a clear evidence of an orbital reconstruction at the interface, ascribed to the hybridization between the Cu 3d3z2-r2 and the Mn 3d3z2-r2 orbitals via interface apical oxygen ions. Such a mechanism localizes holes at the interfaces, thus preventing charge transfer to the CaCuO2 block. Some charge (holes) transfer occurs toward the La0.7Sr0.3MnO3 block in strongly oxidized superlattices, contributing to the suppression of the magnetotransport properties.

cond-mat.supr-con↗

arXiv2012

High Tc superconductivity in superlattices of insulating oxides

We report the occurrence of superconductivity, with maximum Tc = 40 K, in superlattices (SLs) based on two insulating oxides, namely CaCuO2 and SrTiO3. In these (CaCuO2)n/(SrTiO3)m SLs, the CuO2 planes belong only to CaCuO2 block, which is an antiferromagnetic insulator. Superconductivity, confined within few unit cells at the CaCuO2/SrTiO3 interface, shows up only when the SLs are grown in a highly oxidizing atmosphere, because of extra oxygen ions entering at the interfaces. Evidence is reported that the hole doping of the CuO2 planes is obtained by charge transfer from the interface layers, which act as charge reservoir.

cond-mat.supr-con↗

arXiv2012

Electronic structure and optical band gap of CoFe2O4 thin films

Electronic structure and optical band gap of CoFe2O4 thin films grown on (001) oriented LaAlO3 have been investigated. Surprisingly, these films show additional Raman modes at room temperature as compared to a bulk spinel structure. The splitting of Raman modes is explained by considering the short-range ordering of Co and Fe cations in octahedral site of spinel structure. In addition, an expansion of band-gap is observed with the reduction of film thickness, which is explained by the quantum size effect and misfit dislocation. Such results provide interesting insights for the growth of spinel phases.

cond-mat.mtrl-sci↗

arXiv2012

Incipient ferroelectricity in 2.3% tensile-strained CaMnO3 films

Epitaxial CaMnO3 films grown with 2.3% tensile strain on (001)-oriented LaAlO3 substrates are found to be incipiently ferroelectric below 25 K. Optical second harmonic generation (SHG) was used for the detection of the incipient polarization. The SHG analysis reveals that CaMnO3 crystallites with in-plane orientation of the orthorhombic b axis contribute to an electric polarization oriented along the orthorhombic a (resp.\ c) axis in agreement with the predictions from density functional calculations.

cond-mat.mtrl-sci↗

arXiv2011

Switching magnetoresistance in vertically interfaced Pr0.5Ca0.5MnO3 grown on ZnO nanowires

The synthesis, morphology and magneto-transport properties of nanostructure-engineered charge-ordered Pr0.5Ca0.5MnO3 grown on ZnO nanowires are reported. The stability of the charge-ordering can be tuned, but more interestingly the sign of the magnetoresistance is inverted at low temperatures. Coexistence of ferromagnetic clusters on the surface and antiferromagnetic phase in the core of the grains were considered in order to understand these features. This work suggests that such a process of growing on nanowires network can be readily extended to other transition metal oxides and open doors towards tailoring their functionalities.

cond-mat.mtrl-sci↗

arXiv2011

Structural transition in LaVO3/SrVO3 superlattices and its influence on transport properties

Measurements of the resistive properties and the lattice parameters of a (LaVO3)[6 unit cells]/(SrVO3)[1 unit cell] superlattice between 10K and room temperature are presented. A low temperature metallic phase compatible with a Fermi liquid behavior is evidenced. It disappears in the vicinity of a structural transition from a monoclinic to tetragonal phase, in which disorder seems to strongly influence the transport. Our results will enrich the understanding of the electronic properties of complex heterostructures.

cond-mat.str-el↗