arXiv subjects

Jean-Pierre Locquet

Publications and source records attributed to Jean-Pierre Locquet.

17 recordsLinked to original sources

arXiv2025

Sub-unit cell engineering of CrVO$_3$ superlattice thin films

Ordered corundum oxides introduce new prospects in the field of functional oxides thin films, complementing the more widely studied class of ABO$_3$ perovskites. In this work, we take advantage of the layer-by-layer growth regime to fabricate epitaxial CrVO$_3$ superlattice thin films with atomic-scale accuracy on the periodic arrangement of Cr and V layers. By means of X-ray diffraction, scanning transmission electron microscopy and Raman spectroscopy, we confirm the thickness control in the sub-unit cell scale, alternating 3, 2 or 1 single atomic layers of Cr$_2$O$_3$ and V$_2$O$_3$. For the first time, we stabilize the ilmenite phase of CrVO$_3$ (space group R-3) and compare the functional properties of the thin film with those calculated by density functional theory. This novel approach to the growth of ordered corundum oxides opens the path towards the stabilization of new complex oxides with tailored properties by varying the composition and the superlattice period, ultimately broadening the family of functional rhombohedral oxides.

cond-mat.mtrl-sci↗

arXiv2024

Mott resistive switching initiated by topological defects

Resistive switching is the fundamental process that triggers the sudden change of the electrical properties in solid-state devices under the action of intense electric fields. Despite its relevance for information processing, ultrafast electronics, neuromorphic devices, resistive memories and brain-inspired computation, the nature of the local stochastic fluctuations that drive the formation of metallic nuclei out of the insulating state has remained hidden. Here, using operando X-ray nano-imaging, we have captured the early-stages of resistive switching in a V2O3-based device under working conditions. V2O3 is a paradigmatic Mott material, which undergoes a first-order metal-to-insulator transition coupled to a lattice transformation that breaks the threefold rotational symmetry of the rhombohedral metal phase. We reveal a new class of volatile electronic switching triggered by nanoscale topological defects of the lattice order parameter of the insulating phase. Our results pave the way to the use of strain engineering approaches to manipulate topological defects and achieve the full control of the electronic Mott switching. The concept of topology-driven reversible electronic transition is of interest for a broad class of quantum materials, comprising transition metal oxides, chalcogenides and kagome metals, that exhibit first-order electronic transitions coupled to a symmetry-breaking order.

cond-mat.str-el↗

arXiv2023

Confinement-Induced Isosymmetric Metal-Insulator Transition in Ultrathin Epitaxial V2O3 Films

Dimensional confinement has shown to be an effective strategy to tune competing degrees of freedom in complex oxides. Here, we achieved atomic layered growth of trigonal vanadium sesquioxide (V2O3) by means of oxygen-assisted molecular beam epitaxy. This led to a series of high-quality epitaxial ultrathin V2O3 films down to unit cell thickness, enabling the study of the intrinsic electron correlations upon confinement. By electrical and optical measurements, we demonstrate a dimensional confinement-induced metal-insulator transition in these ultrathin films. We shed light on the Mott-Hubbard nature of this transition, revealing an abrupt vanishing of the quasiparticle weight as demonstrated by photoemission spectroscopy. Furthermore, we prove that dimensional confinement acts as an effective out-of-plane stress. This highlights the structural component of correlated oxides in a confined architecture, while opening an avenue to control both in-plane and out-of-plane lattice components by epitaxial strain and confinement, respectively.

cond-mat.mtrl-sci↗

arXiv2023

Coherent control of the orbital occupation driving the insulator-to-metal Mott transition in V$_2$O$_3$

Managing light-matter interactions on timescales faster than the loss of electronic coherence is key for achieving full quantum control of the final products in solid-solid transformations. In this work, we demonstrate coherent electronic control of the photoinduced insulator-to-metal transition in the prototypical Mott insulator V$_2$O$_3$. Selective excitation of a specific interband transition with two phase-locked light pulses manipulates the orbital occupation of the correlated bands in a way that depends on the coherent evolution of the photoinduced superposition of states. A comparison between experimental results and numerical solutions of the optical Bloch equations provides an electronic coherence time on the order of 5 fs. Temperature-dependent experiments suggest that the electronic coherence time is enhanced in the vicinity of the insulator-to-metal transition critical temperature, thus highlighting the role of fluctuations in determining the electronic coherence. These results open new routes to selectively switch the functionalities of quantum materials and coherently control solid-solid electronic transformations.

cond-mat.str-el↗

arXiv2022

Nanoscale self-organisation and metastable non-thermal metallicity in Mott insulators

Mott transitions in real materials are first order and almost always associated with lattice distortions, both features promoting the emergence of nanotextured phases. This nanoscale self-organization creates spatially inhomogeneous regions, which can host and protect transient non-thermal electronic and lattice states triggered by light excitation. Here, we combine time-resolved X-ray microscopy with a Landau-Ginzburg functional approach for calculating the strain and electronic real-space configurations. We investigate V$_2$O$_3$, the archetypal Mott insulator in which nanoscale self-organization already exists in the low-temperature monoclinic phase and strongly affects the transition towards the high-temperature corundum metallic phase. Our joint experimental-theoretical approach uncovers a remarkable out-of-equilibrium phenomenon: the photo-induced stabilisation of the long sought monoclinic metal phase, which is absent at equilibrium and in homogeneous materials, but emerges as a metastable state solely when light excitation is combined with the underlying nanotexture of the monoclinic lattice.

cond-mat.str-el↗

arXiv2022

On the origin of supertetragonality in BaTiO$_3$

Understanding ferroelectricity is of both fundamental and technological importance to further stimulate the development of new materials designs and manipulations. Here, we perform an in-depth first-principle study on the well-known ferroelectric barium titanate BaTiO$_{3}$ under a hydrostatic negative pressure, showing an isosymmetric phase transition to a supertetragonal phase with high $c/a$ ratio of $\sim1.3$. The microscopic origin and driving mechanisms of this phase transition are identified as a drastic change of the covalently $π$-bonded electrons. These findings provide guidance in the search for new supertetragonal phases, with great opportunities for novel multiferroic materials; and can be generalized in the understanding of other isosymmetric phase transitions.

cond-mat.mtrl-sci↗

arXiv2021

An efficient direct band-gap transition in germanium by three-dimensional strain

Complementary to the development of highly three-dimensional (3D) integrated circuits in the continuation of Moore's law, there has been a growing interest in new 3D deformation strategies to improve device performance. To continue this search for new 3D deformation techniques, it is essential to explore beforehand - using computational predictive methods - which strain tensor leads to the desired properties. In this work, we study germanium (Ge) under an isotropic 3D strain on the basis of first-principle methods. The transport and optical properties are studied by a fully ab initio Boltzmann transport equation and many-body Bethe-Salpeter equation (BSE) approach, respectively. Our findings show that a direct band gap in Ge could be realized with only 0.34% triaxial tensile strain (negative pressure) and without the challenges associated with Sn doping. At the same time a significant increase in refractive index and carrier mobility - particularly for electrons - is observed. These results demonstrate that there is a huge potential in exploring the 3D deformation space for semiconductors - and potentially many other materials - in order to optimize their properties.

cond-mat.mtrl-sci↗

arXiv2021

Two-dimensional honeycomb-kagome V2O3: a robust room-temperature magnetic Chern insulator interfaced with graphene

The possibility of dissipationless chiral edge states without the need of an external magnetic field in the quantum anomalous Hall effect (QAHE) offers a great potential in electronic/spintronic applications. The biggest hurdle for the realization of a room-temperature magnetic Chern insulator is to find a structurally stable material with a sufficiently large energy gap and Curie temperature that can be easily implemented in electronic devices. This work based on first-principle methods shows that a single atomic layer of V2O3 with honeycomb-kagome (HK) lattice is structurally stable with a spin-polarized Dirac cone which gives rise to a room-temperature QAHE by the existence of an atomic on-site spin-orbit coupling (SOC). Moreover, by a strain and substrate study, it was found that the quantum anomalous Hall system is robust against small deformations and can be supported by a graphene substrate.

cond-mat.mes-hall↗

arXiv2021

Non-thermal light-assisted resistance collapse in a V$_2$O$_3$-based Mott-insulator device

The insulator-to-metal transition in Mott insulators is the key mechanism for a novel class of electronic devices, belonging to the Mottronics family. Intense research efforts are currently devoted to the development of specific control protocols, usually based on the application of voltage, strain, pressure and light excitation. The ultimate goal is to achieve the complete control of the electronic phase transformation, with dramatic impact on the performance, for example, of resistive switching devices. Here, we investigate the simultaneous effect of external voltage and excitation by ultrashort light pulses on a single Mottronic device based on a V$_2$O$_3$ epitaxial thin film. The experimental results, supported by finite-element simulations of the thermal problem, demonstrate that the combination of light excitation and external electrical bias drives a volatile resistivity drop which goes beyond the combined effect of laser and Joule heating. Our results impact on the development of protocols for the non-thermal control of the resistive switching transition in correlated materials.

cond-mat.str-el↗

arXiv2021

Quarter-filled Kane-Mele Hubbard model: Dirac half-metals

Recent experimental success in the realization of two-dimensional (2D) magnetism has stimulated the search for new magnetic 2D materials with strong magnetic anisotropy and high Curie temperature. One promising subgroup of 2D magnetic systems are Dirac half-metals (DHM) which have gained a lot of interest recently, as they host a high-temperature quantum anomalous Hall effect (QAHE). This article discusses predictions for intrinsic DHMs and identifies them as realizations of the Kane-Mele Hubbard model at quarter filling. This proposed unification contributes to a firmer understanding of these materials and suggests pathways for the discovery of new DHM systems.

cond-mat.str-el↗

arXiv2020

Temporal dynamics of all-optical switching in hybrid VO2/Si waveguides

Vanadium dioxide (VO2) is one of the most promising materials for developing hybrid photonic integrated devices (PICs). However, despite switching times as low as a few femtoseconds have been reported, the all-optical temporal dynamics of VO2 embedded in a waveguide using an in-plane optical signal remain still hidden. Here, we experimentally investigate this behavior in hybrid VO2/Si waveguides by using pump-probe measurements at telecom wavelengths. Our results show switching times in the micro and nanosecond range, suggesting that the phase transition is triggered thermally from the light absorbed by the VO2 and the temporal response is governed by thermal conductive dynamics. By properly engineering the optical pulse, we prospect switching times of nanoseconds with an energy consumption of a few nanojoules. Our results unveil a new temporal dynamic that would be useful for developing future all-optical VO2 photonic integrated devices.

physics.optics↗

arXiv2019

Early-stage dynamics of metallic droplets embedded in the nanotextured Mott insulating phase of V$_2$O$_3$

Unveiling the physics that governs the intertwining between the nanoscale self-organization and the dynamics of insulator-to-metal transitions (\textit{IMT}) is key for controlling on demand the ultrafast switching in strongly correlated materials and nano-devices. A paradigmatic case is the \textit{IMT} in V$_2$O$_3$, for which the mechanism that leads to the nucleation and growth of metallic nano-droplets out of the supposedly homogeneous Mott insulating phase is still a mystery. Here, we combine X-ray photoemission electron microscopy and ultrafast non-equilibrium optical spectroscopy to investigate the early stage dynamics of isolated metallic nano-droplets across the \textit{IMT} in V$_2$O$_3$ thin films. Our experiments show that the low-temperature monoclinic antiferromagnetic insulating phase is characterized by the spontaneous formation of striped polydomains, with different lattice distortions. The insulating domain boundaries accommodate the birth of metallic nano-droplets, whose non-equilibrium expansion can be triggered by the photo-induced change of the 3$d$-orbital occupation. We address the relation between the spontaneous nanotexture of the Mott insulating phase in V$_2$O$_3$ and the timescale of the metallic seeds growth. We speculate that the photoinduced metallic growth can proceed along a non-thermal pathway in which the monoclinic lattice symmetry of the insulating phase is partially retained.

cond-mat.str-el↗

arXiv2018

Ultrafast orbital manipulation and Mott physics in multi-band correlated materials

Multiorbital correlated materials are often on the verge of multiple electronic phases (metallic, insulating, super- conducting, charge and orbitally ordered), which can be explored and controlled by small changes of the external parameters. The use of ultrashort light pulses as a mean to transiently modify the band population is leading to fundamentally new results. In this paper we will review recent advances in the field and we will discuss the pos- sibility of manipulating the orbital polarization in correlated multi-band solid state systems. This technique can provide new understanding of the ground state properties of many interesting classes of quantum materials and offers a new tool to induce transient emergent properties with no counterpart at equilibrium. We will address: the discovery of high-energy Mottness in superconducting copper oxides and its impact on our understanding of the cuprate phase diagram; the instability of the Mott insulating phase in photoexcited vanadium oxides; the manipulation of orbital-selective correlations in iron-based superconductors; the pumping of local electronic excitons and the consequent transient effective quasiparticle cooling in alkali-doped fullerides. Finally, we will discuss a novel route to manipulate the orbital polarization in a a k-resolved fashion.

cond-mat.str-el↗

arXiv2015

Collapse of the low temperature insulating state in Cr-doped V$_2$O$_3$ thin films

We have grown epitaxial Cr-doped V$_2$O$_3$ thin films with Cr concentrations between $0$ and $20\%$ on $(0001)$-Al$_2$O$_3$ by oxygen-assisted molecular beam epitaxy. For the highly doped samples (> $3\%$), a regular and monotonous increase of the resistance with decreasing temperature is measured. Strikingly, in the low doping samples (between $1\%$ and $3\%$), a collapse of the insulating state is observed with a reduction of the low temperature resistivity by up to 5 orders of magnitude. A vacuum annealing at high temperature of the films recovers the low temperature insulating state for doping levels below $3\%$ and increases the room temperature resistivity towards the values of Cr-doped V$_2$O$_3$ single crystals. It is well-know that oxygen excess stabilizes a metallic state in V$_2$O$_3$ single crystals. Hence, we propose that Cr doping promotes oxygen excess in our films during deposition leading to the collapse of the low temperature insulating state at low Cr concentrations. These results suggest that slightly Cr-doped V$_2$O$_3$ films can be interesting candidates for field effect devices.

cond-mat.str-el↗

arXiv2015

An electric-field driven Mott metal-insulator transition in correlated thin films: an inhomogeneous dynamical mean-field theory approach

Simulations are carried out based on the dynamical mean-field theory (DMFT) in order to investigate the properties of correlated thin films for various values of the chemical potential, temperature, interaction strength, and applied transverse electric field. Application of a sufficiently strong field to a thin film at half-filling leads to the appearance of conducting regions near the surfaces of the film, whereas in doped slabs the application of a field leads to a conductivity enhancement on one side of the film and a gradual transition to the insulating state on the opposite side. In addition to the inhomogeneous DMFT, an independent layer approximation (ILA) is considered, in which the properties of each layer are approximated by a homogeneous bulk environment. A comparison between the two approaches reveals that the less expensive ILA results are in good agreement with the DMFT approach, except close to the metal-to-insulator transition points and in the layers immediately at the film surfaces. The hysteretic behavior (memory effect) characteristic of the bulk doping driven Mott transition persists in the slab.

cond-mat.str-el↗

arXiv2013

The Continuous-Pole-Expansion method to obtain spectra of electronic lattice models

We present a new algorithm to analytically continue the self-energy of quantum many-body systems from Matsubara frequencies to the real axis. The method allows straightforward, unambiguous computation of electronic spectra for lattice models of strongly correlated systems from self-energy data that has been collected with state-of-the are continuous time solvers within dynamical mean field simulations. Using well-known analytical properties of the self-energy, the analytic continuation is cast into a constrained minimization problem that can be formulated as a quadratic programmable optimization with linear constraints. The algorithm is validated against exactly solvable finite size problems, showing that all features of the spectral function near the Femi level are very well reproduced and coarse features are reproduced for all energies. The method is applied to two well known lattice problems, the two-dimensional Hubbard model at half filling where the momentum dependence of the gap formation is studied, as well as a multi-band model of NiO, for which the spectral function can be directly compared to experiment. Agreement with results published results is very good.

cond-mat.str-el↗

arXiv1999

Normal State Resistivity of Underdoped YBa2Cu3Ox Thin Films and La2-xSrxCuO4 Ultra-Thin Films under Epitaxial Strain

The normal state resistivity of high temperature superconductors can be probed in the region below Tc by suppressing the superconducting state in high magnetic fields. Here we present the normal state properties of YBa2Cu3Ox thin films in the underdoped regime and the normal state resistance of La2-xSrxCuO4 thin films under epitaxial strain, measured below Tc by applying pulsed fields up to 60 T. A universal rho(T) behaviour is reported. We interpret these data in terms of the recently proposed 1D quantum transport model with the 1D paths corresponding to the charge stripes.

cond-mat.supr-con↗