arXiv subjects

Pierre-Eymeric Janolin

Publications and source records attributed to Pierre-Eymeric Janolin.

14 recordsLinked to original sources

arXiv2026

Consistent transition model for Bi0.5Na0.5TiO3 from temperature-dependent structural and electrical properties

BNT based solid solutions are promising parent materials for lead free dielectric capacitors, thanks to their high recoverable energy densities and breakdown strengths. However, the ambient temperature symmetry and high temperature phase evolution of BNT remain unclear. Crucially, structural transformations and electrical ordering are most often considered independently, hindering a coherent understanding of the BNT phase transition. In this work, we combine X ray diffraction, transmission electron microscopy, Raman spectroscopy, impedance spectroscopy, and high field polarization cycling to establish a unified picture of the structural and dielectric response of BNT. Based on these results, we propose a consistent transition model for BNT that reconciles previously conflicting interpretations. This integrated structure property study provides a rationale for developing high performance, lead free energy storage materials.

cond-mat.mtrl-sci↗

arXiv2026

Giant photostriction in lead-free ferroelectric stemming from photo-excited thermalized carriers

Ferroelectrics are polar materials whose polarization can be switched by applying electric fields; they offer unique opportunities to develop performant photostrictive materials, i.e., materials that can deform under visible light illumination. Naturally devoid of inversion symmetry, they exhibit original photogalvanic effects such as the Bulk Photovoltaic Effect, which relies on ``hot'' photoexcited carriers. It has long been thought that the electric field generated by this effect may couple to the natural piezoelectric abilities of ferroelectrics to provide large photoinduced deformations. However, due to competing effects, such as thermal dilatation, deformation potential, polarization, or depolarizing-field screening by \textit{thermalized} carriers, it remains unclear which microscopic phenomena govern the photoinduced deformations in classical ferroelectric materials. Here, we demonstrate the largest photoinduced deformation measured in a ferroelectric thin film. Reaching 1 %, this giant photostriction likely originates from the contribution of thermalized photoinduced carriers.

cond-mat.mtrl-sci↗

arXiv2025

Characteristic ferroelectric domains and their dynamic behavior in ordered Pb(Sc$_{1/2}$Nb$_{1/2}$)O$_{3}$

Pb-based perovskites with multiple cations are fascinating materials showing various phenomena such as high piezoelectric, electromechanical, and relaxor properties. While chemical disordering accompanied by polar nanoregions and nanosized domains is commonly believed to cause the relaxor nature, little is known about ferroelectric microstructures of chemically ordered Pb-based perovskites. In this study, we discovered intriguing meandering ferroelectric domains in chemically ordered ferroelectric Pb(Sc$_{1/2}$Nb$_{1/2}$)O$_{3}$ using in-situ transmission electron microscopy with dark-field imaging. Observation results demonstrate that electric polarization can fluctuate around the [111] direction despite the formation of long-range ordered rhombohedral domains, which results in unique weak relaxor properties. In-situ imaging upon heating successfully reveals the dynamic behavior of domain-wall movements with lattice distortion and paraelectric-ferroelectric phase coexistence in the vicinity of the Curie temperature, indicating a discontinuous phase transition. Our research provides new insights into the effect of chemical ordering on ferroelectric nanodomains.

cond-mat.mtrl-sci↗

arXiv2024

Origin of the Apparent Electric-Field Dependence of Electrostrictive Coefficients

Electrostrictive materials exhibit a strain that is proportional to the square of the induced polarization. In linear dielectrics where the permittivity is constant, this electromechanical strain is also proportional to the square of the electric field. However, under increasing amplitudes of the driving field, the electromechanical strain sometimes saturates; the electrostrictive coefficients therefore appear to depend on the amplitude of the electric field used to measure them. Here, we present a methodology showing that this apparent field dependence is a consequence of neglecting higher-order electromechanical phenomena. When these are taken into account, not only do the electrostrictive coefficients remain constant but the signs of the high-order coefficients enable the prediction of the saturation behavior from a single measurement. We illustrate this approach on both classical and non-classical (so-called ``giant'') electrostrictors.

cond-mat.mtrl-sci↗

arXiv2022

A new look at the temperature-dependent properties of the antiferroelectric model PbZrO3: an effective Hamiltonian study

A novel atomistic effective Hamiltonian scheme, incorporating an original and simple bilinear energetic coupling, is developed and used to investigate the temperature dependent physical properties of the prototype antiferroelectric PbZrO3 (PZO) system. This scheme reproduces very well the known experimental hallmarks of the complex Pbam orthorhombic phase at low temperatures and the cubic paraelectric state of Pm 3m symmetry at high temperatures. Unexpectedly, it further predicts a novel intermediate state also of Pbam symmetry, but in which anti-phase oxygen octahedral tiltings have vanished with respect to the Pbam ground state. Interestingly, such new state exhibits a large dielectric response and thermal expansion that remarkably agree with previous experimental observations and the x-ray experiments we performed. We also conducted direct first-principles calculations at 0K which further support such low energy phase. Within this fresh framework, a re-examination of the properties of PZO is thus called for.

cond-mat.mtrl-sci↗

arXiv2022

Generalized relation between electromechanical responses at fixed voltage and fixed electric field

We present a general relation between the electromechanical couplings of infinitesimal strain and electric field to arbitrary order, measured at fixed voltage and at fixed electric field. We show that the improper response at fixed field can be written as the strain derivative of the $n^{\text{th}}$ order susceptibility tensor, and the proper response at fixed voltage drop can be written as the response at fixed field plus corrections for dilations and 90$^{\circ}$ rotations induced by strain. Our theory correctly reproduces the proper piezoelectric response and we go beyond with the electrostrictive response. We present first-principles calculations of the improper electrostrictive response at fixed field, and illustrate how the correction is used to obtain the proper response at fixed voltage. This distinction is of high importance given the recent interest in giant electrostrictors exhibiting electromechanical responses as large as the piezoelectric ones.

cond-mat.mtrl-sci↗

arXiv2022

Divergent electrostriction at ferroelectric phase transitions: example of strain-induced ferroelectiricty in KTaO3

We investigate the electrostrictive response across a ferroelectric phase transition from first-principles calculations and refute the prevailing view of constant electrostriction across the ferroelectric phase boundary. We take as a case study the epitaxial strain-induced transition from para- to feroelectricity of \ce{KTaO3}. We show that the magnitude of the electrostriction diverges with the permitivity at the transition, hence exhibiting giant responses through a calculation of both the M and Q electrostrictive tensors. We explain the origin of this giant electrostrictive response in \ce{KTaO3} using a microscopic decomposition of the electrostriction coefficients, and use this understanding to propose design rules for the development of future giant electrostrictors for electromechanical applications. Finally, we introduce a further means to calculate electrostriction, specific to ferroelectrics, and not yet utilised in the literature.

cond-mat.mtrl-sci↗

arXiv2022

Direct observation of monoclinic polar nanoregions in the relaxor ferroelectric Pb(Yb$_{1/2}$Nb$_{1/2}$)O$_{3}$-PbTiO$_{3}$

Relaxor ferroelectrics are applied in electronic devices such as actuators and sonars. Morphotrophic phase boundaries (MPBs) with monoclinic structures are known for their high piezoelectricity and electromechanical coupling factors in solid solutions of PbTiO$_{3}$ and relaxor ferroelectrics (Pb(Mg$_{1/3}$, Nb$_{2/3}$)O$_{3}$ or Pb(Zn$_{1/3}$, Nb$_{1/3}$)O$_{3}$). However, the monoclinic structures related to polar nanosize domains (polar nanoregions) exhibiting the relaxor properties of dielectric dispersion have not been reported. Using transmission electron microscopy and synchrotron x-ray scattering, we present the first observations of coexisting monoclinic structures and polar nanoregions near the MPB in Pb(Yb$_{1/2}$Nb$_{1/2}$)O$_{3}$-PbTiO$_{3}$. The polar nanoregions in this material are randomly shaped, unlike the ferroelectric nanodomains of the canonical relaxor Pb(Mg$_{1/3}$, Nb$_{1/3}$)O$_{3}$-PbTiO$_{1/3}$. Furthermore, in situ observations reveal that the monoclinic polar nanoregions grow as the temperature decreases. A pair-distribution function analysis reveals a mixture of monoclinic Pm and Cm structures in the polar nanoregions without the rhombohedral structure of other Pb-based relaxor solid solutions. Owing to the peculiar nature of the coexistence of the relaxor property (polar nanoregions) and high piezoelectricity (monoclinic structure), this material is expected as a new platform for understanding relaxor ferroelectricity.

cond-mat.mtrl-sci↗

arXiv2022

Defining "Giant" Electrostriction

The recent discovery of giant electrostrictors has re-ignited the interest in electrostriction, an electromechanical coupling existing in all dielectrics but overshadowed by its linear counterpart: piezoelectricity. In this review, after a reminder of classical electrostriction, we propose a definition of giant electrostriction based on two empirical relations (Newnam relation and one we propose). From this definition, we review previous reports on giant electrostrictors, to assess their nature. Focusing on the ones satisfying our definition, we compare their performances and characteristics. We also identify some of the hurdles to their adoption in the wide range of electromechanical applications, despite their fundamental and applicative interests.

cond-mat.mtrl-sci↗

arXiv2021

Optimized methodology for the calculation of electrostriction from first-principles

In this work we present a new method for the calculation of the electrostrictive properties of materials using density functional theory. The method relies on the thermodynamical equivalence, in a dielectric, of the quadratic mechanical responses (stress or strain) to applied electric stimulus (electric or polarisation fields) to the strain or stress dependence of its dielectric susceptibility or stiffness tensors. Comparing with current finite-field methodologies for the calculation of electrostriction, we demonstrate that our presented methodology offers significant advantages of efficiency, robustness, and ease of use. These advantages render tractable the highthroughput theoretical investigation into the largely unknown electrostrictive properties of materials.

cond-mat.mtrl-sci↗

arXiv2012

Synthesis dependent characteristics of Sr1-xMnxTiO3 (x=0.03, 0.05, 0.07 and 0.09)

Sr1-xMnxTiO3 (where x = 0.03, 0.05, 0.07 and 0.09) was synthesized via different routes that include solid-state, oxalate precipitation and freeze drying. In oxalate precipitation technique, compositions corresponding to 3 and 5 mol % doping of Mn were monophasic whereas the higher compositions revealed the presence of the secondary phases such as MnO, Mn3O4 etc., as confirmed by high resolution X-ray diffraction (XRD) studies. The decomposition behavior of the precursors prepared using oxalate precipitation method corresponding to the above mentioned compositions was studied. Nanopowders of compositions pertaining to 5 to 9 mol % of Mn doping were obtained using freeze-drying technique. The average crystallite size of these nanopowders was found to be in the 35 to 65 nm range. The microstructural studies carried out on the sintered ceramics, fabricated using powders synthesized by different routes established the fine grained nature (< 1 microm) of the one obtained by freeze drying method. Raman scattering studies were carried out in order to complement the observations made from XRD regarding the phase purity. The dielectric properties of the ceramics obtained by different synthesis routes were studied in the 80 - 300 K temperature range at 100 kHz and the effect of grain size has been discussed.

cond-mat.mtrl-sci↗

arXiv2012

Giant direct magnetoelectric effect in strained multiferroic heterostructures

The direct magnetoelectric (ME) effect mediated by lattice strains induced in a ferroelectric film by a ferromagnetic substrate is evaluated using first-principles-based calculations. To that end, the strain sensitivity of ferroelectric polarization and the film permittivity are calculated as a function of the in-plane biaxial strain for Pb(Zr0.52Ti0.48)O3 films under various depolarizing fields. It is found that the ME voltage coefficient varies nonmonotonically with this strain and may reach giant values exceeding 100 Vcm-1 Oe-1 over a strain range that can be controlled through the electrical boundary conditions.

cond-mat.mtrl-sci↗

arXiv2007

Partial decoupling between strain and polarization in mono-oriented Pb(Zr0.2Ti0.8)O3 thin film

The structural evolution of epitaxial mono-oriented (i.e. with the c-axis perpendicular to the interface) ferroelectric Pb(Zr0.2,Ti0.8)O3 thin film has been investigated, using high resolution, temperature dependent, X-ray diffraction. The full set of lattice parameters was obtained, it allowed to estimate the variation of the polarization as a function of temperature, underlying the difference between the polarization-induced tetragonality and the elastic one. The temperature evolution of the misfit strain has been calculated and found to be in good agreement with the theoretical temperature-misfit strain phase diagram

cond-mat.mtrl-sci↗

arXiv2007

Domain structure sequence in ferroelectric Pb(Zr0.2Ti0.8)O3 thin film on MgO

The structural evolution of a polydomain ferroelectric Pb(Zr0.2Ti0.8)O3 film was studied by temperature dependent X-ray diffraction. Two critical temperatures were evidenced: T*=740K, corresponding to a change in the domain structure (a/c/a/c to a1/a2/a1/a2), and Tc_film = 825K where the film undergoes a ferroelectricparaelectric phase transition. The films remains tetragonal on the whole range of temperature investigated. The evolutions of the domain structure and lattice parameters were found to be in very good agreement with the calculated domain stability map and theoretical temperature-misfit strain phase diagram respectively.

cond-mat.mtrl-sci↗