arXiv subjects

D. Rubi

Publications and source records attributed to D. Rubi.

At least 19 recordsLinked to original sources

arXiv2026

Tuning the memristive response of TaO$_x$-based devices with Ag Nanoparticles

Defect engineering is a key strategy to control resistive switching (RS) in oxide-based memristive devices, where oxygen vacancy (OV) dynamics governs filament formation and rupture. We investigate the effect of Ag nanoparticles (AgNPs) embedded in the top electrode of Pt/Ta2O5/TaO2/Pt memristors and analyze their RS behavior and statistical stability. Devices without AgNPs exhibit two hysteresis switching loops (HSLs) with opposite chiralities, originating from the participation of the Pt/Ta2O5 top interface and the Ta2O5/TaO2 bottom interface. Incorporating AgNPs reduces the overall device resistance and selectively suppresses one loop, yielding a single, well-defined switching mode. Moreover, devices incorporating Ag-NPs show markedly reduced cycle-to-cycle variability of the high-resistance state, as confirmed by Weibull analysis, indicating improved endurance and switching reproducibility. Within a filamentary RS framework, we attribute this behavior to local metallization of the top interface by AgNPs, which partially inhibit OV transport and confines the RS dynamics to the bottom interface. Numerical simulations with the Oxygen Vacancy Resistive Network (OVRN) model succesfully reproduce the experimental HSLs, statistical trends, and tunable ON/OFF ratios with AgNPs coverage. These findings demonstrate that targeted interface metallization via metallic nanoparticles provides an effective route to control multi-interface RS dynamics and improve switching stability in without modifying the oxide architecture.

cond-mat.mes-hall↗

arXiv2024

On the origin of filamentary resistive switching in oxides-based memristive devices

The control and manipulation of filamentary resistive switching (FRS) is essential for practical applications in fields like non-volatile memories and neuromorphic computing. However, key aspects of the dynamics of conductive filament formation and their influence on device resistance remain incompletely understood. In this work we study FRS in binary oxides based memristors by investigating the dynamics of oxygen vacancies (OV) on a two dimensional lattice and their role in forming low-resistance paths that facilitate the transition between high and low global resistance states. We reveal that the mere formation of an OV percolation path is insufficient to induce a transition to a low-resistance state. Instead, an OV concentration exceeding a critical threshold across all sites in the filament is required to generate a low-resistivity conducting path. Furthermore, we simulate the impact of static defects -which block OV migration and would correspond to voids in real porous samples-, on filament formation. We show that there is a range of defect density values where OV percolate through the sample, leading to the formation of OV filaments, but conductive paths remain absent. Additionally, a small concentration of defects can reduce the final value of the low-resistance state, thereby increasing the ON-OFF ratio. These findings provide valuable insights into optimizing defective nanomaterials with memristive properties, which are crucial for advancing in-memory and neuromorphic computing technologies.

cond-mat.mes-hall↗

arXiv2024

Oxygen vacancies kinetics in $TaO_{2-h}$/$Ta_{2}$$O_{5-x}$ memristive interfaces

Oxygen vacancies (OV) are pervasive in metal oxides and play a pivotal role in the switching behaviour of oxide-based memristive devices. In this work we address, through a combination of experiments and theoretical simulations, OV dynamics in $Pt/TaO_{2-h}/Ta_{2}O_{5-x}/TaO_${2-y}$/Pt$ devices. In particular, we focus on the RESET transition (from low to high resistance), induced by the application of electrical pulse(s), by choosing different initial OV profiles and studying their kinetics during the mentioned process. We demonstrate that by selecting specific OV profiles it is possible to tune the characteristic time-scale of the RESET. Finally, we show that the implementation of gradual RESETs, induced by applying many (small) successive pulses, allows estimating the activation energies involved in the OV electromigration process. Our results help paving the way for OV engineering aiming at optimizing key memristive figures such as switching speed or power consumption, which are highly relevant for neuromorphic or in-memory computing implementations.

cond-mat.mes-hall↗

arXiv2024

Memristive response and neuromorphic functionality of polycrystalline ferroelectric Ca:HfO$_{2}$-based devices

Memristors are considered key building blocks for the development of neuromorphic computing hardware. For ferroelectric memristors with a capacitor-like structure, the polarization direction modulates the height of the Schottky barriers -- present at ferroelectric/metal interfaces -- that control the device resistance. Here, we unveil the coexistence of multiple memristive mechanisms in Pt/Ca:HfO$_2$/Pt devices fabricated on silicon by a simple and effective low-toxicity chemical solution method. Depending on the fabrication conditions, either dielectric or ferroelectric devices are obtained, each one presenting a distinct memristive response. The devices are forming-free and can sustain ferroelectric switching and memristive behavior simultaneously. Aided by numerical simulations, we describe this behavior as a competition of different mechanisms, including the effect of the ferroelectric polarization on Schottky interfaces and oxygen vacancy electromigration. Finally, we propose a simple learning algorithm for time-series recognition, designed to take advantage of the resistance relaxations present in the case of the ferroelectric devices.

physics.app-ph↗

arXiv2022

Coexistance of volatile and non-volatile memristive effects in phase-separated La$_{0.5}$Ca$_{0.5}$MnO$_{3}$-based devices

In this work, we have investigated the coexistance of volatile and non-volatile memristive effects in epitaxial phase-separated La$_{\text{0.5}}$Ca$_{\text{0.5}}$MnO$_{3}$ thin films. At low temperatures (50 K), we observed volatile resistive changes arising from self-heating effects in the vicinity of a metal-to-insulator transition. At higher temperatures (140 K and 200 K) we measured a combination of volatile and non-volatile effects arising from the synergy between self-heating effects and ferromagnetic-metallic phase growth induced by an external electrical field. The results reported here add phase separated manganites to the list of materials which can electrically mimic, on the same device, the behavior of both neurons and synapses, a feature that might be useful for the development of neuromorphic computing hardware

cond-mat.mtrl-sci↗

arXiv2021

Optimization of the multi-mem response of topotactic redox La$_{1/2}$Sr$_{1/2}$Mn$_{1/2}$Co$_{1/2}$O$_{3-x}$

Memristive systems emerge as strong candidates for the implementation of Resistive Random Access Memories (RRAM) and neuromorphic computing devices, as they can mimic the electrical analog behavior or biological synapses. In addition, complementary functionalities such as memcapacitance could significantly improve the performance of bio-inspired devices in key issues such as energy consumption. However, the physics of mem-systems is not fully understood so far, hampering their large-scale implementation in devices. Perovskites that undergo topotactic transitions and redox reactions show improved performance as mem-systems, compared to standard perovskites. In this paper we analyze different strategies to optimize the multi-mem behavior (memristive and memcapacitive) of topotactic redox La$_{1/2}$Sr$_{1/2}$Mn$_{1/2}$Co$_{1/2}$O$_{3-x}$ (LSMCO) films grown on Nb:SrTiO$_3$ (NSTO). We explored devices with different crystallinity (from amorphous to epitaxial LSMCO), out-of-plane orientation ((001) and (110)) and stimulated either with voltage or current pulses. We found that an optimum memory response is found for epitaxial (110) LSMCO stimulated with current pulses. Under these conditions, the system efficiently exchanges oxygen with the environment minimizing, at the same time, self-heating effects that trigger nanostructural and chemical changes which could affect the device integrity and performance. Our work contributes to pave the way for the integration of LSMCO-based devices in cross-bar arrays, in order to exploit their memristive and memcapacitive properties for the development of neuromorphic or in-memory computing devices

cond-mat.mtrl-sci↗

arXiv2021

Polarons formation in Bi-deficient BaBiO$_3$

BaBiO$_3$ is a charged ordered Peierls-like perovskite well known for its superconducting properties upon K or Pb doping. We present a study on the transport and electronic properties of BaBiO$_3$ perovskite with strong Bi-deficiency. We show that it is possible to synthesize BaBiO$_3$ thin layers with Bi-vacancies above 8-10% by depositing an yttrium-stabilized zirconia capping layer. By combining transport measurements with ab initio calculations we propose an scenario where the Bi-vacancies give rise to the formation of polarons and suggest that the electrical transport is dominated by the migration of these polarons trapped at Bi$^{3+}$ sites. Our work shows that cation vacancies engineering -- hardly explored to date -- appears as a promising pathway to tune the electronic and functional properties of perovskites.

cond-mat.other↗

arXiv2020

On the key role of oxygen vacancies electromigration in the memristive response of ferroelectric devices

Ferroelectric memristors are intensively studied due to their potential implementation in data storage and processing devices. In this work we show that the memristive behavior of metal/ferroelectric oxide/metal devices relies on the competition of two effects: the modulation of metal/ferroelectric interface barriers by the switchable ferroelectric polarization and the electromigration of oxygen vacancies, with the depolarizing field playing a fundamental role in the latter. We simulate our experimental results with a phenomenological model that includes both effects and we reproduce several non-trivial features of the electrical response, including resistance relaxations observed after external poling. Besides providing insight into the underlying physics of these complex devices, our work suggests that it is possible to combine non-volatile and volatile resistive changes in single ferroelectric memristors, an issue that could be useful for the development of neuromorphic devices.

physics.app-ph↗

arXiv2019

Electric selective activation of memristive interfaces in TaO$_x$-based devices

The development of novel devices for neuromorphic computing and non-traditional logic operations largely relies on the fabrication of well controlled memristive systems with functionalities beyond standard bipolar behavior and digital ON-OFF states. In the present work we demonstrate for Ta$_2$O$_5$-based devices that it is possible to selectively activate/deactivate two series memristive interfaces in order to obtain clockwise or counter-clockwise multilevel squared remanent resistance loops, just by controlling the (a)symmetry of the applied stimuli and independently of the nature of the used metallic electrodes. Based on our thorough characterization, analysis and modeling, we show that the physical origin of this electrical behavior relies on controlled oxygen vacancies electromigration between three different zones of the active Ta$_2$O$_{5-x}$ layer: a central -- bulk -- one and two quasi-symmetric interfaces with reduced TaO$_{2-h(y)}$ layers. Our devices fabrication process is rather simple as it implies the room temperature deposition of only one CMOS compatible oxide -- Ta-oxide -- and one metal, suggesting that it might be possible to take advantage of these properties at low cost and with easy scability. The tunable opposite remanent resistance loops circulations with multiple -- analogic -- intermediate stable states allows mimicking the adaptable synaptic weight of biological systems and presents potential for non-standard logic devices.

physics.app-ph↗

arXiv2019

Large memcapacitance and memristance at Nb:SrTiO$_{3}$ / La$_{0.5}$Sr$_{0.5}$Mn$_{0.5}$Co$_{0.5}$O$_{3-\delta}$ Topotactic Redox Interface

The possibility to develop neuromorphic computing devices able to mimic the extraordinary data processing capabilities of biological systems spurs the research on memristive systems. Memristors with additional functionalities such as robust memcapacitance can outperform standard devices in key aspects such as power consumption or miniaturization possibilities. In this work, we demonstrate a large memcapacitive response of a perovskite memristive interface, using the topotactic redox ability of La$_{0.5}$Sr$_{0.5}$Mn$_{0.5}$Co$_{0.5}$O$_{3-\delta}$ (LSMCO, 0 $\leq$ $\delta$ $\leq$ 0.62). We demonstrate that the multi-mem behaviour originates at the switchable n-p diode formed at the Nb:SrTiO3/LSMCO interface. We found for our Nb:SrTiO$_{3}$/LSMCO/Pt devices a memcapacitive effect C$_{HIGH}$/C$_{LOW}$ ~ 100 at 150 kHz. The proof-of-concept interface reported here opens a promising venue to use topotactic redox materials for disruptive nanoelectronics, with straightforward applications in neuromorphic computing technology.

physics.app-ph↗

arXiv2016

Origin of multistate resistive switching in Ti/manganite/Si$O_x$/Si heterostructures

We report on the growth and characterization of Ti/$La_{1/3}$$Ca_{2/3}$Mn$O_3$/Si$O_x$/n-Si memristive devices. We demonstrate that using current as electrical stimulus unveils an intermediate resistance state, in addition to the usual high and low resistance states that are observed in standard voltage controlled experiments. Based on thorough electrical characterization (impedance spectroscopy, current-voltage curves analysis), we disclose the contribution of three different microscopic regions of the device to the transport properties: an ohmic incomplete metallic filament, a thin manganite layer below the filament tip exhibiting Poole-Frenkel like conduction, and the SiOx layer with an electrical response well characterized by a Child-Langmuir law. Our results suggest that the existence of the SiOx layer plays a key role in the stabilization of the intermediate resistance level, indicating that the combination of two or more active RS oxides adds functionalities in relation to single-oxide devices. We understand that these multilevel devices are interesting and promising as their fabrication procedure is rather simple and they are fully compatible with standard Si-based electronics.

cond-mat.mtrl-sci↗

arXiv2016

Manganite-based three level memristive devices with self-healing capability

We report on non-volatile memory devices based on multifunctional manganites. The electric field induced resistive switching of Ti/$La_{1/3}$$Ca_{2/3}$Mn$O_3$/n-Si devices is explored using different measurement protocols. We show that using current as the electrical stimulus (instead of standard voltage-controlled protocols) improves the electrical performance of our devices and unveils an intermediate resistance state. We observe three discrete resistance levels (low, intermediate and high), which can be set either by the application of current-voltage ramps or by means of single pulses. These states exhibit retention and endurance capabilities exceeding $10^4$ s and 70 cycles, respectively. We rationalize our experimental observations by proposing a mixed scenario were a metallic filament and a Si$O_x$ layer coexist, accounting for the observed resistive switching. Overall electrode area dependence and temperature dependent resistance measurements support our scenario. After device failure takes place, the system can be turned functional again by heating up to low temperature (120 C), a feature that could be exploited for the design of memristive devices with self-healing functionality. These results give insight into the existence of multiple resistive switching mechanisms in manganite-based memristive systems and provide strategies for controlling them.

cond-mat.mtrl-sci↗

arXiv2009

Epitaxial TbMnO3 thin films on SrTiO3 substrates: A structural study

TbMnO$_{3}$ films have been grown under compressive strain on (001)-oriented SrTiO$_{3}$ crystals. They have an orthorhombic structure and display the (001) orientation. With increasing thickness, the structure evolves from a more symmetric (tetragonal) to a less symmetric (bulk-like orthorhombic) structure, while keeping constant the in-plane compression thereby leaving the out-of-plane lattice spacing unchanged. The domain microstructure of the films is also revealed, showing an increasing number of orthorhombic domains as the thickness is decreased: we directly observe ferroelastic domains as narrow as 4nm. The high density of domain walls may explain the induced ferromagnetism observed in the films, while both the decreased anisotropy and the small size of the domains could account for the absence of a ferroelectric spin spiral phase.

cond-mat.mtrl-sci↗

arXiv2008

Ferromagnetism and increased ionicity in epitaxially grown TbMnO3 films

Thin films of TbMnO3 have been grown on SrTiO3 substrates. The films grow under compressive strain and are only partially clamped to the substrate. This produces remarkable changes in the magnetic properties and, unlike the bulk material, the films display ferromagnetic interactions below the ordering temperature of ~40K. X-ray photoemission measurements in the films show that the Mn-3s splitting is 0.3eV larger than that of the bulk. Ab initio embedded cluster calculations yield Mn-3s splittings that are in agreement with the experiment and reveal that the larger observed values are due to a larger ionicity of the films.

cond-mat.mtrl-sci↗

arXiv2008

Growth of flat SrRuO3(111) thin films suitable as bottom electrodes in heterostructures

Thin film growth of ferroelectric or multiferroic materials on SrTiO3(111) with a buffer electrode has been hampered by the difficulty of growing flat electrodes on this polar orientation. We report on the growth and characterization of SrRuO3 thin films deposited by pulsed laser deposition on SrTiO3(111). We show that our SrRuO3(111) films are epitaxial and display magnetic bulk-like properties. Films presenting a thickness between 20 and 30nm are found to be very flat (with an RMS of about 0.5 nm) and therefore suitable as bottom electrodes in heterostructures.

cond-mat.mtrl-sci↗

arXiv2008

Magnetic and dielectric properties of YbMnO3 perovskite thin films

Metastable manganite perovskites displaying the antiferromagnetic so-called E-phase are predicted to be multiferroic. Due to the need of high-pressures for the synthesis of this phase, this prediction has only been confirmed in bulk HoMnO3. Here we report on the growth and characterization of YbMnO3 perovskite thin films grown under epitaxial strain. Highly-oriented thin films, with thickness down to ~30nm, can be obtained showing magneto-dielectric coupling and magnetic responses as those expected for the E-phase. We observe that the magnetic properties depart from the bulk behavior only in the case of ultrathin films (d< 30nm), which display a glassy magnetic behavior. We show that strain effects alone cannot account for this difference and that the film morphology plays, instead, a crucial role.

cond-mat.mtrl-sci↗

arXiv2007

Reversible Ferromagnetic Switching in Zno:(Co,Mn) Powders

We report here on the magnetic properties of ZnO:Mn and ZnO:Co doped nanoparticles. We have found that the ferromagnetism of ZnO:Mn can be switched on and off by consecutive low-temperature annealings in O2 and N2 respectively, while the opposite phenomenology was observed for ZnO:Co. These results suggest that different defects (presumably n-type for ZnO:Co and p-type for ZnO:Mn) are required to induce a ferromagnetic coupling in each case. We will argue that ferromagnetism is likely to be restricted to a very thin, nanometric layer, at the grain surface. These findings reveal and give insight into the dramatic relevance of surface effects for the occurrence of ferromagnetism in ZnO doped oxides.

cond-mat.mtrl-sci↗

arXiv2006

Structural and magnetic properties of ZnO:TM (TM: Co,Mn) nanopowders

We report on the structural and magnetic characterization of Co0.1Zn0.9O and Mn0.1Zn0.9O nanopowders obtained by a soft chemistry route. We show that those samples fired at low temperatures display a ferromagnetic interaction that can not be attributed to the presence of impurities. A magnetic aging mechanism is observed, reflecting the key role played by defects in the stabilization of ferromagnetism in this kind of diluted magnetic semiconductors.

cond-mat.mtrl-sci↗