arXiv subjects

Philippe Lecoeur

Publications and source records attributed to Philippe Lecoeur.

At least 19 recordsLinked to original sources

arXiv2025

Light-induced photomechanical patterning of ferroelectric polarization

Tailoring at will polar textures in ferroelectrics is critical for the development of nanoscale electronics and functional oxide technologies. Freestanding ferroelectric membranes have enabled studies of strain-induced polarization responses, but the control over membrane shape and local polarization typically remains limited to spontaneous buckling or uniaxial mechanical deformations. In this work, we employ a versatile photosensitive-polymer patterning approach to impose programmable bending strain profiles in ferroelectric membranes. Using BaTiO3 as a model system, we demonstrate deterministic 90{\deg} polarization rotation driven by engineered in-plane strain, and 180{\deg} polarization reversal arising from flexoelectric coupling through a controlled strain gradient. These results establish this programmable bending as a powerful approach to investigate strain-dependent domain structures, leverage flexoelectric effects, and engineer custom ferroelectric landscapes across a wide range of oxide membranes.

cond-mat.mtrl-sci↗

arXiv2025

Strain-induced polarization rotation in freestanding ferroelectric oxide membranes

Freestanding ferroelectric membranes have emerged as a versatile tool for strain engineering, enabling the exploration of ferroelectric properties beyond traditional epitaxy. The resulting ferroelectric domain patterns stem from the balance at the local scale of several effects playing a key role, i.e. piezoelectricity linked to strain, and flexoelectricity arising from strain gradients. To weight their respective contributions for a given membrane geometry, the strain profile has to be mapped with respect to the ferroelectric polarization landscape, a necessary step to allow for a controlled tailoring of the latter. In this study, we examine the effect of bending strain on a Pb(Zr,Ti)O3 membrane in a fold-like structure, observing a polarization rotation from out-of-plane to in-plane at the fold apex. Combining piezoresponse force microscopy, Raman spectroscopy, and scanning transmission electron microscopy, we map the ferroelectric polarization direction relative to the height profile of the membrane, and discuss the contributions of strain and strain gradients for this archetypal fold geometry. Our findings offer new insights into strain-engineered polarization configurations, and emphasize strain effects at the nanoscale to tune the functional properties in freestanding membranes.

cond-mat.mtrl-sci↗

arXiv2023

Magneto-optical properties of textured La$_{2/3}$Sr$_{1/3}$MnO$_3$ thin films integrated on silicon via a Ca$_2$Nb$_3$O$_{10}$ nanosheet layer

We demonstrate the possibility of growing textured La$_{2/3}$Sr$_{1/3}$MnO$_3$ (LSMO) thin films on silicon substrates with magneto-optical and optical properties comparable to high-quality epitaxial layers grown on bulk SrTiO$_3$ (STO). The pulsed laser deposition growth of LSMO is achieved by a two-dimensional nanosheet (NS) seed layer of Ca$_2$Nb$_3$O$_{10}$ (CNO) inducing epitaxial stabilization of LSMO films. The resulting layers possess a higher Curie temperature and a lower overall magnetization than samples of LSMO on STO. Spectra of the full permittivity tensor were calculated from optical and magneto-optical measurements. Spectral dependencies of both the diagonal and off-diagonal elements share many similarities between the LSMO/NS/Si and LSMO/STO samples. These similarities indicate comparable electronic structures of the layers and demonstrate comparable optical quality of textured LSMO on NS/Si and epitaxial LSMO on STO.

cond-mat.mtrl-sci↗

arXiv2023

Ferroelectricity in tetragonal ZrO$_2$ thin films

We report on the crystal structure and ferroelectric properties of epitaxial ZrO$_2$ films ranging from 7 to 42 nm thickness grown on La$_{0.67}$Sr$_{0.33}$MnO$_3$-buffered (110)-oriented SrTiO$_3$ substrate. By employing X-ray diffraction, we confirm a tetragonal phase at all investigated thicknesses, with slight in-plane strain due to the substrate in the thinnest films. Further confirmation of the tetragonal phase was obtained through Infrared absorption spectroscopy with synchrotron light, performed on ZrO$_2$ membrane transferred onto a high resistive Silicon substrate. Up to a thickness of 31 nm, the ZrO$_2$ epitaxial films exhibit ferroelectric behavior, at variance with the antiferroelectric behavior reported previously for the tetragonal phase in polycrystalline films. However, the ferroelectricity is found here to diminish with increasing film thickness, with a polarization of about 13 $\mu$C.cm$^{-2}$ and down to 1 $\mu$C.cm$^{-2}$ for 7 nm and 31 nm-thick ZrO$_2$ films, respectively. This highlights the role of thickness reduction, substrate strain, and surface effects in promoting polarization in the tetragonal ZrO$_2$ thin films. These findings provide new insights into the ferroelectric properties and structure of ZrO$_2$ thin films, and open up new directions to investigate the origin of ferroelectricity in ZrO$_2$ and to optimize this material for future applications.

cond-mat.mtrl-sci↗

arXiv2022

Electro-optic properties of ZrO2, HfO2 and LiNbO3 ferroelectric phases: A comprehensive and comparative study with density functional theory

We report the Pockels electro-optic properties of ZrO2 and HfO2 orthorhombic Pbc21 and rhombohedral R3m ferroelectric phases, and we compare them to the well-known LiNbO3 Pockels material from density functional theory calculations using the CRYSTAL suite of programs. Specifically, three essential processes are explicitly investigated: The electronic, the ionic (or vibrational), and the piezoelectric contributions. Our calculations reveal that the ionic part coming from the low frequency phonon modes contributes the most to the electro-optic coefficients of rhombohedral LiNbO3 and of orthorhombic ZrO2 and HfO2. While these low-frequency modes show zero contribution to Pockels coefficients for the rhombohedral phase of the latter compounds.

cond-mat.mtrl-sci↗

arXiv2021

Stabilization of the epitaxial rhombohedral ferroelectric phase in ZrO2 by surface energy

Doped HfO2 and HfO2-ZrO2 compounds are gaining significant interest thanks to their ferroelectric properties in ultrathin films. Here, we show that ZrO2 could be a playground for doping and strain engineering to increase the thickness in epitaxial thin films. Based on surface energy considerations supported by ab initio calculations, we show that a pure ZrO2 epitaxial thin film exhibits a ferroelectric rhombohedral phase (r-phase, with R3m space group) more stable than for the Hf0.5Zr0.5O2 (HZO) and pure HfO2 cases. In particular, for a thickness up to 37 nm we experimentally evidence a single (111)-oriented r-phase in ZrO2 films deposited on La2/3Sr1/3MnO3-buffered DyScO3(110) substrate, while a tetragonal phase is observed alongside the rhombohedral one on SrTiO3(001). The formation of this r-phase is discussed and compared between HfO2, ZrO2 and HZO, highlighting the role of surface energy.

cond-mat.mtrl-sci↗

arXiv2021

Universal Fabrication of Two-Dimensional Electron Systems in Functional Oxides

Two-dimensional electron systems (2DESs) in functional oxides are promising for applications, but their fabrication and use, essentially limited to SrTiO$_3$-based heterostructures, are hampered by the need of growing complex oxide over-layers thicker than 2~nm using evolved techniques. This work shows that thermal deposition of a monolayer of an elementary reducing agent suffices to create 2DESs in numerous oxides.

cond-mat.str-el↗

arXiv2020

Stress measurements in silicon photonics by integrated Raman spectroscopy

Complex 3D integration of photonic and electronic integrated circuits is of particular interest to carry the photonics roadmap and to address challenges but involves mechanical stress, often detrimental for the behavior of optical components. Existing experiments failed to carefully analyze the stress in such integrated optical devices due to the requirement in terms of feature sizes, few hundreds of nanometers, and 3D-stacked integration. We present for the first time the characterization of the stress tensor of a silicon waveguide using Integrated Raman Spectroscopy (IRS). This experimental technique is directly sensitive to the effective stress, which involves changes in optical properties of the guided mode, at the working wavelength and polarization state of the photonic component. The experimental stress tensor is in good agreement with simulations.

physics.app-ph↗

arXiv2019

Magnetic domain wall motion in SrRuO$_3$ thin films

Influence of substrate miscut on magnetization dynamics in SrRuO$_3$ (SRO) thin films was studied. Two films were grown on SrTiO$_3$ substrates with high ($\sim1^{\circ}$) and low ($\sim0.1^{\circ}$) miscut angles, respectively. As expected, high miscut angle leads to suppression of multi-variant growth. By means of SQUID magnetometry, comparable relaxation effects were observed in both the multi-variant and the nearly single-variant sample. Differences in the magnetization reversal process were revealed by magnetic force microscopy. It showed that the multi-variant growth leads to higher density of defects acting as pinning or nucleation sites for magnetic domains, which consequently results in deterioration of magnetic properties. It was demonstrated that the use of high miscut substrate is important for fabrication of high quality SRO thin films with low density of crystallographic defects and excellent magnetic properties.

cond-mat.mtrl-sci↗

arXiv2019

Magneto-ionic control of spin polarization in magnetic tunnel junctions

Magnetic tunnel junctions (MTJs) with Hf0.5Zr0.5O2 barriers are reported to show both tunneling magnetoresistance effect (TMR) and tunneling electroresistance effect (TER), displaying four resistance states by magnetic and electric field switching. Here we show that, under electric field cycling of large enough magnitude, the TER can reach values as large as 10^6%. Moreover, concomitant with this TER enhancement, the devices develop electrical control of spin polarization, with sign reversal of the TMR effect. Currently, this intermediate state exists for a limited number of cycles and understanding the origin of these phenomena is key to improve its stability. The experiments presented here point to the magneto-ionic effect as the origin of the large TER and strong magneto-electric coupling, showing that ferroelectric polarization switching of the tunnel barrier is not the main contribution.

cond-mat.mtrl-sci↗

arXiv2019

Magnetic tunnel junctions based on ferroelectric Hf0.5Zr0.5O2 tunnel barriers

A ferroelectric tunnel barrier in between two ferromagnetic electrodes (multiferroic tunnel junction, MFTJ), is one of the most promising concepts for future microelectronic devices. In parallel, Hafnia based ferroelectrics are showing great potential for device miniaturization down to the nanoscale. Here we utilize ferroelectric Hf0.5Zr0.5O2 (HZO) with thickness of only 2 nm, epitaxially grown on La0.7Sr0.3MnO3 (LSMO) ferromagnetic electrodes, as a large band-gap insulating barrier integrated in MFTJs with cobalt top electrodes. As previously reported for other MFTJs with similar electrodes, the tunneling magnetoresistance (TMR) can be tuned and its sign can even be reversed by the bias voltage across the junction. We demonstrate four non-volatile resistance states generated by magnetic and electric field switching with high reproducibility in this system.

physics.app-ph↗

arXiv2018

Gate-tunable superconductivity at SrTiO3 surface realized by Al layer evaporation

Electronic properties of low dimensional superconductors are determined by many-body-effects. This physics has been studied traditionally with superconducting thin films, and in recent times with two-dimensional electron gases (2DEGs) at oxide interfaces. In this work, we show that a superconducting 2DEG can be generated by simply evaporating a thin layer of metallic Al under ultra-high vacuum on a SrTiO3 crystal, whereby Al oxidizes into amorphous insulating alumina, doping the SrTiO3 surface with oxygen vacancies. The superconducting critical temperature of the resulting 2DEG is found to be tunable with a gate voltage with a maximum value of 360 mK. A gate-induced switching between superconducting and resistive states is demonstrated. Compared to conventionally-used pulsed-laser deposition (PLD), our work simplifies to a large extent the process of fabricating oxide-based superconducting 2DEGs. It will make such systems accessible to a broad range of experimental techniques useful to understand low-dimensional phase transitions and complex many-body-phenomena in electronic systems.

cond-mat.supr-con↗

arXiv2018

Non-linear impedance spectroscopy applied to thermoelectric measurements: beyond the ZT estimation

Thermoelectric measurement of the dimensionless zT parameter requires multiple physical quantities to be measured, therefore there is great interest to find an experimental setup capable of measuring all these properties at once. Previous works on impedance spectroscopy have shown promising results in this direction, however, this technique does not lead to a complete characterization of the thermoelectric system without additional measurement. In order to extend impedance spectroscopy, we have investigated the measurement of the non-linear harmonic response of a Peltier device. The experiments are analyzed using an analytic model obtained by solving the heat equation in the frequency regime. Our work shows that fitting the experimental response of the system in the harmonic regime can lead to a complete characterization of the thermoelectric properties without the need of additional measurement.

physics.app-ph↗

arXiv2018

A rhombohedral ferroelectric phase in epitaxially-strained Hf0.5Zr0.5O2 thin films

After decades of searching for robust nanoscale ferroelectricity that could enable integration into the next generation memory and logic devices, hafnia-based thin films have appeared as the ultimate candidate because their ferroelectric (FE) polarization becomes more robust as the size is reduced. This exposes a new kind of ferroelectricity, whose mechanism still needs to be understood. Towards this end, thin films with increased crystal quality are needed. We report the epitaxial growth of Hf0.5Zr0.5O2 (HZO) thin films on (001)-oriented La0.7Sr0.3MnO3/SrTiO3 (STO) substrates. The films, which are under epitaxial compressive strain and are predominantly (111)-oriented, display large FE polarization values up to 34 μC/cm2 and do not need wake-up cycling. Structural characterization reveals a rhombohedral phase, different from the commonly reported polar orthorhombic phase. This unexpected finding allows us to propose a compelling model for the formation of the FE phase. In addition, these results point towards nanoparticles of simple oxides as a vastly unexplored class of nanoscale ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2017

True nature of the Curzon-Ahlborn efficiency

The Curzon-Ahlborn efficiency has long served as the definite upper bound for the thermal efficiency at maximum output power, and has thus shaped the development of finite-time thermodynamics. In this paper, we repeal the ruling consensus according to which it has a genuine universal character that can be derived from linear irreversible thermodynamics. We demonstrate that the Curzon-Ahlborn efficiency should instead properly be associated with a particular case of nonlinear heat engines, and we derive a generalized expression for the efficiency at maximum power beyond the restrictive case of linear models.

cond-mat.stat-mech↗

arXiv2015

Continuity and boundary conditions in thermodynamics: From Carnot's efficiency to efficiencies at maximum power

[...] By the beginning of the 20th century, the principles of thermodynamics were summarized into the so-called four laws, which were, as it turns out, definitive negative answers to the doomed quests for perpetual motion machines. As a matter of fact, one result of Sadi Carnot's work was precisely that the heat-to-work conversion process is fundamentally limited; as such, it is considered as a first version of the second law of thermodynamics. Although it was derived from Carnot's unrealistic model, the upper bound on the thermodynamic conversion efficiency, known as the Carnot efficiency, became a paradigm as the next target after the failure of the perpetual motion ideal. In the 1950's, Jacques Yvon published a conference paper containing the necessary ingredients for a new class of models, and even a formula, not so different from that of Carnot's efficiency, which later would become the new efficiency reference. Yvon's first analysis [...] went fairly unnoticed for twenty years, until Frank Curzon and Boye Ahlborn published their pedagogical paper about the effect of finite heat transfer on output power limitation and their derivation of the efficiency at maximum power, now known as the Curzon-Ahlborn (CA) efficiency. The notion of finite rate explicitly introduced time in thermodynamics, and its significance cannot be overlooked as shown by the wealth of works devoted to what is now known as finite-time thermodynamics since the end of the 1970's. [...] The object of the article is thus to cover some of the milestones of thermodynamics, and show through the illustrative case of thermoelectric generators, our model heat engine, that the shift from Carnot's efficiency to efficiencies at maximum power explains itself naturally as one considers continuity and boundary conditions carefully [...].

physics.hist-ph↗

arXiv2013

On the efficiency at maximum cooling power

The efficiency at maximum power (EMP) of heat engines operating as generators is one corner stone of finite-time thermodynamics, the Curzon-Ahlborn efficiency $η_{\rm CA}$ being considered as a universal upper bound. Yet, no valid counterpart to $η_{\rm CA}$ has been derived for the efficiency at maximum cooling power (EMCP) for heat engines operating as refrigerators. In this Letter we analyse the reasons of the failure to obtain such a bound and we demonstrate that, despite the introduction of several optimisation criteria, the maximum cooling power condition should be considered as the genuine equivalent of maximum power condition in the finite-time thermodynamics frame. We then propose and discuss an analytic expression for the EMCP in the specific case of exoreversible refrigerators.

cond-mat.stat-mech↗

arXiv2013

From local force-flux relationships to internal dissipations and their impact on heat engine performance: The illustrative case of a thermoelectric generator

We present an in-depth analysis of the sometimes understated role of the principle of energy conservation in linear irreversible thermodynamics. Our case study is that of a thermoelectric generator (TEG), which is a heat engine of choice in irreversible thermodynamics, owing to the coupling between the electrical and heat fluxes. We show why Onsager's reciprocal relations must be considered locally and how internal dissipative processes emerge from the extension of these relations to a global scale: the linear behavior of a heat engine at the local scale is associated with a dissipation process that must partake in the global energy balance. We discuss the consequences of internal dissipations on the so-called efficiency at maximum power, in the light of our comparative analyses of exoreversibility and endoreversibility on the one hand, and of two classes of heat engines, autonomous and periodically-driven, on the other hand. Finally, basing our analysis on energy conservation, we also discuss recent works which claim the possibility to overcome the traditional boundaries on efficiency imposed by finite-time thermodynamics in thermoelectric systems with broken time-reversal symmetry; this we do by introducing a "thermal" thermopower and an "electrical" thermopower which permits an analysis of the thermoelectric response of the TEG considering a possible dissymmetry between the electrical/thermal and the thermal/electrical couplings.

cond-mat.stat-mech↗