Showing 1–26 of 26 results for author: Gazquez, J

Detecting Linear Dichroism with Atomic Resolution

Authors: Roger Guzman, Ján Rusz, Ang Li, Juan Carlos Idrobo, Wu Zhou, Jaume Gazquez

Abstract: X-ray linear dichroism has been pivotal for probing electronic anisotropies, but its inherent limited spatial resolution precludes atomic-scale investigations of orbital polarization. Here we introduce a versatile electron linear dichroism methodology in scanning transmission electron microscopy that overcomes these constraints. By exploiting momentum-transfer-dependent electron energy-loss spectr… ▽ More X-ray linear dichroism has been pivotal for probing electronic anisotropies, but its inherent limited spatial resolution precludes atomic-scale investigations of orbital polarization. Here we introduce a versatile electron linear dichroism methodology in scanning transmission electron microscopy that overcomes these constraints. By exploiting momentum-transfer-dependent electron energy-loss spectroscopy with an atomic-sized probe, we directly visualize orbital occupation at individual atomic columns in real space. Using strained La0.7Sr0.3MnO3 thin films as a model system, we resolve the Mn-3d eg orbital polarization with sub-angstrom precision. We show that compressive strain stabilizes 3z2-r2 occupation while tensile strain favors x2-y2. These results validate our approach against established X-ray measurements while achieving the ultimate single atomic-column sensitivity. We further demonstrate two optimized signal extraction protocols that adapt to experimental constraints without compromising sensitivity. This generalizable platform opens unprecedented opportunities to study symmetry-breaking phenomena at individual defects, interfaces, and in quantum materials where atomic-scale electronic anisotropy governs emergent functionality. △ Less

Submitted 24 November, 2025; originally announced November 2025.

Comments: 16 pages, 2 Figures, 3 Extended Figures

Sustainable wafer-scale integration of epitaxial ZnO on silicon for piezoelectric devices

Authors: D. Sanchez-Fuentes, R. Desgarceaux, A. Rahal, L. Garcia, S. Bousri, S. Ding, N. Camara, F. Pascal, R. Garcia-Bermejo, N. Guillaume, G. Ardila, J. Gazquez, C. Magen, S Plana-Ruiz, C. Guasch, A. Carretero-Genevrier

Abstract: To sustainably support the ongoing energetic transition, we need functional metal oxides capable of converting energy, and produce storage, and sensing devices. However, these materials suffer from a high economic cost of manufacturing, and their production in a sustainable way is, to date, a milestone. Additionally, the technical challenges, such as scalability and integration of silicon for indu… ▽ More To sustainably support the ongoing energetic transition, we need functional metal oxides capable of converting energy, and produce storage, and sensing devices. However, these materials suffer from a high economic cost of manufacturing, and their production in a sustainable way is, to date, a milestone. Additionally, the technical challenges, such as scalability and integration of silicon for industrial processing using microelectronic technologies, impose strict conditions for the entire materials process. In this work, we engineer α-quartz virtual substrates up to 4 inches facilitating the large-scale and sustainable integration of multifunctional epitaxial ZnO metal oxide microwire films on silicon. These materials are exclusively manufactured on silicon using solution chemistry, providing single-chip solutions that can meet strict economic constraints for developing sustainable devices at a lower cost. Through this integrative technology, we demonstrate the microfabrication of epitaxial (110)ZnO/(100)α-quartz/(100)silicon piezoelectric membrane resonators at the wafer-scale with potential applications in energy conversion and sensing. We combined four dimensional (4D)-STEM diffraction technology and Piezoelectric Force Microscopy (PFM) to establish a correlation between out of plane crystalline strain and piezoelectric response in epitaxial (110) ZnO at the microscale. Finally, we proved the fabrication of 800 nm thick (110) ZnO suspended membranes that can be transferred to flexible substrates, making them suitable for flexible devices. △ Less

Submitted 18 March, 2025; originally announced March 2025.

Comments: 40, 8 figures

Stoichiometric control of electron mobility and 2D superconductivity at LaAlO$_3$-SrTiO$_3$ interfaces

Authors: Gyanendra Singh, Roger Guzman, Guilhem Saïz, Wu Zhou, Jaume Gazquez, Jordi Fraxedas, Fereshteh Masoudinia, Dag Winkler, Tord Claeson, Nicolas Bergeal, Gervasi Herranz, Alexei Kalaboukhov

Abstract: SrTiO$_3$-based conducting interfaces, which exhibit coexistence of gate-tunable 2D superconductivity and strong Rashba spin-orbit coupling (RSOC), are candidates to host topological superconductive phases. Yet, superconductivity is usually in the dirty limit, which tends to suppress nonconventional pairing and therefore challenges these expectations. Here we report on LaAlO$_3$/SrTiO$_3$ (LAO/STO… ▽ More SrTiO$_3$-based conducting interfaces, which exhibit coexistence of gate-tunable 2D superconductivity and strong Rashba spin-orbit coupling (RSOC), are candidates to host topological superconductive phases. Yet, superconductivity is usually in the dirty limit, which tends to suppress nonconventional pairing and therefore challenges these expectations. Here we report on LaAlO$_3$/SrTiO$_3$ (LAO/STO) interfaces with remarkably large mobility and mean free paths comparable to the superconducting coherence length, approaching the clean limit for superconductivity. We further show that the carrier density, mobility, and formation of the superconducting condensate are controlled by the fine-tuning of La/Al chemical ratio in the LAO film. Interestingly, we find a region in the superconducting phase diagram where the critical temperature is not suppressed below the Lifshitz transition, at odds with previous experimental investigations. These findings point out the relevance of achieving a clean-limit regime to enhance the observation of unconventional pairing mechanisms in these systems △ Less

Submitted 25 January, 2024; originally announced January 2024.

Formation of Mn-rich interfacial phases in Co2FexMn1-xSi thin films

Authors: Ka Ming Law, Arashdeep S. Thind, Mihir Pendharkar, Sahil J. Patel, Joshua J. Phillips, Chris J. Palmstrom, Jaume Gazquez, Albina Borisevich, Rohan Mishra, Adam J. Hauser

Abstract: We report the formation of Mn-rich regions at the interface of Co2FexMn1-xSi thin films grown on GaAs substrates by molecular beam epitaxy (MBE). Scanning transmission electron microscopy (STEM) with electron energy loss (EEL) spectrum imaging reveals that each interfacial region: (1) is 1-2 nm wide, (2) occurs irrespective of the Fe/Mn composition ratio and in both Co-rich and Co-poor films, and… ▽ More We report the formation of Mn-rich regions at the interface of Co2FexMn1-xSi thin films grown on GaAs substrates by molecular beam epitaxy (MBE). Scanning transmission electron microscopy (STEM) with electron energy loss (EEL) spectrum imaging reveals that each interfacial region: (1) is 1-2 nm wide, (2) occurs irrespective of the Fe/Mn composition ratio and in both Co-rich and Co-poor films, and (3) displaces both Co and Fe indiscriminately. We also observe a Mn-depleted region in each film directly above each Mn-rich interfacial layer, roughly 3 nm in width in the x = 0 and x = 0.3 films, and 1 nm in the x = 0.7 (less Mn) film. We posit that growth energetics favor Mn diffusion to the interface even when there is no significant Ga interdiffusion into the epitaxial film. Element-specific X-ray magnetic circular dichroism (XMCD) measurements show larger Co, Fe, and Mn orbital to spin magnetic moment ratios compared to bulk values across the Co2FexMn1-xSi compositional range. The values lie between reported values for pure bulk and nanostructured Co, Fe, and Mn materials, corroborating the non-uniform, layered nature of the material on the nanoscale. Finally, SQUID magnetometry demonstrates that the films deviate from the Slater-Pauling rule for uniform films of both the expected and the measured composition. The results inform a need for care and increased scrutiny when forming Mn-based magnetic thin films on III-V semiconductors like GaAs, particularly when films are on the order of 5 nm or when interface composition is critical to spin transport or other device applications. △ Less

Submitted 24 December, 2023; originally announced December 2023.

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

Authors: Milena Cervo Sulzbach, Huan Tan, Saul Estandia, Jaume Gazquez, Florencio Sanchez, Ignasi Fina, Josep Fontcuberta

Abstract: 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 implementatio… ▽ More 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. △ Less

Submitted 23 August, 2021; originally announced August 2021.

Journal ref: ACS Appl. Electron. Mater. 2021

Critical Effect of Bottom Electrode on Ferroelectricity of Epitaxial Hf0.5Zr0.5O2 Thin Films

Authors: Saul Estandia, Jaume Gazquez, Maria Varela, Nico Dix, Mengdi Qian, Raul Solanas, Ignasi Fina, Florencio Sanchez

Abstract: Epitaxial orthorhombic Hf0.5Zr0.5O2 (HZO) films on La0.67Sr0.33MnO3 (LSMO) electrodes show robust ferroelectricity, with high polarization, endurance and retention. However, no similar results have been achieved using other perovskite electrodes so far. Here, LSMO and other perovskite electrodes are compared. A small amount of orthorhombic phase and low polarization is found in HZO films grown on… ▽ More Epitaxial orthorhombic Hf0.5Zr0.5O2 (HZO) films on La0.67Sr0.33MnO3 (LSMO) electrodes show robust ferroelectricity, with high polarization, endurance and retention. However, no similar results have been achieved using other perovskite electrodes so far. Here, LSMO and other perovskite electrodes are compared. A small amount of orthorhombic phase and low polarization is found in HZO films grown on La-doped BaSnO3 and Nb-doped SrTiO3, while null amounts of orthorhombic phase and polarization are detected in films on LaNiO3 and SrRuO3. The critical effect of the electrode on the stabilized phases is not consequence of differences in the electrode lattice parameter. The interface is critical, and engineering the HZO bottom interface on just a few monolayers of LSMO permits the stabilization of the orthorhombic phase. Furthermore, while the specific divalent ion (Sr or Ca) in the manganite is not relevant, reducing the La content causes a severe reduction of the amount of orthorhombic phase and the ferroelectric polarization in the HZO film. △ Less

Submitted 18 February, 2021; originally announced February 2021.

Comments: Open access, published (2021) in Journal of Materials Chemistry C

Crystal Engineering and Ferroelectricity at the Nanoscale in Epitaxial 1D Manganese Oxide on Silicon

Authors: Andrés Gomez, José Manuel Vila-Fungueiriño, Claire Jolly, Ricardo Garcia-Bermejo, Judith Oró-Solé, Etienne Ferain, Narcís Mestres, César Magén, Jaume Gazquez, Juan Rodriguez-Carvajal, Adrián Carretero-Genevrier

Abstract: Ferroelectric oxides have attracted much attention due to their wide range of applications, especially in electronic devices such as nonvolatile memories and tunnel junctions. As a result, the monolithic integration of these materials into silicon technology and its nanostructuration to develop alternative cost-effective processes are among the central points in current technology. In this work, w… ▽ More Ferroelectric oxides have attracted much attention due to their wide range of applications, especially in electronic devices such as nonvolatile memories and tunnel junctions. As a result, the monolithic integration of these materials into silicon technology and its nanostructuration to develop alternative cost-effective processes are among the central points in current technology. In this work, we used a chemical route to obtain nanowire thin films of a novel Sr1+δMn8O16 (SMO) hollandite-type manganese oxide on silicon. Scanning transmission electron microscopy combined with crystallographic computing reveals a crystal structure comprising hollandite and pyrolusite units sharing the edges of their MnO6 octahedra, resulting in three types of tunnels arranged along the c axis, where ordering of the Sr atoms produces a natural symmetry breaking. The novel structure gives rise to a ferroelectricity and piezoelectricity, as revealed by local Direct Piezoelectric Force Microscopy measurements, which confirmed the ferroelectric nature of SMO nanowire thin films at room temperature and showed a piezoelectric coefficient d33 value of 22,6 pC/N. Moreover, we proved that flexible vertical SMO nanowires can be harvested and converted into electric output energy through the piezoelectric effect, showing an excellent deformability and high interface recombination. This work indicates the possibility of engineering the integration of 1D manganese oxides on silicon, a step which precedes the production of microelectronic devices. △ Less

Submitted 31 December, 2020; v1 submitted 7 July, 2020; originally announced July 2020.

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

Authors: Milena Cervo Sulzbach, Saúl Estandía, Xiao Long, Jike Lyu, Nico Dix, Jaume Gàzquez, Matthew F. Chisholm, Florencio Sánchez, Ignasi Fina, Josep Fontcuberta

Abstract: 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… ▽ More 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. △ Less

Submitted 12 June, 2020; originally announced June 2020.

Journal ref: Adv. Electron. Mater. 2020, 6, 1900852

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

Authors: Milena Cervo Sulzbach, Saúl Estandía, Jaume Gàzquez, Florencio Sánchez, Ignasi Fina, Josep Fontcuberta

Abstract: 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 polarizat… ▽ More 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. △ Less

Submitted 12 June, 2020; originally announced June 2020.

Journal ref: Advanced Functional Materials 2020, 2002638

Enhancement in Thermally Generated Spin Voltage at Pd/NiFe$_2$O$_4$ Interfaces by the Growth on Lattice-Matched Substrates

Authors: A. Rastogi, Z. Li, A. V. Singh, S. Regmi, T. Peters, P. Bougiatioti, D. Carsten né Meier, J. B. Mohammadi, B. Khodadadi, T. Mewes, R. Mishra, J. Gazquez, A. Y. Borisevich, Z. Galazka, R. Uecker, G. Reiss, T. Kuschel, A. Gupta

Abstract: Efficient spin injection from epitaxial ferrimagnetic NiFe$_2$O$_4$ thin films into a Pd layer is demonstrated via spin Seebeck effect measurements in the longitudinal geometry. The NiFe$_2$O$_4$ films (60 nm to 1 $μ$m) are grown by pulsed laser deposition on isostructural spinel MgAl$_2$O$_4$, MgGa$_2$O$_4$, and CoGa$_2$O$_4$ substrates with lattice mismatch varying between 3.2% and 0.2%. For the… ▽ More Efficient spin injection from epitaxial ferrimagnetic NiFe$_2$O$_4$ thin films into a Pd layer is demonstrated via spin Seebeck effect measurements in the longitudinal geometry. The NiFe$_2$O$_4$ films (60 nm to 1 $μ$m) are grown by pulsed laser deposition on isostructural spinel MgAl$_2$O$_4$, MgGa$_2$O$_4$, and CoGa$_2$O$_4$ substrates with lattice mismatch varying between 3.2% and 0.2%. For the thinner films ($\leq$ 330 nm), an increase in the spin Seebeck voltage is observed with decreasing lattice mismatch, which correlates well with a decrease in the Gilbert damping parameter as determined from ferromagnetic resonance measurements. High resolution transmission electron microscopy studies indicate substantial decrease of antiphase boundary and interface defects that cause strain-relaxation, i.e., misfit dislocations, in the films with decreasing lattice mismatch. This highlights the importance of reducing structural defects in spinel ferrites for efficient spin injection. It is further shown that angle-dependent spin Seebeck effect measurements provide a qualitative method to probe for in-plane magnetic anisotropies present in the films. △ Less

Submitted 1 June, 2020; originally announced June 2020.

Comments: 18 pages, 6 figures

Journal ref: Phys. Rev. Applied 14, 014014 (2020)

Rotational polarization nanotopologies in BaTiO3/SrTiO3 superlattices

Authors: Saul Estandia, Florencio Sanchez, Matthew F. Chisholm, Jaume Gazquez

Abstract: Ferroelectrics are characterized by domain structures as are other ferroics. At the nanoscale though, ferroelectrics may exhibit non-trivial or exotic polarization configurations under proper electrostatic and elastic conditions. These polar states may possess emerging properties not present in the bulk compounds and are promising for technological applications. Here, the observation of rotational… ▽ More Ferroelectrics are characterized by domain structures as are other ferroics. At the nanoscale though, ferroelectrics may exhibit non-trivial or exotic polarization configurations under proper electrostatic and elastic conditions. These polar states may possess emerging properties not present in the bulk compounds and are promising for technological applications. Here, the observation of rotational polarization topologies at the nanoscale by means of aberration-corrected scanning transmission electron microscopy is reported in BaTiO3/SrTiO3 superlattices grown on cubic SrTiO3(001). The transition from a highly homogeneous polarization state to the formation of rotational nanodomains has been achieved by controlling the superlattice period while maintaining compressive clamping of the superlattice to the cubic SrTiO3 substrate. The nanodomains revealed in BaTiO3 prove that its nominal tetragonal structure also allows rotational polar textures. △ Less

Submitted 14 November, 2019; originally announced November 2019.

Comments: Published in Nanoscale. Open access

Journal ref: Nanoscale, 2019, 11, 21275

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

Authors: Saul Estandia, Nico Dix, Jaume Gazquez, Ignasi Fina, Jike Lyu, Matthew F. Chisholm, Josep Fontcuberta, Florencio Sanchez

Abstract: 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, det… ▽ More 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. △ Less

Submitted 4 September, 2019; originally announced September 2019.

Journal ref: ACS Applied Electronic Materials, 1, 1449 (2019)

Nanostructure engineering of epitaxial piezoelectric α-quartz thin films on silicon

Authors: Q. Zhang, D. Sánchez-garcia, R. Desgarceaux, A. Gomez, P. Escofet-Majora, J. Oró-soler, J. Gazquez, G. Larrieu, B. Charlot, M. Gich, A. Carretero-Genevrier

Abstract: The monolithic integration of sub-micron quartz structures on silicon substrates is a key issue for the future development of telecommunication to the GHz frequencies. Here we report unprecedented large-scale fabrication of ordered arrays of piezoelectric epitaxial quartz nanostructures on silicon substrates by the combination of soft-chemistry and three cost effective lithographic techniques: (i)… ▽ More The monolithic integration of sub-micron quartz structures on silicon substrates is a key issue for the future development of telecommunication to the GHz frequencies. Here we report unprecedented large-scale fabrication of ordered arrays of piezoelectric epitaxial quartz nanostructures on silicon substrates by the combination of soft-chemistry and three cost effective lithographic techniques: (i) laser transfer lithography, (ii) soft nanoimprint lithography on Sr-doped SiO2 sol-gel thin films and (iii) self-assembled SrCO3 nanoparticles reactive nanomasks. Epitaxial α-quartz nanopillars with different diameters (down to 50 nm) and heights (up to 2000 nm) were obtained for the first time. This work proves the control over the shape, micro- and nano-patterning of quartz thin films while preserving its crystallinity, texture and piezoelectricity. This work opens up the opportunity to fabricate new high frequency resonators and high sensitivity sensors relevant in different fields of application. △ Less

Submitted 19 August, 2019; originally announced August 2019.

Enhanced ferroelectricity in epitaxial Hf0.5Zr0.5O2 thin films integrated with Si(001) using SrTiO3 templates

Authors: J. Lyu, I. Fina, R. Bachelet, G. Saint-Girons, S. Estandia, J. Gazquez, J. Fontcuberta, F. Sanchez

Abstract: SrTiO3 templates have been used to integrate epitaxial bilayers of ferroelectric Hf0.5Zr0.5O2 and La2/3Sr1/3MnO3 bottom electrode on Si(001). The Hf0.5Zr0.5O2 films show enhanced properties in comparison to equivalent films on SrTiO3(001) single crystalline substrates. The films, thinner than 10 nm, have very high remnant polarization of 34 uC/cm2. Hf0.5Zr0.5O2 capacitors at operating voltage of 4… ▽ More SrTiO3 templates have been used to integrate epitaxial bilayers of ferroelectric Hf0.5Zr0.5O2 and La2/3Sr1/3MnO3 bottom electrode on Si(001). The Hf0.5Zr0.5O2 films show enhanced properties in comparison to equivalent films on SrTiO3(001) single crystalline substrates. The films, thinner than 10 nm, have very high remnant polarization of 34 uC/cm2. Hf0.5Zr0.5O2 capacitors at operating voltage of 4 V present long retention time well beyond 10 years and high endurance against fatigue up to 109 cycles. The robust ferroelectric properties displayed by the epitaxial Hf0.5Zr0.5O2 films on Si(001) using SrTiO3 templates paves the way for the monolithic integration on silicon of emerging memory devices based on epitaxial HfO2. △ Less

Submitted 5 June, 2019; originally announced June 2019.

Journal ref: Applied Physics Letters 114, 222901 (2019)

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

Authors: Hari Babu Vasili, Matheus Gamino, Jaume Gazquez, Florencio Sanchez, Manuel Valvidares, Pierluigi Gargiani, Eric Pellegrin, Josep Fontcuberta

Abstract: 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 e… ▽ More 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. △ Less

Submitted 7 March, 2018; originally announced March 2018.

Comments: ACS Applied Materials & Interfaces, 2018 (under revision)

Report number: Vol. 10 (14), pp 12031--12041

Journal ref: ACS Appl. Mater. Interfaces 2018

Evaluation of microstructure and mechanical property variations in AlxCoCrFeNi high entropy alloys produced by a high-throughput laser deposition method

Authors: Mu Li, Jaume Gazquez, Albina Borisevich, Rohan Mishra, Katharine M. Flores

Abstract: Twenty-one distinct AlxCoCrFeNi alloys were rapidly prepared by laser alloying an equiatomic CoCrFeNi substrate with Al powder to create an alloy library ranging x=0.15-1.32. Variations in crystal structure, microstructure and mechanical properties were investigated using X-ray diffraction, scanning electron microscopy, scanning transmission electron microscopy and nanoindentation. With increasing… ▽ More Twenty-one distinct AlxCoCrFeNi alloys were rapidly prepared by laser alloying an equiatomic CoCrFeNi substrate with Al powder to create an alloy library ranging x=0.15-1.32. Variations in crystal structure, microstructure and mechanical properties were investigated using X-ray diffraction, scanning electron microscopy, scanning transmission electron microscopy and nanoindentation. With increasing Al content, the crystal structure transitioned from a disordered FCC to a mixture of disordered BCC and ordered B2 structures. While the onset of BCC/B2 formation was consistent with previously reported cast alloys, the FCC structure was observed at larger Al contents in the laser processed materials, resulting in a wider two phase regime. The FCC phase was primarily confined to the BCC/B2 grain boundaries at these high Al contents. The nanoindentation modulus and hardness of the FCC phase increased with Al content, while the properties of the BCC/B2 structure were insensitive to composition. The structure and mechanical properties of the laser-processed alloys were surprisingly consistent with reported results for cast alloys, demonstrating the feasibility of applying this high-throughput methodology to multicomponent alloy design. △ Less

Submitted 24 October, 2017; originally announced October 2017.

Comments: 20 pages, 8 figures and 1 table

Thermoelectric La-doped SrTiO3 epitaxial layers with single-crystal quality: from nanometer to micrometer and mosaicity effects

Authors: M. Apreutesei, R. Debord, M. Bouras, P. Regreny, C. Botella, A. Benamrouche, A. Carretero-Genevrier, J. Gazquez, G. Grenet, S. Pailhes, G. Saint-Girons, R. Bachelet

Abstract: High-quality thermoelectric LaxSr1-xTiO3 (LSTO) layers (here with x = 0.2), with thicknesses ranging from 20 nm to 700 nm, have been epitaxially grown on SrTiO3(001) substrates by enhanced solid-source oxide molecular-beam epitaxy. All films are atomically flat (with rms roughness < 0.2 nm), with low mosaicity (<0.1°), and present very low electrical resistivity (<5 x 10-4 ohm.cm at room temperatu… ▽ More High-quality thermoelectric LaxSr1-xTiO3 (LSTO) layers (here with x = 0.2), with thicknesses ranging from 20 nm to 700 nm, have been epitaxially grown on SrTiO3(001) substrates by enhanced solid-source oxide molecular-beam epitaxy. All films are atomically flat (with rms roughness < 0.2 nm), with low mosaicity (<0.1°), and present very low electrical resistivity (<5 x 10-4 ohm.cm at room temperature), one order of magnitude lower than commercial Nb-doped SrTiO3 single-crystalline substrate. The conservation of transport properties within this thickness range has been confirmed by thermoelectric measurements where Seebeck coefficients of around -60 microV/K have been found for all films, accordingly. Finally, a correlation is given between the mosaicity and the (thermo)electric properties. These functional LSTO films can be integrated on Si in opto-microelectronic devices as transparent conductor, thermoelectric elements or in non-volatile memory structures. △ Less

Submitted 28 March, 2017; originally announced March 2017.

Conducting interfaces between amorphous oxide layers and SrTiO3(110) and SrTiO3(111)

Authors: Mateusz Scigaj, Jaume Gazquez, Maria Varela, Josep Fontcuberta, Gervasi Herranz, Florencio Sanchez

Abstract: Interfaces between (110) and (111)SrTiO3 (STO) single crystalline substrates and amorphous oxide layers, LaAlO3 (a-LAO), Y:ZrO2 (a-YSZ), and SrTiO3 (a-STO) become conducting above a critical thickness tc. Here we show that tc for a-LAO is not depending on the substrate orientation, i.e. tc (a-LAO/(110)STO) ~ tc(a-LAO/(111)STO) interfaces, whereas it strongly depends on the composition of the amorp… ▽ More Interfaces between (110) and (111)SrTiO3 (STO) single crystalline substrates and amorphous oxide layers, LaAlO3 (a-LAO), Y:ZrO2 (a-YSZ), and SrTiO3 (a-STO) become conducting above a critical thickness tc. Here we show that tc for a-LAO is not depending on the substrate orientation, i.e. tc (a-LAO/(110)STO) ~ tc(a-LAO/(111)STO) interfaces, whereas it strongly depends on the composition of the amorphous oxide: tc(a-LAO/(110)STO) < tc(a-YSZ/(110)STO) < tc(a-STO/(110)STO). It is concluded that the formation of oxygen vacancies in amorphous-type interfaces is mainly determined by the oxygen affinity of the deposited metal ions, rather than orientational-dependent enthalpy vacancy formation and diffusion. Scanning transmission microscopy characterization of amorphous and crystalline LAO/STO(110) interfaces shows much higher amount of oxygen vacancies in the former, providing experimental evidence of the distinct mechanism of conduction in these interfaces. △ Less

Submitted 28 September, 2015; originally announced September 2015.

Journal ref: Solid State Ionics 281, 68 (2015)

Multiple-stable anisotropic magnetoresistance memory in antiferromagnetic MnTe

Authors: D. Kriegner, K. Vyborny, K. Olejnik, H. Reichlova, V. Novak, X. Marti, J. Gazquez, V. Saidl, P. Nemec, V. V. Volobuev, G. Springholz, V. Holy, T. Jungwirth

Abstract: A common perception assumes that magnetic memories require ferromagnetic materials with a non-zero net magnetic moment. However, it has been recently proposed that compensated antiferromagnets with a zero net moment may represent a viable alternative to ferromagnets. So far, experimental research has focused on bistable memories in antiferromagnetic metals. In the present work we demonstrate a mul… ▽ More A common perception assumes that magnetic memories require ferromagnetic materials with a non-zero net magnetic moment. However, it has been recently proposed that compensated antiferromagnets with a zero net moment may represent a viable alternative to ferromagnets. So far, experimental research has focused on bistable memories in antiferromagnetic metals. In the present work we demonstrate a multiple-stable memory device in epitaxial manganese telluride (MnTe) which is an antiferromagnetic counterpart of common II-VI semiconductors. Favorable micromagnetic characteristics of MnTe allow us to demonstrate a smoothly varying antiferromagnetic anisotropic magnetoresistance (AMR) with a harmonic angular dependence on the applied magnetic field, analogous to ferromagnets. The continuously varying AMR provides means for the electrical read-out of multiple-stable antiferromagnetic memory states which we set by heat-assisted magneto-recording and by changing the angle of the writing field. We explore the dependence of the magnitude of the zero-field read-out signal on the strength of the writing field and demonstrate the robustness of the antiferromagnetic memory states against strong magnetic field perturbations. We ascribe the multiple-stability in our antiferromagnetic memory to different distributions of domains with the Néel vector aligned along one of the three $c$-plane magnetic easy axes in the hexagonal MnTe film. The domain redistribution is controlled during the heat-assisted recording by the strength and angle of the writing field and freezes when sufficiently below the Néel temperature. △ Less

Submitted 20 August, 2015; originally announced August 2015.

Journal ref: Nature Communications 7,11623 (2016)

Multiferroic Iron Oxide Thin Films at Room-Temperature

Authors: Marti Gich, Ignasi Fina, Alessio Morelli, Florencio Sanchez, Marin Alexe, Jaume Gazquez, Josep Fontcuberta, Anna Roig

Abstract: In spite of being highly relevant for the development of a new generation of information storage devices, not many single-phase materials displaying magnetic and ferroelectric orders above room temperature are known. Moreover, these uncommon materials typically display insignificant values of the remanent moment in one of the ferroic orders or are complex multicomponent oxides which will be very c… ▽ More In spite of being highly relevant for the development of a new generation of information storage devices, not many single-phase materials displaying magnetic and ferroelectric orders above room temperature are known. Moreover, these uncommon materials typically display insignificant values of the remanent moment in one of the ferroic orders or are complex multicomponent oxides which will be very challenging to integrate in devices. Here we report on the strategy to stabilize the metastable epsilon-Fe2O3 in thin film form, and we show that besides its already known ferrimagnetic nature, the films are also ferroelectric at 300 K with a remanent polarization of 1 microC/cm2. The film polarization shows long retention times and can be switched under small applied voltages. These characteristics make of epsilon-Fe2O3 the first single-ion transition-metal oxide which is ferro(ferri)magnetic and ferroelectric at room temperature. The simple composition of this new multiferroic oxide and the discovery of a robust path for its thin film growth may boost the exploitation of epsilon-Fe2O3 in novel devices. △ Less

Submitted 19 May, 2014; originally announced May 2014.

Comments: 27 pages, 11 figures; Advanced Materials 2014

Tetragonal phase of epitaxial room-temperature antiferromagnet CuMnAs

Authors: P. Wadley, V. Novák, R. P. Campion, C. Rinaldi, X. Martí, H. Reichlová, J. Zelezný, J. Gazquez, M. A. Roldan, M. Varela, D. Khalyavin, S. Langridge, D. Kriegner, F. Máca, J. Masek, R. Bertacco, V. Holy, A. W. Rushforth, K. W. Edmonds, B. L. Gallagher, C. T. Foxon, J. Wunderlich, T. Jungwirth

Abstract: Recent studies have demonstrated the potential of antiferromagnets as the active component in spintronic devices. This is in contrast to their current passive role as pinning layers in hard disk read heads and magnetic memories. Here we report the epitaxial growth of a new high-temperature antiferromagnetic material, tetragonal CuMnAs, which exhibits excellent crystal quality, chemical order and c… ▽ More Recent studies have demonstrated the potential of antiferromagnets as the active component in spintronic devices. This is in contrast to their current passive role as pinning layers in hard disk read heads and magnetic memories. Here we report the epitaxial growth of a new high-temperature antiferromagnetic material, tetragonal CuMnAs, which exhibits excellent crystal quality, chemical order and compatibility with existing semiconductor technologies. We demonstrate its growth on the III-V semiconductors GaAs and GaP, and show that the structure is also lattice matched to Si. Neutron diffraction shows collinear antiferromagnetic order with a high Neél temperature. Combined with our demonstration of room-temperature exchange coupling in a CuMnAs/Fe bilayer, we conclude that tetragonal CuMnAs films are suitable candidate materials for antiferromagnetic spintronics. △ Less

Submitted 14 February, 2014; originally announced February 2014.

Comments: 16 pages, 5 figures, Published in Nature Communications (2013)

Journal ref: Nat. Commun. 4:2322

Orientational tuning of the 2D-superconductivity in LaAlO3/SrTiO3 interfaces

Authors: G. Herranz, N. Bergeal, J. Lesueur, J. Gazquez, M. Scigaj, N. Dix, F. Sanchez, J. Fontcuberta

Abstract: The discovery of a two-dimensional (2D) electron gas at the (110)-oriented LaAlO3/SrTiO3 in- terface provided us with the opportunity to probe the effect of crystallographic orientation and the ensuing electronic reconstructions on interface properties beyond the conventional (001)-orientation. At temperatures below 200 mK, we have measured 2D superconductivity with a spatial extension significant… ▽ More The discovery of a two-dimensional (2D) electron gas at the (110)-oriented LaAlO3/SrTiO3 in- terface provided us with the opportunity to probe the effect of crystallographic orientation and the ensuing electronic reconstructions on interface properties beyond the conventional (001)-orientation. At temperatures below 200 mK, we have measured 2D superconductivity with a spatial extension significantly larger (d approx. 24 - 30 nm) than previously reported for (001)-oriented LaAlO3/SrTiO3 interfaces (d approx. 10 nm). The more extended superconductivity brings about the absence of violation of the Pauli paramagnetic limit for the upper critical fields, signaling the distinctive nature of the electronic structure of the (110)-oriented interface with respect to their (001)-counterparts △ Less

Submitted 10 May, 2013; originally announced May 2013.

Comments: 5 pages, 5 figures

Storing magnetic information in IrMn/MgO/Ta tunnel junctions via field-cooling

Authors: D. Petti, E. Albisetti, H. Reichlová, J. Gazquez, M. Varela, M. Molina-Ruiz, A. F. Lopeandía, K. Olejník, V. Novák, I. Fina, B. Dkhil, J. Hayakawa, X. Marti, J. Wunderlich, T. Jungwirth, R. Bertacco

Abstract: Tunneling junctions containing no ferromagnetic elements have been fabricated and we show that distinct resistance states can be set by field cooling the devices from above the Néel along different orientations. Variations of the resistance up to 10% are found upon field cooling in applied fields of 2T, in-plane or out of plane. Below TN, we found that the metastable states are insensitive to magn… ▽ More Tunneling junctions containing no ferromagnetic elements have been fabricated and we show that distinct resistance states can be set by field cooling the devices from above the Néel along different orientations. Variations of the resistance up to 10% are found upon field cooling in applied fields of 2T, in-plane or out of plane. Below TN, we found that the metastable states are insensitive to magnetic fields thus constituting a memory element robust against external magnetic fields. Our work provides the demonstration of an electrically readable magnetic memory device, which contains no ferromagnetic elements and stores the information in an antiferromagnetic active layer. △ Less

Submitted 15 February, 2013; originally announced February 2013.

Solving and refining novel thin film phases using Cu X-ray radiation: the epitaxy-induced CuMnAs tetragonal phase

Authors: P. Wadley, A. Crespi, J. Gazquez, M. A. Roldan, P. Garcia, V. Novak, R. Campion, T. Jungwirth, C. Rinaldi, X. Marti, V. Holy, C. Frontera, J. Rius

Abstract: We present a combined experimental and computational method which enables the precise determination of the atomic positions in a thin film using CuKα radiation, only. The capabilities of this technique surpass simple structure refinement and allow solving unknown phases stabilized by substrate-induced stress. We derive the appropriate corrections to transform the measured integrated intensities in… ▽ More We present a combined experimental and computational method which enables the precise determination of the atomic positions in a thin film using CuKα radiation, only. The capabilities of this technique surpass simple structure refinement and allow solving unknown phases stabilized by substrate-induced stress. We derive the appropriate corrections to transform the measured integrated intensities into structure factors. Data collection was performed entirely on routinely available laboratory diffractometers (CuKα radiation); the subsequent analysis was carried out by single-crystal direct methods (δ recycling procedure) followed by the least-squares refinement of the structural parameters of the unit cell content. We selected an epitaxial thin film of CuMnAs grown on top of a GaAs substrate, which formed a crystal structure with tetragonal symmetry, differing from the bulk material which is orthorhombic. Here we demonstrate the new tetragonal form of epitaxial CuMnAs grown on GaAs substrate and present consistent high-resolution scanning transmission electron microscopy and stoichiometry analyses. △ Less

Submitted 22 January, 2013; originally announced January 2013.

Electron transfer and ionic displacements at the origin of the 2D electron gas at the LAO/STO interface: Direct measurements with atomic-column spatial resolution

Authors: C. Cantoni, J. Gazquez, F. Miletto Granozio, M. P. Oxley, M. Varela, A. R. Lupini, S. J. Pennycook, C. Aruta, U. Scotti di Uccio, P. Perna, D. Maccariello

Abstract: The discovery that the interface between two band gap insulators LaAlO3 and SrTiO3 is highly conducting has raised an enormous interest in the field of oxide electronics. The LAlO3/SrTiO3 interface can be tuned using an electric field and switched from a superconducting to an insulating state. Conducting paths in an insulating background can be written applying a voltage with the tip of an atomic… ▽ More The discovery that the interface between two band gap insulators LaAlO3 and SrTiO3 is highly conducting has raised an enormous interest in the field of oxide electronics. The LAlO3/SrTiO3 interface can be tuned using an electric field and switched from a superconducting to an insulating state. Conducting paths in an insulating background can be written applying a voltage with the tip of an atomic force microscope, creating great promise for the development of a new generation of nanoscale electronic devices. However, the mechanism for interface conductivity in LaAlO3/SrTiO3 has remained elusive. The theoretical explanation based on an intrinsic charge transfer (electronic reconstruction) has been strongly challenged by alternative descriptions based on point defects. In this work, thanks to modern aberration-corrected electron probes with atomic-scale spatial resolution, interfacial charge and atomic displacements originating the electric field within the system can be simultaneously measured, yielding unprecedented experimental evidence in favor of an intrinsic electronic reconstruction. △ Less

Submitted 20 June, 2012; originally announced June 2012.

Comments: Accepted for publication in Advanced Materials. Published online on 06/20/2012

Journal ref: Advanced Materials 24, 3952 (2012)

Conducting interfaces between band insulating oxides: the LaGaO3/SrTiO3

Authors: Paolo Perna, Davide Maccariello, Milan Radovic, Umberto Scotti di Uccio, Ilaria Pallecchi, Marta Codda, Daniele Marré, Claudia Cantoni, Jaume Gazquez, Maria Varela, Steve Pennycook, Fabio Miletto Granozio

Abstract: We show that the growth of the heterostructure LaGaO3/SrTiO3 yields the formation of a highly conductive interface. Our samples were carefully analyzed by high resolution electron microscopy, in order to assess their crystal perfection and to evaluate the abruptness of the interface. Their carrier density and sheet resistance are compared to the case of LaAlO3/SrTiO3 and a superconducting transiti… ▽ More We show that the growth of the heterostructure LaGaO3/SrTiO3 yields the formation of a highly conductive interface. Our samples were carefully analyzed by high resolution electron microscopy, in order to assess their crystal perfection and to evaluate the abruptness of the interface. Their carrier density and sheet resistance are compared to the case of LaAlO3/SrTiO3 and a superconducting transition is found. The results open the route to widening the field of polar-non polar interfaces, pose some phenomenological constrains to their underlying physics and highlight the chance of tailoring their properties for future applications by adopting suitable polar materials. △ Less

Submitted 1 October, 2010; v1 submitted 22 January, 2010; originally announced January 2010.

Comments: in press Appl. Phys. Lett. 97, 1 (2010)

Journal ref: APPLIED PHYSICS LETTERS 97, 152111 (2010)