arXiv subjects

G. Herranz

Publications and source records attributed to G. Herranz.

At least 19 recordsLinked to original sources

arXiv2025

Emergent Orbital Dynamics in Strongly Spin-Orbit Coupled Systems

The interplay between spin and orbital degrees of freedom gives rise to a variety of emergent phases in correlated 4d and 5d transition-metal systems. Strong spin-orbit coupling (SOC) significantly alters Jahn-Teller (JT) physics, often suppressing static distortions or promoting dynamic fluctuations, thereby reducing or even quenching orbital polarization. While intersite hybridization is a fundamental aspect of crystalline solids, its role in shaping the dynamics of spin-orbit-entangled states has received comparatively little attention. Here, we show that electronic hopping can locally restore orbital polarization when the ground state is perturbed, even in the absence of static orbital order. Using a Matsubara lattice formalism, we analyze how local orbital perturbations propagate through correlated, spin-orbit-entangled systems. When intersite hopping is included, such perturbations induce short-range orbital polarization with a characteristic orthogonal response at nearest-neighbor sites. Although the energy scale of these hybridization-driven orbital reconstructions likely makes their detection challenging, they may still influence low-energy spectral features and interact with other excitations. These results underscore the importance of including orbital dynamics in the interpretation of spectroscopic data and provide a framework for understanding dynamical responses in spin-orbit-entangled materials.

cond-mat.str-el↗

arXiv2024

Superconductivity in the parent infinite-layer nickelate NdNiO$_2$

We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound NdNiO$_2$. A combination of oxide molecular-beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to its nodal order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity.

cond-mat.supr-con↗

arXiv2023

Absence of $3a_0$ Charge Density Wave Order in the Infinite Layer Nickelates

A hallmark of many unconventional superconductors is the presence of many-body interactions which give rise to broken symmetry states intertwined with superconductivity. Recent resonant soft x-ray scattering experiments report commensurate $3a_0$ charge density wave order in the infinite layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both the cuprates and nickelates. Here, we present x-ray scattering and spectroscopy measurements on a series of NdNiO$_{2+x}$ samples which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO$_2$. The $3a_0$ superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with 3 unit cell periodicity. The absence of any observable charge density wave order in NdNiO$_2$ highlights a crucial difference between the phase diagrams of the cuprate and nickelate superconductors.

cond-mat.supr-con↗

arXiv2018

Single-band to two-band superconductivity transition in two-dimensional oxide interfaces

In multiorbital materials, superconductivity can exhibit new exotic forms that include several coupled condensates. In this context, quantum confinement in two-dimensional superconducting oxide interfaces offers new degrees of freedom to engineer the band structure and selectively control 3d-orbitals occupancy by electrostatic doping. However, the presence of multiple superconducting condensates in these systems has not yet been demonstrated. Here, we use resonant microwave transport to extract the superfluid stiffness of the (110)-oriented LaAlO3/SrTiO3 interface in the entire phase diagram. We evidence a transition from single-band to two-band superconductivity driven by electrostatic doping, which we relate to the filling of the different 3d-orbitals based on numerical simulations of the quantum well. Interestingly, the superconducting transition temperature decreases while the second band is populated, which challenges the Bardeen-Cooper-Schrieffer theory. To explain this behaviour, we propose that the superconducting order parameters associated with the two bands have opposite signs with respect to each other.

cond-mat.supr-con↗

arXiv2017

Infrared ellipsometry study of the photo-generated charge carriers at the (001) and (110) surfaces of SrTiO$_3$ crystals and the interface of corresponding LaAlO$_3$/SrTiO$_3$ heterostructures

With infrared (IR) ellipsometry and DC resistance measurements we investigated the photo-doping at the (001) and (110) surfaces of SrTiO$_3$ (STO) single crystals and at the corresponding interfaces of LaAlO$_3$/SrTiO$_3$ (LAO/STO) heterostructures. In the bare STO crystals we find that the photo-generated charge carriers, which accumulate near the (001) surface, have a similar depth profile and sheet carrier concentration as the confined electrons that were previously observed in LAO/STO (001) heterostructures. A large fraction of these photo-generated charge carriers persist at low temperature at the STO (001) surface even after the UV light has been switched off again. These persistent charge carriers seem to originate from oxygen vacancies that are trapped at the structural domain boundaries which develop below the so-called antiferrodistortive transition at T* = 105 K. This is most evident from a corresponding photo-doping study of the DC transport in STO (110) crystals for which the concentration of these domain boundaries can be modified by applying a weak uniaxial stress. The oxygen vacancies and their trapping by defects are also the source of the electrons that are confined to the interface of LAO/STO (110) heterostructures which likely do not have a polar discontinuity as in LAO/STO (001). In the former, the trapping and clustering of the oxygen vacancies also has a strong influence on the anisotropy of the charge carrier mobility. We show that this anisotropy can be readily varied and even inverted by various means, such as a gentle thermal treatment, UV irradiation, or even a weak uniaxial stress. Our experiments suggest that extended defects, which develop over long time periods (of weeks to months), can strongly influence the response of the confined charge carriers at the LAO/STO (110) interface.

cond-mat.str-el↗

arXiv2016

Multiple strain-induced phase transitions in LaNiO3 thin films

Strain effects on epitaxial thin films of LaNiO3 grown on different single crystalline substrates are studied by Raman scattering and first-principles simulation. New Raman modes, not present in bulk or fully-relaxed films, appear under both compressive and tensile strains, indicating symmetry reductions. Interestingly, the Raman spectra and the underlying crystal symmetry for tensile and compressively strained films are different. Extensive mapping of LaNiO3 phase stability is addressed by simulations, showing that a variety of crystalline phases are indeed stabilized under strain which may impact the electronic orbital hierarchy. The calculated Raman frequencies reproduce the principal features of the experimental spectra, supporting the validity of the multiple strain-driven structural transitions predicted by the simulations.

cond-mat.mtrl-sci↗

arXiv2014

Laterally-confined two-dimensional electron gases in self-patterned LaAlO3/SrTiO3 interfaces

A bottom-up process has been used to engineer the LaAlO3/SrTiO3 interface atomic composition and locally confine the two-dimensional electron gas to lateral sizes in the order of 100 nm. This is achieved by using SrTiO3(001) substrate surfaces with self-patterned chemical termination, which is replicated by the LaAlO3 layer, resulting in a modulated LaO/TiO2 and AlO2/SrO interface composition. We demonstrate the confinement of the conducting interface forming either long-range ordered nanometric stripes or isolated regions. Our results demonstrate that engineering the interface chemical termination is a suitable strategy towards nanoscale lateral confinement of two-dimensional high-mobility systems.

cond-mat.mtrl-sci↗

arXiv2013

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

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

cond-mat.str-el↗

arXiv2013

X-ray interference effects on the determination of structural data in ultrathin La2/3Sr1/3MnO3 epitaxial thin films

We analyze X-ray diffraction data used to extract cell parameters of ultrathin films on closely matching substrates. We focus on epitaxial La2/3Sr1/3MnO3 films grown on (001) SrTiO3 single crystalline substrates. It will be shown that, due to extremely high structural similarity of film and substrate, data analysis must explicitly consider the distinct phase of the diffracted waves by substrate and films to extract reliable unit cell parameters. The implications of this finding for the understanding of strain effects in ultrathin films and interfaces will be underlined

cond-mat.mtrl-sci↗

arXiv2010

Unveiling a two-dimensional electron gas with universal subbands at the surface of SrTiO3

Similar to silicon that is the basis of conventional electronics, strontium titanate (SrTiO3) is the bedrock of the emerging field of oxide electronics. SrTiO3 is the preferred template to create exotic two-dimensional (2D) phases of electron matter at oxide interfaces, exhibiting metal-insulator transitions, superconductivity, or large negative magnetoresistance. However, the physical nature of the electronic structure underlying these 2D electron gases (2DEGs) remains elusive, although its determination is crucial to understand their remarkable properties. Here we show, using angle-resolved photoemission spectroscopy (ARPES), that there is a highly metallic universal 2DEG at the vacuum-cleaved surface of SrTiO3, independent of bulk carrier densities over more than seven decades, including the undoped insulating material. This 2DEG is confined within a region of ~5 unit cells with a sheet carrier density of ~0.35 electrons per a^2 (a is the cubic lattice parameter). We unveil a remarkable electronic structure consisting on multiple subbands of heavy and light electrons. The similarity of this 2DEG with those reported in SrTiO3-based heterostructures and field-effect transistors suggests that different forms of electron confinement at the surface of SrTiO3 lead to essentially the same 2DEG. Our discovery provides a model system for the study of the electronic structure of 2DEGs in SrTiO3-based devices, and a novel route to generate 2DEGs at surfaces of transition-metal oxides.

cond-mat.mtrl-sci↗

arXiv2009

Dynamical response and confinement of the electrons at the LaAlO3/SrTiO3 interface

With infrared ellipsometry and transport measurements we investigated the electrons at the interface between LaAlO3 and SrTiO3. We obtained a sheet carrier density of Ns~5-9x 10E13 cm^-2, an effective mass of m*~3m_e, and a strongly frequency dependent mobility. The latter are similar as in bulk SrTi1-xNbxO3 and therefore suggestive of polaronic correlations of the confined carriers. We also determined the vertical density profile which has a strongly asymmetric shape with a rapid initial decay over the first 2 nm and a pronounced tail that extends to about 11 nm.

cond-mat.mtrl-sci↗

arXiv2009

Towards two-dimensional metallic behavior at LaAlO3/SrTiO3 interfaces

Using a low-temperature conductive-tip atomic force microscope in cross-section geometry we have characterized the local transport properties of the metallic electron gas that forms at the interface between LaAlO3 and SrTiO3. At low temperature, we find that the carriers do not spread away from the interface but are confined within ~10 nm, just like at room temperature. Simulations taking into account both the large temperature and electric-field dependence of the permittivity of SrTiO3 predict a confinement over a few nm for sheet carrier densities larger than ~6 10^13 cm-2. We discuss the experimental and simulations results in terms of a multi-band carrier system. Remarkably, the Fermi wavelength estimated from Hall measurements is ~16 nm, indicating that the electron gas in on the verge of two-dimensionality.

cond-mat.mtrl-sci↗

arXiv2008

Mapping the Spatial Distribution of Charge Carriers in LaAlO3/SrTiO3 Heterostructures

At the interface between complex insulating oxides, novel phases with interesting properties may occur, such as the metallic state reported in the LaAlO3/SrTiO3 system. While this state has been predicted and reported to be confined at the interface, some works indicate a much broader spatial extension, thereby questioning its origin. Here we provide for the first time a direct determination of the carrier density profile of this system through resistance profile mappings collected in cross-section LaAlO3/SrTiO3 samples with a conducting-tip atomic force microscope (CT-AFM). We find that, depending upon specific growth protocols, the spatial extension of the high-mobility electron gas can be varied from hundreds of microns into SrTiO3 to a few nanometers next to the LaAlO3/SrTiO3 interface. Our results emphasize the potential of CT-AFM as a novel tool to characterize complex oxide interfaces and provide us with a definitive and conclusive way to reconcile the body of experimental data in this system.

cond-mat.mtrl-sci↗

arXiv2007

High Mobility in LaAlO3/SrTiO3 Heterostructures: Origin, Dimensionality and Perspectives

We have investigated the dimensionality and origin of the magnetotransport properties of LaAlO3 films epitaxially grown on TiO2-terminated SrTiO3(001) substrates. High mobility conduction is observed at low deposition oxygen pressures (PO2 < 10^-5 mbar) and has a three-dimensional character. However, at higher PO2 the conduction is dramatically suppressed and nonmetallic behavior appears. Experimental data strongly support an interpretation of these properties based on the creation of oxygen vacancies in the SrTiO3 substrates during the growth of the LaAlO3 layer. When grown on SrTiO3 substrates at low PO2, other oxides generate the same high mobility as LaAlO3 films. This opens interesting prospects for all-oxide electronics.

cond-mat.mtrl-sci↗

arXiv2006

Tunnel magnetoresistance and robust room temperature exchange bias with multiferroic BiFeO3 epitaxial thin films

We report on the functionalization of multiferroic BiFeO3 epitaxial films for spintronics. A first example is provided by the use of ultrathin layers of BiFeO3 as tunnel barriers in magnetic tunnel junctions with La2/3Sr1/3MnO3 and Co electrodes. In such structures, a positive tunnel magnetoresistance up to 30% is obtained at low temperature. A second example is the exploitation of the antiferromagnetic spin structure of a BiFeO3 film to induce a sizeable (~60 Oe) exchange bias on a ferromagnetic film of CoFeB, at room temperature. Remarkably, the exchange bias effect is robust upon magnetic field cycling, with no indications of training.

cond-mat.str-el↗

arXiv2006

Origin and Perspectives of High Mobility in LaAlO3/SrTiO3 Structures

LaAlO3/SrTiO3 structures showing high mobility conduction have recently aroused large expectations as they might represent a major step towards the conception of all-oxide electronics devices. For the development of these technological applications a full understanding of the dimensionality and origin of the conducting electronic system is crucial. To shed light on this issue, we have investigated the magnetotransport properties of a LaAlO3 layer epitaxially grown at low oxygen pressure on a TiO2-terminated (001)-SrTiO3 substrate. In agreement with recent reports, a low-temperature mobility of about 10^4 cm2/Vs has been found. We conclusively show that the electronic system is three-dimensional, excluding any interfacial confinement of carriers. We argue that the high-mobility conduction originates from the doping of SrTiO3 with oxygen vacancies and that it extends over hundreds of microns into the SrTiO3 substrate. Such high mobility SrTiO3-based heterostructures have a unique potential for electronic and spintronics devices.

cond-mat.mtrl-sci↗

arXiv2005

Full oxide heterostructure combining a high-Tc diluted ferromagnet with a high-mobility conductor

We report on the growth of heterostructures composed of layers of the high-Curie temperature ferromagnet Co-doped (La,Sr)TiO3 (Co-LSTO) with high-mobility SrTiO3 (STO) substrates processed at low oxygen pressure. While perpendicular spin-dependent transport measurements in STO//Co-LSTO/LAO/Co tunnel junctions demonstrate the existence of a large spin polarization in Co-LSTO, planar magnetotransport experiments on STO//Co-LSTO samples evidence electronic mobilities as high as 10000 cm2/Vs at T = 10 K. At high enough applied fields and low enough temperatures (H < 60 kOe, T < 4 K) Shubnikov-de Haas oscillations are also observed. We present an extensive analysis of these quantum oscillations and relate them with the electronic properties of STO, for which we find large scattering rates up to ~ 10 ps. Thus, this work opens up the possibility to inject a spin-polarized current from a high-Curie temperature diluted oxide into an isostructural system with high-mobility and a large spin diffusion length.

cond-mat.mtrl-sci↗

arXiv2005

Combining half-metals and multiferroics into epitaxial heterostructures for spintronics

We report on the growth of epitaxial bilayers of the La2/3Sr1/3MnO3 (LSMO) half-metallic ferromagnet and the BiFeO3 (BFO) multiferroic, on SrTiO3(001) by pulsed laser deposition. The growth mode of both layers is two-dimensional, which results in unit-cell smooth surfaces. We show that both materials keep their properties inside the heterostructures, i.e. the LSMO layer (11 nm thick) is ferromagnetic with a Curie temperature of ~330K, while the BFO films shows ferroelectricity down to very low thicknesses (5 nm). Conductive-tip atomic force microscope mappings of BFO/LSMO bilayers for different BFO thicknesses reveal a high and homogeneous resistive state for the BFO film that can thus be used as a ferroelectric tunnel barrier in tunnel junctions based on a half-metal.

cond-mat.mtrl-sci↗