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Beatriz Noheda

Publications and source records attributed to Beatriz Noheda.

At least 37 records · Page 2Linked to original sources

Phenomenological classification of metals based on resistivity

Efforts to understand metallic behaviour have led to important concepts such as those of strange metal, bad metal or Planckian metal. However, a unified description of metallic resistivity is still missing. An empirical analysis of a large variety of metals shows that the parallel resistor formalism used in the cuprates, which includes T-linear and T-quadratic dependence of the electron scattering rates, can be used to provide a phenomenological description of the electrical resistivity in all metals, where these two contributions are shown to correspond to the two first terms of a Taylor expansion of the resistivity, detached of their physics origin, and thus, valid for any metal. Here we show that the different metallic classes are then determined by the relative magnitude of these two components and the magnitude of the extrapolated residual resistivity. These two parameters allow to categorize a few systems that are notoriously hard to ascribe to one of the currently accepted metallic classes. This approach also reveals that the T-linear term has a common origin in all cases, strengthening the arguments that propose the universal character of the Planckian dissipation bound.

cond-mat.str-el↗

Unusual ferrimagnetism in CaFe2O4

Incomplete cancellation of collinear antiparallel spins gives rise to ferrimagnetism. Even if the oppositely polarized spins are owing to the equal number of a single magnetic element having the same valence state, in principle, a ferrimagnetic state can still arise from the crystallographic inequivalence of the host ions. However, experimental identification of such a state as ferrimagnetic is not straightforward because of the tiny magnitude expected for M and the requirement for a sophisticated technique to differentiate similar magnetic sites. We report a synchrotron-based resonant x-ray investigation at the Fe L2,3 edges on an epitaxial film of CaFe2O4, which exhibits two magnetic phases with similar energies. We find that while one phase of CaFe2O4 is antiferromagnetic, the other one is ferrimagnetic with an antiparallel arrangement of an equal number of spins between two distinct crystallographic sites with very similar local coordination environments. Our results further indicate two distinct origins of an overall minute M; one is intrinsic, from distinct Fe3+ sites, and the other one is extrinsic, arising from defective Fe2+ likely forming weakly-coupled ferrimagnetic clusters. These two origins are uncorrelated and have very different coercive fields. Hence, this work provides a direct experimental demonstration of ferrimagnetism solely due to crystallographic inequivalence of the Fe3+ as the origin of the weak M of CaFe2O4.

cond-mat.mtrl-sci↗

Ferroelastic domain walls in BiFeO$_3$ as memristive networks

Electronic conduction along individual domain walls (DWs) has been reported in BiFeO$_3$ (BFO) and other nominally insulating ferroelectrics. DWs in these materials separate regions of differently oriented electrical polarization (domains) and are just a few atoms wide, providing self-assembled nanometric conduction paths. In this work, it is shown that electronic transport is possible also from wall to wall through the dense network of as-grown DWs in BFO thin films. Electric field cycling at different points of the network, performed locally by conducting atomic force microscope (cAFM), induces resistive switching selectively at the DWs, both for vertical (single wall) and lateral (wall-to-wall) conduction. These findings are the first step towards investigating DWs as memristive networks for information processing and in-materio computing.

cond-mat.mtrl-sci↗

Thin films of the alpha-quartz SixGe1-xO2 solid-solution

SiO2 with the alpha-quartz structure is one of the most popular piezoelectrics. It is widely used in crystal oscillators, bulk acoustic wave (BAW) devices, surface acoustic wave (SAW) devices, and so on. GeO2 can also be crystallized into the alpha-quartz structure and it has better piezoelectric properties, with higher piezoelectric coefficient and electromechanical coupling coefficients, than SiO2. Experiments on bulk crystals and theoretical studies have shown that these properties can be tuned by varying the Si/Ge ratio in the SixGe1-xO2 solid solution. However, to the best of our knowledge, thin films of SixGe1-xO2 quartz have never been reported. Here we present the successful crystallization of SixGe1-xO2 thin films in the alpha-quartz phase on quartz substrates (SiO2) with x up to 0.75. Generally, the films grow semi-epitaxially, with the same orientation as the substrates. Interestingly, the Si0.75Ge0.25O2 composition grows fully strained by the quartz substrates and this leads to the formation of circular quartz domains with an ordered Dauphine twin structure. These studies represent a first step towards the optimization of piezoelectric quartz thin films for high frequency (> 5 GHz) applications.

cond-mat.mtrl-sci↗

Crystallization of GeO2 thin films into alpha-quartz: from spherulites to single crystals

Piezoelectric quartz SiO2 crystals are widely used in industry as oscillators. As a natural mineral, quartz and its relevant silicates are also of interest of geoscience and mineralogy. However, the nucleation and growth of quartz crystals is difficult to control and not fully understood. Here we report successful solid state crystallization of thin film of amorphous GeO2 into quartz on various substrates including Al2O3, MgAl2O4, MgO, LaAlO3 and SrTiO3. At relatively low annealing temperatures, the crystallization process is spherulitic: with fibers growing radially from the nucleation centers and the crystal lattice rotating along the growth direction with a linear dependence between the rotation angle and the distance to the core. For increasingly higher annealing temperatures, quartz crystals begin to form. The edges of the sample play an important role facilitating nucleation followed by growth sweeping inward until the whole film is crystallized. Control of the growth allows single crystalline quartz to be synthesized. Our study reveals the complexity of the nucleation and growth process of quartz and provides insight for further studies.

cond-mat.mtrl-sci↗

Spherulitic and rotational crystal growth of Quartz thin films

To obtain crystalline thin films of alpha-Quartz represents a challenge due to the tendency for the material towards spherulitic growth. Thus, understanding the mechanisms that give rise to spherulitic growth can help regulate the growth process. Here the spherulitic type of 2D crystal growth in thin amorphous Quartz films was analyzed by electron back-scatter diffraction (EBSD). EBSD was used to measure the size, orientation, and rotation of crystallographic grains in polycrystalline SiO2 and GeO2 thin films with high spatial resolution. Individual spherulitic Quartz crystal colonies contain primary and secondary single crystal fibers, which grow radially from the colony center towards its edge, and fill a near circular crystalline area completely. During their growth, individual fibers form so-called rotational crystals, when some lattice planes are continuously bent. The directions of the lattice rotation axes in the fibers were determined by an enhanced analysis of EBSD data. A possible mechanism, including the generation of the particular type of dislocation(s), is suggested.

cond-mat.mtrl-sci↗

From hidden metal-insulator transition to Planckian-like dissipation by tuning disorder in a nickelate

Heavily oxygen deficient NdNiO$_3$ (NNO) films, which are insulating due to electron localization, contain pristine regions that undergo a hidden metal-insulator transition. Increasing oxygen content increases the connectivity of the metallic regions and the metal-insulator transition is first revealed, upon reaching the percolation threshold, by the presence of hysteresis. Only upon further oxygenation is the global metallic state (with a change in the resistivity slope) eventually achieved. It is shown that sufficient oxygenation leads to linear temperature dependence of resistivity in the metallic state, with a scattering rate directly proportional to temperature. Despite the known difficulties to establish the proportionality constant, the experiments are consistent with a relationship 1/$τ$= $αk_B T/\hbar$, with $α$ not far from unity. These results could provide experimental support for recent theoretical predictions of disorder in a two-fluid model as a possible origin of Planckian dissipation.

cond-mat.str-el↗

Plausible physical mechanisms for unusual volatile/non-volatile resistive switching in HfO2-based stacks

Memristive devices made of silicon compatible simple oxides are of great interest for storage and logic devices in future adaptable electronics and non-digital computing applications. A series of highly desirable properties observed in an atomic-layer-deposited hafnia-based stack, triggered our interest to investigate their suitability for technological implementations. In this paper, we report our attempts to reproduce the observed behaviour within the framework of a proposed underlying mechanism. The inability of achieving the electrical response of the original batch indicates that a key aspect in those devices has remained undetected. By comparing newly made devices with the original ones, we gather some clues on the plausible alternative mechanisms that could give rise to comparable electrical behaviours.

cond-mat.mtrl-sci↗

Guidelines for the stabilization of a polar rhombohedral phase in epitaxial Hf0.5Zr0.5O2 thin films

The unconventional Si-compatible ferroelectricity in hafnia-based systems, which becomes robust only at nanoscopic sizes, has attracted a lot of interest. While a metastable polar orthorhombic (o-) phase (Pca21) is widely regarded as the responsible phase for ferroelectricity, a higher energy polar rhombohedral (r-) phase is recently reported on epitaxial HfZrO4 (HZO) films grown on (001) SrTiO3 (R3m or R3), (0001) GaN (R3), and Si (111). Armed with results on these systems, here we report a systematic study leading towards identifying comprehensive global trends for stabilizing r-phase polymorphs in epitaxially grown HZO thin films (6 nm) on various substrates (perovskites, hexagonal and Si).

cond-mat.mtrl-sci↗

Operando observation of reversible oxygen migration and phase transitions in ferroelectric devices

Unconventional ferroelectricity, robust at reduced nanoscale sizes, exhibited by hafnia-based thin-films presents tremendous opportunities in nanoelectronics. However, the exact nature of polarization switching remains controversial. Here, we investigate epitaxial Hf0.5Zr0.5O2 (HZO) capacitors, interfaced with oxygen conducting metals (La0.67Sr0.33MnO3, LSMO) as electrodes, using atomic resolution electron microscopy while in situ electrical biasing. By direct oxygen imaging, we observe reversible oxygen vacancy migration from the bottom to the top electrode through HZO and reveal associated reversible structural phase transitions in the epitaxial LSMO and HZO layers. We follow the phase transition pathways at the atomic scale and identify that these mechanisms are at play both in tunnel junctions and ferroelectric capacitors switched with sub-millisecond pulses. Our results unmistakably demonstrate that oxygen voltammetry and polarization switching are intertwined in these materials.

cond-mat.mtrl-sci↗

Ferroelectric PbZr$_{1-x}$Ti$_x$O$_3$ by ethylene glycol-based chemical solution synthesis

We have investigated a water-stable sol-gel method based on ethylene glycol as a solvent and bridging ligand for the synthesis of ferroelectric lead zirconate titanate in bulk and thin film forms. This method offers lower toxicity of the solvent, higher stability towards atmospheric moisture and a simplified synthetic procedure compared to traditional sol-gel methods. Ceramic pellets of Nb-doped lead zirconate titanate (PNZT) in the rhombohedral phase were produced with high density and good piezoelectric properties, comparable to those reported in the literature and those found in commercial piezoelectric elements. In addition, a nine-layer thin film stack was fabricated from the same sol by spin coating onto platinized silicon substrates. The films were crack-free and showed a dense perovskite grain structure with a weak (111) orientation. Piezoelectric measurements of the film showed a piezoelectric coefficient comparable to literature values and good stability towards fatigue.

physics.chem-ph↗

Structure and magnetic properties of epitaxial CaFe2O4 thin films

CaFe2O4 is a highly anisotropic antiferromagnet reported to display two spin arrangements with up-up-down-down (phase A) and up-down-up-down (phase B) configurations. The relative stability of these phases is ruled by the competing ferromagnetic and antiferromagnetic interactions between Fe3+ spins arranged in two different environments, but a complete understanding of the magnetic structure of this material does not exist yet. In this study we investigate epitaxial CaFe2O4 thin films grown on TiO2 (110) substrates by means of Pulsed Laser Deposition (PLD). Structural characterization reveals the coexistence of two out-of-plane crystal orientations and the formation of three in-plane oriented domains. The magnetic properties of the films, investigated macroscopically as well as locally, including highly sensitive Mossbauer spectroscopy, reveal the presence of just one order parameter showing long-range ordering below T = 185 K and the critical nature of the transition. In addition, a non-zero in-plane magnetization is found, consistent with the presence of uncompensated spins at phase or domain boundaries, as proposed for bulk samples.

cond-mat.mtrl-sci↗

Atomic Layer Deposition of SiO$_2$-GeO$_2$ multilayers

Despite its interest for CMOS applications, Atomic Layer Deposition (ALD) of GeO$_{2}$ thin films, by itself or in combination with SiO$_{2}$, has not been widely investigated yet. Here we report the ALD growth of SiO$_{2}$/GeO$_{2}$ multilayers on Silicon substrates using a so far unreported Ge precursor. The characterization of multilayers with various periodicities reveals successful layer-by-layer growth with electron density contrast and absence of chemical intermixing, down to a periodicity of 2 atomic layers.

cond-mat.mtrl-sci↗

Stabilization of phase-pure rhombohedral HfZrO4 in Pulsed Laser Deposited thin films

Controlling the crystalline structure of Hafnium Zirconate and its epitaxial relationship to a semiconducting electrode has a high technological interest, as ferroelectric materials are key ingredients for emerging electronic devices. Using Pulsed Laser Deposition, a phase pure, ultra-thin film of HfZrO4 is grown epitaxially on a GaN (0001) / Si (111) template. Since standard microscopy techniques do not allow to determine with certitude the crystalline structure of the film due to the weak scattering of oxygen, differentiated differential phase contrast (DPC) Scanning Transmission Electron Microscopy is used to allow the direct imaging of oxygen columns in the film. Combined with X-Rays diffraction analysis, the polar nature and rhombohedral R3 symmetry of the film are demonstrated.

cond-mat.mtrl-sci↗

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↗

Magneto-ionic control of spin polarization in magnetic tunnel junctions

Magnetic tunnel junctions (MTJs) with Hf0.5Zr0.5O2 barriers are reported to show both tunneling magnetoresistance effect (TMR) and tunneling electroresistance effect (TER), displaying four resistance states by magnetic and electric field switching. Here we show that, under electric field cycling of large enough magnitude, the TER can reach values as large as 10^6%. Moreover, concomitant with this TER enhancement, the devices develop electrical control of spin polarization, with sign reversal of the TMR effect. Currently, this intermediate state exists for a limited number of cycles and understanding the origin of these phenomena is key to improve its stability. The experiments presented here point to the magneto-ionic effect as the origin of the large TER and strong magneto-electric coupling, showing that ferroelectric polarization switching of the tunnel barrier is not the main contribution.

cond-mat.mtrl-sci↗

Direct epitaxial growth of polar (1-x)HfO2-(x)ZrO2 ultra-thin films on Silicon

Ultra-thin Hf1-xZrxO2 films have attracted tremendous interest owing to their Si-compatible ferroelectricity arising from polar polymorphs. While these phases have been grown on Si as polycrystalline films, epitaxial growth was only achieved on non-Si substrates. Here we report direct epitaxy of polar phases on Si using pulsed laser deposition enabled via in situ scavenging of the native a-SiOx under ballistic conditions. On Si (111), polar rhombohedral (r)-phase and bulk monoclinic (m-) phase coexist, with the volume of the former increasing with increasing Zr concentration. R-phase is stabilized in the regions with a direct connection between the substrate and the film through the compressive strain provided by an interfacial crystalline c-SiO2 layer., The film relaxes to a bulk m-phase in regions where a-SiOx regrows. On Si (100), we observe polar orthorhombic o-phase coexisting with m-phase, stabilized by inhomogeneous strains at the intersection of monoclinic domains. This work provides fundamental insight into the conditions that lead to the preferential stabilization of r-, o- and m-phases.

cond-mat.mtrl-sci↗

Magnetic tunnel junctions based on ferroelectric Hf0.5Zr0.5O2 tunnel barriers

A ferroelectric tunnel barrier in between two ferromagnetic electrodes (multiferroic tunnel junction, MFTJ), is one of the most promising concepts for future microelectronic devices. In parallel, Hafnia based ferroelectrics are showing great potential for device miniaturization down to the nanoscale. Here we utilize ferroelectric Hf0.5Zr0.5O2 (HZO) with thickness of only 2 nm, epitaxially grown on La0.7Sr0.3MnO3 (LSMO) ferromagnetic electrodes, as a large band-gap insulating barrier integrated in MFTJs with cobalt top electrodes. As previously reported for other MFTJs with similar electrodes, the tunneling magnetoresistance (TMR) can be tuned and its sign can even be reversed by the bias voltage across the junction. We demonstrate four non-volatile resistance states generated by magnetic and electric field switching with high reproducibility in this system.

physics.app-ph↗