arXiv subjects

B. Noheda

Publications and source records attributed to B. Noheda.

At least 19 recordsLinked to original sources

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↗

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

Patterning enhanced tetragonality in BiFeO3 thin films with effective negative pressure by helium implantation

Helium implantation in epitaxial thin films is a way to control the out-of-plane deformation independently from the in-plane strain controlled by epitaxy. In particular, implantation by means of a helium microscope allows for local implantation and patterning down to the nanometer resolution, which is of interest for device applications. We present here a study of bismuth ferrite (BiFeO3) films where strain was patterned locally by helium implantation. Our combined Raman, XRD and TEM study shows that the implantation causes an elongation of the BiFeO3 unit cell and ultimately a transition towards the so-called super-tetragonal polymorph via states with mixed phases. In addition, TEM reveals the onset of amorphization at a threshold dose that does not seem to impede the overall increase in tetragonality. The phase transition from the R-like to T-like BiFeO3 appears as first-order in character, with regions of phase coexistence and abrupt changes in lattice parameters.

cond-mat.mtrl-sci↗

arXiv2020

High pixel number deformable mirror concept utilizing piezoelectric hysteresis for stable shape configurations

We present the conceptual design and initial development of the Hysteretic Deformable Mirror (HDM). The HDM is a completely new approach to the design and operation of deformable mirrors for wavefront correction in advanced imaging systems. The key technology breakthrough is the application of highly hysteretic piezoelectric material in combination with a simple electrode layout to efficiently define single actuator pixels. The set-and-forget nature of the HDM, which is based on the large remnant deformation of the newly developed piezo material, facilitates the use of time division multiplexing (TDM) to address the single pixels without the need for high update frequencies to avoid pixel drift. This, in combination with the simple electrode layout, paves the way for upscaling to extremely high pixel numbers ($\geq 128\times 128$) and pixel density ($100/mm^2$) deformable mirrors (DMs), which is of great importance for high spatial frequency wavefront correction in some of the most advanced imaging systems in the world.

astro-ph.IM↗

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↗

arXiv2020

Electrical and acoustic self-oscillations in an epitaxial oxide for neuromorphic applications

Developing materials that can lead to compact versions of artificial neurons (neuristors) and synapses (memristors) is the main aspiration of the nascent neuromorphic materials research field. Oscillating circuits are interesting as neuristors, emulating the firing of action potentials. We present room-temperature self-oscillating devices fabricated from epitaxial thin films of semiconducting TbMnO3. We show that these electrical oscillations induce concomitant mechanical oscillations that produce audible sound waves, offering an additional degree of freedom to interface with other devices. The intrinsic nature of the mechanism governing the oscillations gives rise to a high degree of control and repeatability. Obtaining such properties in an epitaxial perovskite oxide, opens the way towards combining self-oscillating properties with those of other piezoelectric, ferroelectric, or magnetic perovskite oxides to achieve hybrid neuristor-memristor functionality in compact heterostuctures.

physics.app-ph↗

arXiv2019

BaTiO3 thin films as transitional ferrroelectrics with giant dielectric response

Proximity to phase transitions (PTs) is frequently responsible for the largest dielectric susceptibilities in ferroelectrics. The impracticality of using temperature as a control parameter to reach those large responses has motivated the design of solid solutions with phase boundaries between different polar phases at temperatures (typically room temperature) significantly lower than the paraelectric-ferroelectric critical temperature. The flat energy landscapes close to these PTs give rise to polarization rotation under external stimuli, being responsible for the best piezoelectrics so far and a their huge market. But this approach requires complex chemistry to achieve temperature-independent PT boundaries and often involves lead-containing compounds. Here we report that such a bridging state is possible in thin films of chemically simple materials such as BaTiO3. A coexistence of tetragonal, orthorhombic and their bridging low-symmetry phases are shown to be responsible for the continuous vertical polarization rotation, recreating a smear in-transition state and leading to giant temperature-independent dielectric response. These features are distinct from those of single crystals, multi-domain crystals, ceramics or relaxor ferroelectrics, requiring a different description. We believe that other materials can be engineered in a similar way to form a class of ferroelectrics, in which MPB solid solutions are also included, that we propose to coin as transitional ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2017

Magnetic properties of strained multiferroic CoCr2O4: a soft X-ray study

Using resonant soft X-ray techniques we follow the magnetic behavior of a strained epitaxial film of CoCr2O4, a type-II multiferroic. The film is [110]-oriented, such that both the ferroelectric and ferromagnetic moments can coexist in plane. X-ray magnetic circular dichroism (XMCD) is used in scattering and in transmission modes to probe the magnetization of Co and Cr separately. The transmission measurements utilized X-ray excited optical luminescence from the substrate. Resonant soft X-ray diffraction (RSXD) was used to study the magnetic order of the low temperature phase. The XMCD signals of Co and Cr appear at the same ordering temperature Tc~90K, and are always opposite in sign. The coercive field of the Co and of Cr moments is the same, and is approximately two orders of magnitude higher than in bulk. Through sum rules analysis an enlarged Co2+ orbital moment (m_L) is found, which can explain this hardening. The RSXD signal of the (q q 0) reflection appears below Ts, the same ordering temperature as the conical magnetic structure in bulk, indicating that this phase remains multiferroic under strain. To describe the azimuthal dependence of this reflection, a slight modification is required to the spin model proposed by the conventional Lyons-Kaplan-Dwight-Menyuk theory for magnetic spinels. Lastly, a slight increase in reflected intensity is observed below Ts=27K when measuring at the Cr edge (but not at the Co edge).

cond-mat.str-el↗

arXiv2011

Local conductivity and the role of vacancies around twin walls of (001)-BiFeO3 thin films

BiFeO3 thin films epitaxially grown on SrRuO3-buffered (001)-oriented SrTiO3 substrates show orthogonal bundles of twin domains, each of which contains parallel and periodic 71o domain walls. A smaller amount of 109o domain walls are also present at the boundaries between two adjacent bundles. All as-grown twin walls display enhanced conductivity with respect to the domains during local probe measurements, due to the selective lowering of the Schottky barrier between the film and the AFM tip (see S. Farokhipoor and B. Noheda, Phys. Rev. Lett. 107, 127601 (2011)). In this paper we further discuss these results and show why other conduction mechanisms are discarded. In addition we show the crucial role that oxygen vacancies play in determining the amount of conduction at the walls. This prompts us to propose that the oxygen vacancies migrating to the walls locally lower the Schottky barrier. This mechanism would then be less efficient in non-ferroelastic domain walls where one expects no strain gradients around the walls and thus (assuming that walls are not charged) no driving force for accumulation of defects.

cond-mat.mtrl-sci↗

arXiv2011

Conduction through 71o domain walls in BiFeO3 thin films

Local conduction at domains and domains walls is investigated in BiFeO3 thin films containing mostly 71o domain walls. Measurements at room temperature reveal conduction through 71o domain walls. Conduction through domains could also be observed at high enough temperatures. It is found that, despite the lower conductivity of the domains, both are governed by the same mechanisms: in the low voltage regime electrons trapped at defect states are temperature-activated but the current is limited by the ferroelectric surface charges; in the large voltage regime, Schottky emission takes place and the role of oxygen vacancies is that of selectively increasing the Fermi energy at the walls and locally reducing the Schottky barrier. This understanding provides the key to engineering conduction paths in oxides.

cond-mat.mtrl-sci↗

arXiv2009

Tuning the atomic and domain structure of epitaxial films of multiferroic BiFeO3

Recent works have shown that the domain walls of room-temperature multiferroic BiFeO3 (BFO) thin films can display distinct and promising functionalities. It is thus important to understand the mechanisms underlying domain formation in these films. High-resolution x-ray diffraction and piezo-force microscopy, combined with first-principles simulations, have allowed us to characterize both the atomic and domain structure of BFO films grown under compressive strain on (001)-SrTiO3, as a function of thickness. We derive a twining model that describes the experimental observations and explains why the 71o domain walls are the ones commonly observed in these films. This understanding provides us with a new degree of freedom to control the structure and, thus, the properties of BiFeO3 thin films.

cond-mat.mtrl-sci↗

arXiv2009

Phase transitions and ferroelectrics: revival and the future in the field

It appeared worthwhile to us to present a state-of-the-art look at the field of ferroelectrics. We are certainly not attempting to provide a complete review of all aspects of the field of ferroelectrics over the last years but we wish to transport a flavour of the current excitement in the field through the (subjective) choice of four specific examples of current interest: (i) Piezoelectrics and the morphotropic phase boundary, (ii) Multiferroics, (iii) The effect of high pressure on ferroelectrics and (iv) Strain-engineering in ferroelectric oxide thin films. For each topic we will try to work out both current interesting approaches and an outlook into future challenges. Throughout our discussion, the reader is referred to a list of significant review articles, books and papers in the field.

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

Smallest 90o domains in epitaxial ferroelectric films

Ferroelectrics display spontaneous and switchable electrical polarization. Until recently, ferroelectricity was believed to disappear at the nanoscale; now, nano-ferroelectrics are being considered in numerous applications. This renewed interest was partly fuelled by the observation of ferroelectric domains in films of a few unit cells thickness, promising further size reduction of ferroelectric devices. It turns out that at reduced scales and dimensionalities the material's properties depend crucially on the intricacies of domain formation, that is, the way the crystal splits into regions with polarization oriented along the different energetically equivalent directions, typically at 180o and 90o from each other. Here we present a step forward in the manipulation and control of ferroelectric domains by the growth of thin films with regular self-patterned arrays of 90o domains only 7 nm wide. This is the narrowest width for 90o domains in epitaxial ferroelectrics that preserves the film lateral coherence, independently of the substrate.

cond-mat.mtrl-sci↗

arXiv2006

Polar domains in lead titanate films under tensile strain

Thin films of PbTiO3, a classical ferroelectric, have been grown under tensile strain on single-crystal substrates of DyScO3. The films, of only 5nm thickness, grow fully coherent with the substrate and show no crystallographic twin domains, as evidenced by synchrotron x-ray diffraction. A mapping of the reciprocal space reveals intensity modulations (satellites) due to regularly-spaced polar domains in which the polarization appears rotated away from the substrate normal, characterizing a low symmetry phase not observed in the bulk material. This could have important practical implications since these phases are known to be responsible for ultrahigh piezoelectric responses in complex systems.

cond-mat.mtrl-sci↗