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Josep Fontcuberta

Publications and source records attributed to Josep Fontcuberta.

At least 19 recordsLinked to original sources

High accuracy Spin Hall Effect Induced Spin Accumulation detection in MOKE Measurements

Charge to spin (orbital) momentum conversion phenomena enclose great potential for advancing applications in spin/orbitronics. Although current-induced magnetic moment accumulation is crucial both for fundamental understanding and practical applications, direct quantifications are scarce. Optical polarization measurements, namely magneto-optical Kerr rotation (MOKE) ($\theta_K$), have been used to get direct evidence of magnetic accumulation perpendicular to a current flow density ($J$) in late transition metals (Pt) as well as in light transition elements (Ti, Cr), and used to conclude evidence of spin or orbital momentum accumulation. However, discrepancies of the reported $\theta_K/J$ values, exceeding one order of magnitude, together with early claims that conventional MOKE experiments were not a suitable tool, is prompting revisions of methods and results. Here, we report on a new methodology for MOKE measurements that solves known bottlenecks. We obtain a sensitivity of $(354 \pm 27)$ nV/nrad and use the designed protocol to measure $|\theta_K^S/J| = (7.92 \pm 1.94)$ nrad/$(10^7$ A/cm$^2)$ and $|\theta_K^P/J| = (6.89 \pm 1.74)$ nrad/$(10^7$ A/cm$^2)$ in a 50 nm thick Pt bar for S and P polarized incident light, respectively.The extracted value of $|\theta_K^S/J|$ is significantly smaller, about a 7-fold reduction, than previous results on a nominally identical device. Given that differences in the microstructure of Pt films cannot account for such large discrepancy, this implies that experimental procedures and models should be revised accordingly.

cond-mat.mtrl-sci

Orbital Occupancy and Hybridization in Strained SrVO$_3$ Epitaxial Films

Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the hierarchy of orbitals within the $t_{2g}$ and $e_g$ manifolds. Data show a remarkable $2p-3d$ hybridization, as well as a strain-induced reordering of the V $3d$($t_{2g}$, $e_g$) orbitals. The latter is itself accompanied by a consequent change of hybridization that modulates the hybrid $π^*$ and $σ^*$ orbitals and the carrier population at the metal ions, challenging a rigid band picture.

cond-mat.str-el

Polarization and resistive switching in epitaxial 2 nm Hf$_{0.5}$Zr$_{0.5}$O$_2$ tunnel junctions

In the quest for reliable and power-efficient memristive devices, ferroelectric tunnel junctions are being investigated as potential candidates. CMOS-compatible ferroelectric hafnium oxides are at the forefront. However, in epitaxial tunnel devices with thicknesses around ${\approx}$ 4 - 6 nm, the relatively high tunnel energy barrier produces a large resistance that challenges their implementation. Here, we show that ferroelectric and electroresistive switching can be observed in ultrathin 2 nm epitaxial Hf$_{0.5}$Zr$_{0.5}$O$_2$ (HZO) tunnel junctions in large area capacitors (${\approx} 300μm^2$). We observe that the resistance area product is reduced to about 160 $Ω{\cdot}$cm$^2$ and 65 $Ω{\cdot}$cm$^2$ for OFF and ON resistance states, respectively. These values are two orders of magnitude smaller than those obtained in equivalent 5 nm HZO tunnel devices while preserving a similar OFF/ON resistance ratio (210 ${\%}$). The devices show memristive and spike-timing-dependent plasticity (STDP) behavior and good retention. Electroresistance and ferroelectric loops closely coincide, signaling ferroelectric switching as a driving mechanism for resistance change.

physics.app-ph

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

Flexible antiferromagnetic FeRh tapes as memory elements

The antiferromagnetic to ferromagnetic transition occurring above room temperature in FeRh is attracting interest for applications in spintronics, with perspectives for robust and untraceable data storage. Here, we show that FeRh films can be grown on a flexible metallic substrate (tape shaped), coated with a textured rock-salt MgO layer, suitable for large scale applications. The FeRh tape displays a sharp antiferromagnetic to ferromagnetic transition at about 90 oC. Its magnetic properties are preserved by bending (radii of 300 mm), and their anisotropic magnetoresistance (up to 0.05 %) is used to illustrate data writing/reading capability.

cond-mat.mtrl-sci

Blocking of conducting channels widens window for ferroelectric resistive switching in interface-engineered Hf0.5Zr0.5O2 tunnel devices

Films of Hf0.5Z0.5O2 (HZO) contain a network of grain boundaries. In (111) HZO epitaxial films on (001) SrTiO3, for instance, twinned orthorhombic (o-HZO) ferroelectric crystallites coexist with grain boundaries between o-HZO and a residual paraelectric monoclinic (m-HZO) phase. These grain boundaries contribute to the resistive switching response in addition to the genuine ferroelectric polarization switching and have detrimental effects on device performance. Here, it is shown that, by using suitable nanometric capping layers deposited on HZO film, a radical improvement of the operation window of the tunnel device can be achieved. Crystalline SrTiO3 and amorphous AlOx are explored as capping layers. It is observed that these layers conformally coat the HZO surface and allow to increase the yield and homogeneity of functioning ferroelectric junctions while strengthening endurance. Data show that the capping layers block ionic-like transport channels across grain boundaries. It is suggested that they act as oxygen suppliers to the oxygen-getters grain boundaries in HZO. In this scenario it could be envisaged that these and other oxides could also be explored and tested for fully compatible CMOS technologies.

cond-mat.mtrl-sci

Unraveling ferroelectric polarization and ionic contributions to electroresistance in epitaxial Hf0.5Zr0.5O2 tunnel junctions

Tunnel devices based on ferroelectric Hf0.5Zr0.5O2 (HZO) barriers hold great promises for emerging data storage and computing technologies. The resistance state of the device can be changed by a suitable writing voltage. However, the microscopic mechanisms leading to the resistance change are an intricate interplay between ferroelectric polarization controlled barrier properties and defect-related transport mechanisms. Here is shown the fundamental role of the microstructure of HZO films setting the balance between those contributions. The oxide film presents coherent or incoherent grain boundaries, associated to the existence of monoclinic and orthorhombic phases in HZO films, which are dictated by the mismatch with the substrates for epitaxial growth. These grain boundaries are the toggle that allows to obtain either large (up to 450 %) and fully reversible genuine polarization controlled electroresistance when only the orthorhombic phase is present or an irreversible and extremely large (1000-100000 %) electroresistance when both phases coexist.

cond-mat.mtrl-sci

Reversible and magnetically unassisted voltage-driven switching of magnetization in FeRh/PMN-PT

Reversible control of magnetization by electric fields without assistance from a subsidiary magnetic field or electric current could help reduce the power consumption in spintronic devices. When increasing temperature above room temperature, FeRh displays an uncommon antiferromagnetic to ferromagnetic phase transition linked to a unit cell volume expansion. Thus, using the strain exerted by an adjacent piezoelectric layer, the relative amount of antiferromagnetic and ferromagnetic regions can be tuned by an electric field applied to the piezoelectric material. Indeed, large variations in the saturation magnetization have been observed when straining FeRh films grown on suitable piezoelectric substrates. In view of its applications, the variations in the remanent magnetization rather than those of the saturation magnetization are the most relevant. Here, we show that in the absence of any bias external magnetic field, permanent and reversible magnetization changes as high as 34% can be induced by an electric field, which remain after this has been zeroed. Bulk and local magnetoelectric characterization reveals that the fundamental reason for the large magnetoelectric response observed at remanence is the expansion (rather than the nucleation) of ferromagnetic nanoregions.

cond-mat.mtrl-sci

Strain and voltage control of magnetic and electric properties of FeRh films

FeRh based alloys may display an uncommon transition from a ferromagnetic to an antiferromagnetic state upon cooling. The transition takes place roughly above room temperature and it can be sensitively modulated by composition and external parameters, including pressure and strain. Consequently, thin films of FeRh have received attention for applications in spintronics, antiferromagnetic spintronics and sensing. Interestingly, the extreme sensitivity of its properties to strain has created expectations for energy friendly voltage-control of the magnetic state of FeRh, with a number of potential applications at the horizon. Here, after summarizing the current understanding of strain effects on the magnetic properties of FeRh thin films, we review achievements on exploiting piezoelectric substrates for in-operando tuning of their magneto-electric properties. We end with a brief summary and an outlook for future initiatives.

cond-mat.mtrl-sci

Engineering Ferroelectric Hf0.5Zr0.5O2 Thin Films by Epitaxial Stress

The critical impact of epitaxial stress on the stabilization of the ferroelectric orthorhombic phase of hafnia is proved. Epitaxial bilayers of Hf0.5Zr0.5O2 and La0.67Sr0.33MnO3 electrodes were grown on a set of single crystalline oxide 001-oriented, cubic or pseudocubic setting, substrates with lattice parameter in the 3.71 - 4.21 A range. The lattice strain of the La0.67Sr0.33MnO3 electrode, determined by the lattice mismatch with the substrate, is critical in the stabilization of the orthorhombic phase of Hf0.5Zr0.5O2. On La0.67Sr0.33MnO3 electrodes tensile strained most of the Hf0.5Zr0.5O2 film is orthorhombic, whereas the monoclinic phase is favored when La0.67Sr0.33MnO3 is relaxed or compressively strained. Therefore, the Hf0.5Zr0.5O2 films on TbScO3 and GdScO3 substrates present substantially enhanced ferroelectric polarization in comparison to films on other substrates, including the commonly used SrTiO3. The capability of having epitaxial doped HfO2 films with controlled phase and polarization is of major interest for a better understanding of the ferroelectric properties and paves the way for fabrication of ferroelectric devices based on nanometric HfO2 films.

cond-mat.mtrl-sci

Growth Window of Ferroelectric Epitaxial Hf0.5Zr0.5O2 Thin Films

The metastable orthorhombic phase of hafnia is generally obtained in polycrystalline films, whereas in epitaxial films, its formation has been much less investigated. We have grown Hf0.5Zr0.5O2 films by pulsed laser deposition, and the growth window (temperature and oxygen pressure during deposition and film thickness) for epitaxial stabilization of the ferroelectric phase is mapped. The remnant ferroelectric polarization, up to around 24 uC/cm2, depends on the amount of orthorhombic phase and interplanar spacing and increases with temperature and pressure for a fixed film thickness. The leakage current decreases with an increase in thickness or temperature, or when decreasing oxygen pressure. The coercive electric field (EC) depends on thickness (t) according to the coercive electric field (Ec) - thickness (t)-2/3 scaling, which is observed for the first time in ferroelectric hafnia, and the scaling extends to thicknesses down to around 5 nm. The proven ability to tailor the functional properties of high-quality epitaxial ferroelectric Hf0.5Zr0.5O2 films paves the way toward understanding their ferroelectric properties and prototyping devices.

cond-mat.mtrl-sci

Epitaxial Integration on Si(001) of Ferroelectric Hf0.5Zr0.5O2 Capacitors with High Retention and Endurance

Epitaxial ferroelectric Hf0.5Zr0.5O2 films have been successfully integrated in a capacitor heterostructure on Si(001). The orthorhombic Hf0.5Zr0.5O2 phase, [111] out-of-plane oriented, is stabilized in the films. The films present high remnant polarization Pr close to 20 μC/cm2, rivaling with equivalent epitaxial films on single crystalline oxide substrates. Retention time is longer than 10 years for writing field of around 5 MV/cm, and the capacitors show endurance up to 1E9 cycles for writing voltage of around 4 MV/cm. It is found that the formation of the orthorhombic ferroelectric phase depends critically on the bottom electrode, being achieved on La0.67Sr0.33MnO3 but not on LaNiO3. The demonstration of excellent ferroelectric properties in epitaxial films of Hf0.5Zr0.5O2 on Si(001) is relevant towards fabrication of devices that require homogeneity in the nanometer scale, as well as for better understanding of the intrinsic properties of this promising ferroelectric oxide.

physics.app-ph

Magnetoresistance in Hybrid Pt/CoFe2O4 Bilayers Controlled by Competing Spin Accumulation and Interfacial Chemical Reconstruction

Pure spin currents hold promises for an energy-friendlier spintronics. They can be generated by a flow of charge along a non-magnetic metal having a large spin-orbit coupling. It produces a spin accumulation at its surfaces, controllable by the magnetization of an adjacent ferromagnetic layer. Paramagnetic metals typically used are close to a ferromagnetic instability and thus magnetic proximity effects can contribute to the observed angular-dependent magnetoresistance (ADMR). As interface phenomena govern the spin conductance across the metal/ferromagnetic-insulator heterostructures, unraveling these distinct contributions is pivotal to full understanding of spin current conductance. We report here x-ray absorption and magnetic circular dichroism (XMCD) at Pt-M and (Co,Fe)-L absorption edges and atomically-resolved energy loss electron spectroscopy (EELS) data of Pt/CoFe2O4 bilayers where CoFe2O4 layers have been capped by Pt grown at different temperatures. It turns out that the ADMR differs dramatically, being either dominated by spin Hall magnetoresistance (SMR) associated to spin Hall effect or anisotropic magnetoresistance (AMR). The XMCD and EELS data indicate that the Pt layer grown at room temperature does not display any magnetic moment, whereas when grown at higher temperature it is magnetic due to interfacial Pt-(Co,Fe) alloying. These results allow disentangling spin accumulation from interfacial chemical reconstructions and for tailoring the angular dependent magnetoresistance.

cond-mat.mtrl-sci

Tailoring Lattice Strain and Ferroelectric Polarization of Epitaxial BaTiO3 Thin Films on Si(001)

Ferroelectric BaTiO3 films with large polarization have been integrated with Si(001) by pulsed laser deposition. High quality c-oriented epitaxial films are obtained in a substrate temperature range of about 300 deg C wide. The deposition temperature critically affects the growth kinetics and thermodynamics balance, resulting on a high impact in the strain of the BaTiO3 polar axis, which can exceed 2% in films thicker than 100 nm. The ferroelectric polarization scales with the strain and therefore deposition temperature can be used as an efficient tool to tailor ferroelectric polarization. The developed strategy overcomes the main limitations of the conventional strain engineering methodologies based on substrate selection: it can be applied to films on specific substrates including Si(001) and perovskites, and it is not restricted to ultrathin films.

cond-mat.mtrl-sci

Strain-controlled responsiveness of slave half-doped manganite La0.5Sr0.5MnO3 layers inserted in BaTiO3 ferroelectric tunnel junctions

Insertion of layers displaying field-induced metal-to-insulator (M/I) transition in ferroelectric tunnel junctions (FTJs) has received attention as a potentially useful way to enlarge junction tunnel electroresistance (TER). Half-doped manganites being at the verge of metal-insulator character are thus good candidates to be slave layers in FTJs. However, the phase diagram of these oxides is extremely sensitive to strain and thus can be radically different when integrated in epitaxial FTJs. Here we report a systematic study of large-area (A = 4 to 100 um2) Pt/La0.5Sr0.5MnO3/BaTiO3/La0.7Sr0.3MnO3 (Pt/HD/BTO/LSMO) FTJs, having different thicknesses of the ferroelectric (2-3nm) and HD layers (1-2nm), grown on substrates imposing either tensile (SrTiO3) or compressive (LaAlO3) strains. Room-temperature electric characterization of the FTJs shows polarization-controlled ON/ OFF states. Clear evidences of field-induced M/I transition (difference between junction resistance in OFF and ON state is increased of more than one order of magnitude) are observed in junctions prepared on SrTiO3 but the HD layer is generally metallic on LaAlO3. Moreover, the M/I transition is only confined in an interfacial layer of the slave film thus entailing an overall reduction of TER. The orderly results reported here give some hints towards selection of HD materials and substrates for optimal FTJ responsiveness.

cond-mat.mtrl-sci

Simultaneous imaging of strain waves and induced magnetization dynamics at the nanometer scale

Changes in strain can be used to modify electronic and magnetic properties in crystal structures, to manipulate nanoparticles and cells, or to control chemical reactions. The magneto-elastic (ME) effect--the change of magnetic properties caused by the elastic deformation (strain) of a magnetic material--has been proposed as an alternative approach to magnetic fields for the low power control of magnetization states of nanoelements since it avoids charge currents, which entail ohmic losses. Multiferroic heterostructures \cite{Zheng2004} and nanocomposites have exploited this effect in search of electric control of magnetic states, mostly in the static regime. Quantitative studies combining strain and magnetization dynamics are needed for practical applications and so far, a high resolution technique for this has been lacking. Here, we have studied the effect of the dynamic strain accompanying a surface acoustic wave on magnetic nanostructures. We have simultaneously imaged the temporal evolution of both strain waves and magnetization dynamics of nanostructures at the picosecond timescale. The newly developed experimental technique, based on X-ray microscopy, is versatile and provides a pathway to the study of strain-induced effects at the nanoscale. Our results provide fundamental insight in the coupling between strain and magnetization in nanostructures at the picosecond timescale, having implications in the design of strain-controlled magnetostrictive nano-devices.

cond-mat.mes-hall

Spin Hall magnetoresistance as a probe for surface magnetization in Pt/CoFe$_2$O$_4$ bilayers

We study the spin Hall magnetoresistance (SMR) in Pt grown $\textit{in situ}$ on CoFe$_2$O$_4$ (CFO) ferrimagnetic insulating (FMI) films. A careful analysis of the angle-dependent and field-dependent longitudinal magnetoresistance indicates that the SMR contains a contribution that does not follow the bulk magnetization of CFO but it is a fingerprint of the complex magnetism at the surface of the CFO layer, thus signaling SMR as a tool for mapping surface magnetization. A systematic study of the SMR for different temperatures and CFO thicknesses gives us information impossible to obtain with any standard magnetometry technique. On one hand, surface magnetization behaves independently of the CFO thickness and does not saturate up to high fields, evidencing that the surface has its own anisotropy. On the other hand, characteristic zero-field magnetization steps are not present at the surface while they are relevant in the bulk, strongly suggesting that antiphase boundaries are the responsible of such intriguing features. In addition, a contribution from ordinary magnetoresistance of Pt is identified, which is only distinguishable due to the low resistivity of the $\textit{in-situ}$ grown Pt.

cond-mat.mes-hall

Giant Optical Polarization Rotation Induced by Spin-Orbit Coupling in Polarons

We have uncovered a giant gyrotropic magneto-optical response for doped ferromagnetic manganite La2/3Ca1/3MnO3 around the near room-temperature paramagnetic-to-ferromagnetic transition. At odds with current wisdom, where this response is usually assumed to be fundamentally fixed by the electronic band structure, we point to the presence of small polarons as the driving force for this unexpected phenomenon. We explain the observed properties by the intricate interplay of mobility, Jahn-Teller effect and spin-orbit coupling of small polarons. As magnetic polarons are ubiquitously inherent to many strongly correlated systems, our results provide an original, general pathway towards the generation of gigantic gyrotropic responses that can be harnessed for nonreciprocal devices that exploit the polarization of light.

cond-mat.str-el