arXiv subjects

Francisco Rivadulla

Publications and source records attributed to Francisco Rivadulla.

14 recordsLinked to original sources

arXiv2026

Boosting the Memory Window of Memristive Stacks via Engineered Interfaces with High Ionic Mobility

Realizing the potential of oxide-based memristive devices for high-density data storage and energy-efficient computing still relies on overcoming key technical challenges, including the need for a larger number of stable resistance states, faster switching speeds, lower SET/RESET voltages, improved endurance, and reduced variability. Addressing these limitations requires innovative material design strategies. Here, we demonstrate that introducing a thin layer of oxide-ion conductor SrCoO3-x between the metal and the SrTiO3-based memristive elements expands the number of distinguishable resistance states from about 8 to about 22. This modification also reduced the SET/RESET voltage by 50% and markedly improved device endurance, albeit with a trade-off of reduced state retention. To assess the performance of this architecture, we trained a two-layer fully connected neural network using the experimental SrTiO3/SrCoO3-x memristor characteristics on the MNIST handwritten digit dataset. Networks with hidden-layer sizes between 64 and 256 neurons achieved classification errors below 7%. Finally, we confirmed the transferability of this interface-engineering approach by applying it to HfOx-based devices, achieving a consistent enhancement in the resistive state window.

cond-mat.mtrl-sci↗

arXiv2026

Depth-Resolved Evolution of Buried Polar Topologies in a PbTiO3/SrTiO3 Superlattice

Polar topologies in complex oxides gives rise to a rich spectrum of emergent functionalities and are fundamentally governed by three-dimensional (3D) atomic structures. However, direct experimental determination of buried 3D polar configurations remains a longstanding challenge because conventional (scanning) transmission electron microscopy ((S)TEM) provides primarily projected structural information with limited depth sensitivity. Here, we combine depth-sectioning low-angle annular dark-field (LAADF) STEM, high-angle ADF (HAADF) STEM, and multislice electron ptychography (MEP) to directly visualize the depth-dependent atomic structure and polarization topology in a PTO/STO superlattice. Depth-sectioning STEM reveals pronounced focal-depth-dependent contrast variations and apparent splitting of Pb atomic columns, indicating significant structural heterogeneity along the beam direction. MEP reconstruction simultaneously resolves the Pb, Ti, and O sublattices with nanometer-scale depth resolution, enabling quantitative mapping of atomic displacements throughout the reconstructed volume. The resulting 3D atomic model reveals substantial depth-dependent displacements of Pb, Ti, and O atoms and a corresponding evolution of the polarization topology. Vortex-like polarization structures are observed near the specimen surfaces but become strongly suppressed within the interior, where distinct polarization configurations emerge. These findings show that polarization patterns observed in conventional projection images can arise from the superposition of multiple depth-dependent polar states and may obscure the underlying 3D polarization texture. Our findings establish a direct experimental link between local atomic displacements and depth-dependent polarization topology, opening new opportunities for investigating and engineering buried functional states in complex oxide nanostructures.

cond-mat.mtrl-sci↗

arXiv2026

Complex polar superstructure controlled thermal conductivity in ferroelectric PbTiO3/SrTiO3 superlattices

Integrating epitaxial thin films of ferroelectric PbTiO3 and paraelectric SrTiO3 into artificially layered periodic superlattices provides a unique platform for tuning strain, depolarization, and interfacial/surface energies, thereby accessing a rich phase diagram of topological polar structures (skyrmions, vortices, merons, or sinusoidal waves) and superstructures (polar supercrystals). Here we show that the 3D arrangement of polar vortices in a supercrystal suppresses thermal conductivity (k) of PTO/STO superlattices (SLs). The temperature dependence of k reflects the evolution of the polar superstructure, as determined by X-ray diffraction and transmission electron microscopy. The comparison with other SLs suggests that the 3D arrangement is crucial for controlling thermal conductivity beyond the usual interfacial scattering. Moreover, we observed an unexpected reduction in thermal conductivity with increasing superlattice thickness, a phenomenon reminiscent of phonon-wave Anderson localization. Our results show that complex polar superstructures can be useful active elements for modulating heat transport in technologies where control over heat dissipation is critical.

cond-mat.mtrl-sci↗

arXiv2025

van der Waals epitaxy of lead monoxide - PbO and application as a virtual substrate for oxide membranes

We report the successful growth of epitaxial layers of van der Waals (vdW) lead oxide (PbO) polymorphs on different substrates, via pulsed laser deposition. A thin layer of vdW $α$-PbO (~5 nm) was subsequently used as a virtual substrate to grow thin films of perovskites BaTiO$_3$, SrTiO$_3$, and the spinel CoFe$_2$O$_4$ with a crystal quality comparable to direct epitaxy on single-crystal oxide substrates. Notably, films with the larger lattice parameter underwent spontaneous, controlled spalling within days of growth, remaining structurally intact, or were easily exfoliated and transferred using the tape method. This work establishes PbO as a promising virtual substrate technology for the fabrication of free-standing oxide membranes through vdW epitaxy, offering advantages over conventional sacrificial layer methods.

cond-mat.mtrl-sci↗

arXiv2025

The coupling of polarization and oxygen vacancy migration in ferroelectric Hf0.5Zr0.5O2 thin films enables electrically controlled thermal memories above room temperature

Here we investigate epitaxial Hf0.5Zr0.5O2 ferroelectric thin films as potential candidates to be used as non-volatile electric-field-modulated thermal memories. The electric-field dependence of the thermal conductivity of metal/Hf0.5Zr0.5O2/YSZ devices is found to be hysteretic, resembling the polarization vs electric field hysteresis loops, being maximum (minimum) at large applied positive (negative) voltages from the top metallic electrode. This dynamic thermal response is compatible with the coupling between the ferroelectric polarization and the oxygen ion migration, in which the oxygen vacancies are the main phonon scattering sources and the polarization acts as an electrically active ion migration barrier that creates the hysteresis. This new mechanism enables two non-volatile thermal states: high (ON) and low (OFF) thermal conductivity, with an ON/OFF ratio of 1.6. Both the ON and OFF states exhibit high stability over time, though the switching speed is limited by ion mobility in the YSZ electrode.

cond-mat.mtrl-sci↗

arXiv2024

Resistive switching acceleration induced by thermal confinement

Enhancing the switching speed of oxide-based memristive devices at a low voltage level is crucial for their use as non-volatile memory and their integration into emerging computing paradigms such as neuromorphic computing. Efforts to accelerate the switching speed often result in an energy tradeoff, leading to an increase of the minimum working voltage. In our study, we present an innovative solution: the introduction of a low thermal conductivity layer placed within the active electrode, which impedes the dissipation of heat generated during the switching process. The result is a notable acceleration in the switching speed of the memristive model system SrTiO$_{3}$ by a remarkable factor of 10$^{3}$, while preserving the integrity of the switching layer and the interfaces with the electrodes, rendering it adaptable to various filamentary memristive systems. The incorporation of HfO$_{2}$ or TaO$_{x}$ as heat-blocking layers not only streamlines the fabrication process, but also ensures compatibility with complementary metal-oxide-semiconductor technology.

physics.app-ph↗

arXiv2023

Annealing effects on the magnetic and magnetotransport properties of iron oxide nanoparticles self-assemblies

In magnetic tunnel junctions based on iron oxide nanoparticles the disorder and the oxidation state of the surface spin as well as the nanoparticles functionalization play a crucial role in the magnetotransport properties. In this work, we report a systematic study of the effects of vacuum annealing on the structural, magnetic and transport properties of self-assembled ~10 nm Fe3O4 nanoparticles. The high temperature treatment (from 573 to 873 K) decomposes the organic coating into amorphous carbon, reducing the electrical resistivity of the assemblies by 4 orders of magnitude. At the same time, the 3Fe2+/(Fe3++Fe2+) ratio is reduced from 1.11 to 0.13 when the annealing temperature of the sample increases from 573 to 873 K, indicating an important surface oxidation. Although the 2 nm physical gap remains unchanged with the thermal treatment, a monotonous decrease of tunnel barrier width was obtained from the electron transport measurements when the annealing temperature increases, indicating an increment in the number of defects and hot-spots in the gap between the nanoparticles. This is reflected in the reduction of the spin dependent tunneling, which reduces the interparticle magnetoresistance. This work shows new insights about influence of the nanoparticle interfacial composition, as well their the spatial arrangement, on the tunnel transport of self-assemblies, and evidence the importance of optimizing the nanostructure fabrication for increasing the tunneling current without degrading the spin polarized current.

cond-mat.mtrl-sci↗

arXiv2023

Temperature and thickness dependence of the thermal conductivity in 2D ferromagnet Fe$_3$GeTe$_2$

The emergence of symmetry-breaking orders such as ferromagnetism and the weak interlayer bonding in van der Waals materials, offers a unique platform to engineer novel heterostructures and tune transport properties like thermal conductivity. Here, we report the experimental and theoretical study of the cross-plane thermal conductivity, $κ_\perp$, of the van der Waals 2D ferromagnet Fe$_3$GeTe$_2$. We observe a non-monotonic increase of $κ_\perp$ with the thickness and a large suppression in artificially-stacked layers, indicating a diffusive transport regime with ballistic contributions. These results are supported by the theoretical analyses of the accumulated thermal conductivity, which show an important contribution of phonons with mean free paths between 10 and 200 nm. Moreover, our experiments show a reduction of the $κ_\perp$ in the low-temperature ferromagnetic phase occurring at the magnetic transition. The calculations show that this reduction in $κ_\perp$ is associated with a decrease in the group velocities of the acoustic phonons and an increase in the phonon-phonon scattering of the Raman modes that couple to the magnetic phase. These results demonstrate the potential of van der Waals ferromagnets for thermal transport engineering.

cond-mat.mtrl-sci↗

arXiv2021

Electron-Phonon Coupling and Electron-Phonon Scattering in SrVO$_3$

Understanding the physics of strongly correlated electronic systems has been a central issue in condensed matter physics for decades. In transition metal oxides, strong correlations characteristic of narrow $d$ bands is at the origin of such remarkable properties as the Mott gap opening, enhanced effective mass, and anomalous vibronic coupling, to mention a few. SrVO$_3$, with V$^{4+}$ in a $3d^1$ electronic configuration is the simplest example of a 3D correlated metallic electronic system. Here, we focus on the observation of a (roughly) quadratic temperature dependence of the inverse electron mobility of this seemingly simple system, which is an intriguing property shared by other metallic oxides. The systematic analysis of electronic transport in SrVO$_3$ thin films discloses the limitations of the simplest picture of e-e correlations in a Fermi liquid; instead, we show that the quasi-2D topology of the Fermi surface and a strong electron-phonon coupling, contributing to dress carriers with a phonon cloud, play a pivotal role on the reported electron spectroscopic, optical, thermodynamic and transport data. The picture that emerges is not restricted to SrVO$_3$ but can be shared with other $3d$ and $4d$ metallic oxides.

cond-mat.str-el↗

arXiv2021

Deconvolution of phonon scattering by ferroelectric domain walls and point defects in a PbTiO3 thin film deposited in a composition-spread geometry

We present a detailed analysis of the temperature dependence of the thermal conductivity of a ferroelectric PbTiO3 thin film deposited in a composition-spread geometry enabling a continuous range of compositions from ~25% titanium-deficient to ~20% titanium-rich to be studied. By fitting the experimental results to the Debye model we deconvolve and quantify the two main phonon scattering sources in the system: ferroelectric domain walls (DWs) and point defects. Our results prove that ferroelectric DWs are the main agent limiting the thermal conductivity in this system, not only in the stoichiometric region of the thin film ([Pb]/[Ti]~1), but also when the concentration of cation point defects is significant (up to ~15%). Hence, DWs in ferroelectric materials are a source of phonon scattering at least as effective as point defects. Our results demonstrate the viability and effectiveness of using reconfigurable DWs to control the thermal conductivity in solid-state devices.

cond-mat.mtrl-sci↗

arXiv2020

Tunnel Magnetoresistance in Self-Assemblies of Exchange Coupled Core/Shell Nanoparticles

We report the precise control of tunneling magnetoresistance (TMR) in devices of self-assembled core/shell Fe$_3$O$_4$/Co$_{1-x}$Zn$_x$Fe$_2$O$_4$ nanoparticles ($0\leq x\leq 1$). Adjusting the magnetic anisotropy through the content of Co$^{2+}$ in the shell, provides an accurate tool to control the switching field between the bistable states of the TMR. In this way, different combinations of soft/hard and hard/soft core/shell configurations can be envisaged for optimizing devices with the required magnetotransport response.

cond-mat.mes-hall↗

arXiv2019

Tunable resistivity exponents in the metallic phase of epitaxial nickelates

We report a detailed analysis of the electrical resistivity exponent of thin films of NdNiO3 as a function of epitaxial strain. Strain-free thin-films show a linear dependence of the resistivity vs temperature, consistent with a classical Fermi gas ruled by electron-phonon interactions. In addition, the apparent temperature exponent, n, can be tuned with the epitaxial strain between n= 1 and n= 3. We discuss the critical role played by quenched random disorder in the value of n. Our work shows that the assignment of Fermi/Non-Fermi liquid behaviour based on experimentally obtained resistivity exponents requires an in-depth analysis of the degree of disorder in the material.

cond-mat.str-el↗

arXiv2018

Tuning oxygen vacancy diffusion through strain in SrTiO$_3$ thin films

Understanding the diffusion of oxygen vacancies in oxides under different external stimuli is crucial for the design of ion-based electronic devices, improve catalytic performance, etc. In this manuscript, using an external electric field produced by an AFM tip, we obtain the room-temperature diffusion coefficient of oxygen-vacancies in thin-films of SrTiO$_3$ under compressive/tensile epitaxial strain. Tensile strain produces a substantial increase of the diffusion coefficient, facilitating the mobility of vacancies through the film. Additionally, the effect of tip bias, pulse time, and temperature on the local concentration of vacancies is investigated. These are important parameters of control in the production and stabilization of non-volatile states in ion-based memresistive devices. Our findings show the key role played by strain for the control of oxygen vacancy migration in thin-film oxides.

cond-mat.mtrl-sci↗

arXiv2014

Anomalous and Planar Nernst effects in thin-films of half-metallic ferromagnet La2/3Sr1/3MnO3

We report the planar and anomalous Nernst effect in epitaxial thin films of spin polarized La2/3Sr1/3MnO3. The thermal counterpart of the anomalous Hall effect in this material (i.e. the anomalous Nernst effect) shows a extreme sensitivity to any parasitic thermal gradient, resulting in large asymmetric voltages under small temperature differences. This should be considered when interpreting the magnitude of the electrical response in nanostructures and devices that operate under high current densities. Finally, none of the observed magneto-thermoelectric signals is compatible with the observation of the Spin Seebeck Effect in this material.

cond-mat.mtrl-sci↗