arXiv subjects

N. Gauquelin

Publications and source records attributed to N. Gauquelin.

17 recordsLinked to original sources

arXiv2025

Tunable and Persistent Macroscopic Polarization in Nominally Centrosymmetric Defective Oxides

Introducing symmetry breaking in materials enables the emergence of functionalities. This can be microscopically and macroscopically driven by applying external stimuli such as mechanical stress, electric field, temperature, and chemical modification. For instance, non-zero net dipole moments are formed in a material with the presence of local charged defects or their clusters, which can alter the crystal structure, charge states, and electrostatic potential across the material. Here, we demonstrate a conceptual approach to defects-mediated symmetry breaking that allows for built-in polarization in a centrosymmetric oxide, $\mathrm{Gd}_x\mathrm{Ce}_{1-x}\mathrm{O}_{2-δ}$ (CGO) films, via creating a macroscopic charge asymmetry. Our results show that switchable and enduring polarization in CGO films is governed by the redistribution of oxygen vacancies. This leads to notable and persistent pyroelectric effects with coefficient of approximately 180 $μ\mathrm{C}\cdot\mathrm{m}^{-2}\cdot\mathrm{K}^{-1}$. Our findings highlight the potential to develop high-performance, sustainable, environmentally friendly polar film materials by manipulating ionic defects from their centrosymmetric ground states. This approach provides new opportunities to expand polar materials in current and future energy and electronic applications.

cond-mat.mtrl-sci↗

arXiv2022

Alternating superconducting and charge density wave monolayers within bulk 6R-TaS2

Van der Waals (vdW) heterostructures continue to attract intense interest as a route of designing materials with novel properties that cannot be found in naturally occurring materials. Unfortunately, this approach is currently limited to only a few layers that can be stacked on top of each other. Here we report a bulk material consisting of superconducting monolayers interlayered with monolayers displaying charge density waves (CDW). This bulk vdW heterostructure is created by phase transition of 1T-TaS2 to 6R at 800 °C in an inert atmosphere. Electron microscopy analysis directly shows the presence of alternating 1T and 1H monolayers within the resulting bulk 6R phase. Its superconducting transition (Tc) is found at 2.6 K, exceeding the Tc of the bulk 2H phase of TaS2. The superconducting temperature can be further increased to 3.6 K by exfoliating 6R-TaS2 and then restacking its layers. Using first-principles calculations, we argue that the coexistence of superconductivity and CDW within 6R-TaS2 stems from amalgamation of the properties of adjacent 1H and 1T monolayers, where the former dominates the superconducting state and the latter the CDW behavior.

cond-mat.supr-con↗

arXiv2022

Induced Giant Piezoelectricity in Centrosymmetric Oxides

Piezoelectrics are materials that linearly deform in response to an applied electric field. As a fundamental prerequisite, piezoelectric material must possess a non centrosymmetric crystal structure. For more than a century, this remains the major obstacle for finding new piezoelectric materials. We circumvent this limitation by breaking the crystallographic symmetry, and inducing large and sustainable piezoelectric effects in centrosymmetric materials by electric field induced rearrangement of oxygen vacancies Surprisingly, the results show the generation of extraordinarily large piezoelectric responses d33 ~200,000 pm/V), in cubic fluorite Gd-doped CeO2-x films, which is two orders of magnitude larger than in the presently best known lead based piezoelectric relaxor ferroelectric oxide. These findings open opportunities to design new piezoelectric materials from environmentally friendly centrosymmetric ones.

cond-mat.mtrl-sci↗

arXiv2021

On the resistance minimum in LaAlO$_3$/Eu$_{1-x}$La$_x$TiO$_3$/SrTiO$_3$ heterostructures

In this paper we study LaAlO$_3$/Eu$_{1-x}$La$_x$TiO$_3$/SrTiO$_3$ structures with nominally x = 0, 0.1 and different thicknesses of the Eu$_{1-x}$La$_x$TiO$_3$ layer. We observe that both systems have many properties similar to previously studied LaAlO$_3$/EuTiO$_3$/SrTiO$_3$ and other oxide interfaces, such as the formation of a 2D electron liquid for 1 or 2 unit cells of Eu$_{1-x}$La$_x$TiO$_3$; a metal-insulator transition driven by the thickness increase of Eu$_{1-x}$La$_x$TiO$_3$ layer; the presence of an Anomalous Hall effect (AHE) when driving the systems above the Lifshitz point with a backgate voltage; and a minimum in the temperature dependence of the sheet resistance below the Lifshitz point in the one-band regime, which becomes more pronounced with increasing gate voltage. However, and notwithstanding the likely presence of magnetism in the system, we do not attribute that minimum to the Kondo effect, but rather to the properties of SrTiO$_3$ crystal and the inevitable effects of charge trapping when using back gates.

cond-mat.str-el↗

arXiv2021

Coupling charge and topological reconstructions at polar oxide interfaces

In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion-symmetry across the heterointerfaces. A notable example is the interface between polar and non-polar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way to the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wavefunctions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO$_3$, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO$_3$, a polar wide-bandgap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO$_2$/SrO interface configuration, leading to excess charge being pinned near the LaAlO$_3$/SrRuO$_3$ interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction modifies the momentum-space Berry curvature in SrRuO$_3$, driving a reorganization of the topological charges in the band structure. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces.

cond-mat.str-el↗

arXiv2021

Optical versus electron diffraction imaging of Twist-angle in 2D transition metal dichalcogenide bilayer superlattices

Atomically thin two-dimensional (2D) materials can be vertically stacked with van der Waals bonds, which enable interlayer coupling. In the particular case of transition metal dichalcogenide (TMD) bilayers, the relative direction between the two monolayers, coined as twist-angle, modifies the crystal symmetry and creates a superlattice with exciting properties. Here, we demonstrate an all-optical method for pixel-by-pixel mapping of the twist-angle with resolution of 0.23 degrees, via polarization-resolved second harmonic generation (P-SHG) microscopy and we compare it with four-dimensional scanning transmission electron microscopy (4D-STEM). It is found that the twist-angle imaging of WS2 bilayers, using the P-SHG technique is in excellent agreement with that obtained using electron diffraction. The main advantages of the optical approach are that the characterization is performed on the same substrate that the device is created on and that it is three orders of magnitude faster than the 4D-STEM. We envisage that the optical P-SHG imaging could become the gold standard for the quality examination of TMD superlattice-based devices.

cond-mat.mtrl-sci↗

arXiv2020

Wide field of view crystal orientation mapping of layered materials

Layered materials (LMs) are at the centre of an ever increasing research effort due to their potential use in a variety of applications. The presence of imperfections, such as bi- or multilayer areas, holes, grain boundaries, isotropic and anisotropic deformations, etc. are detrimental for most (opto)electronic applications. Here, we present a set-up able to transform a conventional scanning electron microscope into a tool for structural analysis of a wide range of LMs. An hybrid pixel electron detector below the sample makes it possible to record two dimensional (2d) diffraction patterns for every probe position on the sample surface (2d), in transmission mode, thus performing a 2d+2d=4d STEM (scanning transmission electron microscopy) analysis. This offers a field of view up to 2 mm2, while providing spatial resolution in the nm range, enabling the collection of statistical data on grain size, relative orientation angle, bilayer stacking, strain, etc. which can be mined through automated open-source data analysis software. We demonstrate this approach by analyzing a variety of LMs, such as mono- and multi-layer graphene, graphene oxide and MoS2, showing the ability of this method to characterize them in the tens of nm to mm scale. This wide field of view range and the resulting statistical information are key for large scale applications of LMs.

physics.app-ph↗

arXiv2020

Inhomogeneous superconductivity and quasilinear magnetoresistance at amorphous LaTiO3/SrTiO3 interfaces

We have studied the transport properties of LaTiO3/SrTiO3 (LTO/STO) heterostructures. In spite of 2D growth observed in reflection high energy electron diffraction, Transmission Electron Microscopy images revealed that the samples tend to amorphize. Still, we observe that the structures are conducting, and some of them exhibit high conductance and/or superconductivity. We established that conductivity arises mainly on the STO side of the interface, and shows all the signs of the 2-dimensional electron gas usually observed at interfaces between SrTiO3 and LaTiO3 or LaAlO3, including the presence of two electron bands and tunability with a gate voltage. Analysis of magnetoresistance (MR) and superconductivity indicates presence of a spatial fluctuations of the electronic properties in our samples. That can explain the observed quasilinear out-of-plane MR, as well as various features of the in-plane MR and the observed superconductivity.

cond-mat.mes-hall↗

arXiv2020

Gate-tuned Anomalous Hall Effect Driven by Rashba Splitting in Intermixed LaAlO3/GdTiO3/SrTiO3

The Anomalous Hall Effect (AHE) is an important quantity in determining the properties and understanding the behavior of the two-dimensional electron system forming at the interface of SrTiO3-based oxide heterostructures. The occurrence of AHE is often interpreted as a signature of ferromagnetism, but it is becoming more and more clear that also paramagnets may contribute to AHE. We studied the influence of magnetic ions by measuring intermixed LaAlO3/GdTiO3/SrTiO3 at temperatures below 10 K. We find that, as function of gate voltage, the system undergoes a Lifshitz transition, while at the same time an onset of AHE is observed. However, we do not observe clear signs of ferromagnetism. We argue the AHE to be due to the change in Rashba spin-orbit coupling at the Lifshitz transition and conclude that also paramagnetic moments which are easily polarizable at low temperatures and high magnetic filds lead to the presence of AHE, which needs to be taken into account when extracting carrier densities and mobilities.

cond-mat.mtrl-sci↗

arXiv2019

Efficient charge modulation in ultrathin LaAlO$_3$-SrTiO$_3$ field-effect transistors

At the LaAlO$_3$-SrTiO$_3$ interface, electronic phase transitions can be triggered by modulation of the charge carrier density, making this system an excellent prospect for the realization of versatile electronic devices. Here, we report repeatable transistor operation in locally gated LaAlO$_3$-SrTiO$_3$ field-effect devices of which the LaAlO$_3$ dielectric is only four unit cells thin, the critical thickness for conduction at this interface. This extremely thin dielectric allows a very efficient charge modulation of ${\sim}3.2\times10^{13}$ cm$^{-2}$ within a gate-voltage window of $\pm1$ V, as extracted from capacitance-voltage measurements. These also reveal a large stray capacitance between gate and source, presenting a complication for nanoscale device operation. Despite the small LaAlO$_3$ thickness, we observe a negligible gate leakage current, which we ascribe to the extension of the conducting states into the SrTiO$_3$ substrate.

cond-mat.mes-hall↗

arXiv2018

Berry phase engineering at oxide interfaces

Geometric phases in condensed matter play a central role in topological transport phenomena such as the quantum, spin and anomalous Hall effect (AHE). In contrast to the quantum Hall effect - which is characterized by a topological invariant and robust against perturbations - the AHE depends on the Berry curvature of occupied bands at the Fermi level and is therefore highly sensitive to subtle changes in the band structure. A unique platform for its manipulation is provided by transition metal oxide heterostructures, where engineering of emergent electrodynamics becomes possible at atomically sharp interfaces. We demonstrate that the Berry curvature and its corresponding vector potential can be manipulated by interface engineering of the correlated itinerant ferromagnet SrRuO$_3$ (SRO). Measurements of the AHE reveal the presence of two interface-tunable spin-polarized conduction channels. Using theoretical calculations, we show that the tunability of the AHE at SRO interfaces arises from the competition between two topologically non-trivial bands. Our results demonstrate how reconstructions at oxide interfaces can be used to control emergent electrodynamics on a nanometer-scale, opening new routes towards spintronics and topological electronics.

cond-mat.str-el↗

arXiv2018

Synthesis of high-oxidation Y-Ba-Cu-O phases in superoxygenated thin films

It is known that solid-state reaction in high-pressure oxygen can stabilize high-oxidation phases of Y-Ba-Cu-O superconductors in powder form. We extend this superoxygenation concept of synthesis to thin films which, due to their large surface-to-volume ratio, are more reactive thermodynamically. Epitaxial thin films of $\rm{YBa_2Cu_3O_{7-δ}}$ grown by pulsed laser deposition are annealed at up to 700 atm O$_2$ and 900$^\circ$C, in conjunction with Cu enrichment by solid-state diffusion. The films show clear formation of $\rm{Y_2Ba_4Cu_7O_{15-δ}}$ and $\rm{Y_2Ba_4Cu_8O_{16}}$ as well as regions of $\rm{YBa_2Cu_5O_{9-δ}}$ and YBa$_2$Cu$_6$O$_{10-δ}$ phases, according to scanning transmission electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. Similarly annealed $\rm{YBa_2Cu_3O_{7-δ}}$ powders show no phase conversion. Our results demonstrate a novel route of synthesis towards discovering more complex phases of cuprates and other superconducting oxides.

cond-mat.supr-con↗

arXiv2017

Formation of a conducting LaAlO$_3$ / SrTiO$_3$ interface studied by low energy electron reflection during growth

The two-dimensional electron gas occurring between the band insulators SrTiO$_3$ and LaAlO$_3$ continues to attract considerable interest, due to the possibility of dynamic control over the carrier density, and the ensuing phenomena such as magnetism and superconductivity. The formation of this conducting interface is sensitive to the growth conditions, but despite numerous investigations, there are still questions about the details of the physics involved. In particular, not much is known about the electronic structure of the growing LaAlO$_3$ layer at the growth temperature (around 800 $^o$C) in oxygen (pressure around $5\times 10^{-5}$ mbar), since analysis techniques at these conditions are not readily available. We developed a pulsed laser deposition system inside a low-energy electron microscope in order to study this issue. The setup allows for layer-by-layer growth control and in-situ measurements of the angle-dependent electron reflection intensity, which can be used as a fingerprint of the electronic structure of the surface layers during growth. By using different substrate terminations and growth conditions we observe two families of reflectivity maps, which we can connect either to samples with an AlO$_2$-rich surface and a conducting interface; or to samples with a LaO-rich surface and an insulating interface. Our observations emphasize that substrate termination and stoichiometry determine the electronic structure of the growing layer, and thereby the conductance of the interface.

cond-mat.mtrl-sci↗

arXiv2017

Spin-orbit semimetal SrIrO$_3$ in the two-dimensional limit

We investigate the thickness-dependent electronic structure of ultrathin SrIrO$_3$ and discover a transition from a semimetallic to a correlated insulating state below 4 unit cells. Low-temperature magnetoconductance measurements show that spin fluctuations in the semimetallic state are significantly enhanced while approaching the transition point. The electronic structure is further studied by scanning tunneling spectroscopy, showing that 4 unit cells SrIrO$_3$ is on the verge of a gap opening. Our density functional theory calculations reproduce the critical thickness of the transition and show that the opening of a gap in ultrathin SrIrO$_3$ is accompanied by antiferromagnetic order.

cond-mat.str-el↗

arXiv2015

Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces via charge transfer induced modulation doping

The discovery of two-dimensional electron gases (2DEGs) at the interface between two insulating complex oxides, such as LaAlO3 (LAO) or gamma-Al2O3 (GAO) epitaxially grown on SrTiO3 (STO) 1,2, provides an opportunity for developing all-oxide electronic devices3,4. These 2DEGs at complex oxide interfaces involve many-body interactions and give rise to a rich set of phenomena5, for example, superconductivity6, magnetism7,8, tunable metal-insulator transitions9, and phase separation10. However, large enhancement of the interfacial electron mobility remains a major and long-standing challenge for fundamental as well as applied research of complex oxides11-15. Here, we inserted a single unit cell insulating layer of polar La1-xSrxMnO3 (x=0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 created at room temperature. We find that the electron mobility of the interfacial 2DEG is enhanced by more than two orders of magnitude. Our in-situ and resonant x-ray spectroscopic in addition to transmission electron microscopy results indicate that the manganite layer undergoes unambiguous electronic reconstruction and leads to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits clear Shubnikov-de Haas oscillations and the initial manifestation of the quantum Hall effect, demonstrating an unprecedented high-mobility and low electron density oxide 2DEG system. These findings open new avenues for oxide electronics.

cond-mat.str-el↗

arXiv2014

Atomic resolution mapping of phonon excitations in STEM-EELS experiments

Atomically resolved electron energy-loss spectroscopy experiments are commonplace in modern aberrationcorrected transmission electron microscopes. Energy resolution has also been increasing steadily with the continuous improvement of electron monochromators. Electronic excitations however are known to be delocalised due to the long range interaction of the charged accelerated electrons with the electrons in a sample. This has made several scientists question the value of combined high spatial and energy resolution for mapping interband transitions and possibly phonon excitation in crystals. In this paper we demonstrate experimentally that atomic resolution information is indeed available at very low energy losses around 100 meV expressed as a modulation of the broadening of the zero loss peak. Careful data analysis allows us to get a glimpse of what are likely phonon excitations with both an energy loss and gain part. These experiments confirm recent theoretical predictions on the strong localisation of phonon excitations as opposed to electronic excitations and show that a combination of atomic resolution and recent developments in increased energy resolution will offer great benefit for mapping phonon modes in real space.

cond-mat.mtrl-sci↗

arXiv2013

Attenuation of superconductivity in manganite/cuprate heterostructures by epitaxially-induced CuO intergrowths

We examine the effect of CuO intergrowths on the superconductivity in epitaxial La_{2/3}Ca_{1/3}MnO_3/YBa_2Cu_3O_{7-δ} (LCMO/YBCO) thin-film heterostructures. Scanning transmission electron microscopy on bilayer LCMO/YBCO thin films revealed double CuO-chain intergrowths which form regions with the 247 lattice structure in the YBCO layer. These nanoscale 247 regions do not appear in x-ray diffraction, but can physically account for the reduced critical temperature Tc of bilayer thin films relative to unilayer films with the same YBCO thickness, at least down to ~25 nm. We attribute the CuO intergrowths to the bilayer heteroepitaxial mismatch and the Tc reduction to the generally lower Tc seen in bulk 247 samples. These epitaxially-induced CuO intergrowths provide a microstructural mechanism for the attenuation of superconductivity in LCMO/YBCO heterostructures.

cond-mat.supr-con↗