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Stefano Gariglio

Publications and source records attributed to Stefano Gariglio.

At least 19 recordsLinked to original sources

Disentangling pre-transitional fluctuations in metallic VO2

VO2 features concomitant structural and metal-insulator transitions. This poses a challenge for understanding the underlying mechanism: is the transition triggered by a structural or by an electronic instability? The two scenarios are expected to produce very different pre-transitional fluctuations above TC. By combining magnetic susceptibility, IR reflectivity and X-ray diffuse scattering measurements, we observe that metallic VO2 features strong electronic and structural fluctuations towards the insulating monoclinic phase. By measuring resonant diffuse X-ray scattering across the Vanadium K-edge, we search for a potential decoupling between electronic and structural ordering in these fluctuations, finding no evidence of it. While our results do not completely rule out pure electronic fluctuations, they constrain them, favoring the interpretation that the VO2 metal-insulator transition is triggered by a structural instability. Our work offers a novel approach to solve similar problems in other strongly correlated systems.

cond-mat.str-el

Probing the quantum metric of 3D topological insulators

The surface states of 3D topological insulators possess geometric structures that imprint distinctive signatures on electronic transport. A prime example is the Berry curvature, which controls, for instance, electric frequency doubling via its higher order moments. In addition to the Berry curvature, topological surface states are expected to exhibit a nontrivial quantum metric, which plays a key role in governing nonlinear magnetotransport. However, its manifestation has yet to be experimentally observed and controlled in 3D topological insulators. Here, we provide evidence for a nonlinear response activated by the quantum metric of the topological surface states of Sb$_2$Te$_3$. We measure a time-reversal odd, nonlinear magnetoresistance that is independent from the temperature and the scattering time below 30 K, and is thus of intrinsic geometrical origin. This quantum metric magnetoresistance can be controlled by tuning the contributions of the top and bottom topological surface states by voltage gating. Our measurements thus demonstrate the existence and tunability of quantum geometry-induced transport in topological phases of matter and provide strategies for designing novel functionalities in topological devices.

cond-mat.mes-hall

The quantum metric of electrons with spin-momentum locking

Quantum materials are characterized by electromagnetic responses intrinsically linked to the geometry and topology of electronic wavefunctions, encoded in the quantum metric and Berry curvature. Whereas Berry curvature-mediated transport effects have been identified in several magnetic and nonmagnetic systems, quantum metric-induced transport phenomena remain limited to topological antiferromagnets. Here we show that spin-momentum locking -- a general characteristic of the electronic states at surfaces and interfaces of spin-orbit coupled materials -- leads to a finite quantum metric. This metric activates a nonlinear in-plane magnetoresistance that we measure and electrically control in 111-oriented LaAlO$_3$/SrTiO$_3$ interfaces. These findings demonstrate the existence of quantum metric effects in a vast class of materials and enable previously unexplored strategies to design functionalities based on quantum geometry.

cond-mat.mes-hall

Electric field control of superconducting fluctuations and quasiparticle interference at oxide interfaces

We investigate tunable superconducting transitions in (111)$\mathrm{LaAlO}_3/\mathrm{KTaO}_3$ field-effect devices. Large increases in conductivity, associated with superconducting fluctuations, are observed far above the transition temperature. However, the standard Aslamazov-Larkin paraconductivity model significantly underestimates the effect observed here. We use a model that includes conductivity corrections from normal state quasiparticle interference together with all contributions from superconducting fluctuations evaluated at arbitrary temperatures and in the short-wavelength limit. Through analysis of the magnetoconductance and resistive transitions, we find that the large conductivity increase can be explained by a combination of weak anti-localization and Maki-Thompson superconducting fluctuations. Both contributions are enabled by a strong temperature dependence of the electron's decoherence time compatible with an electron-phonon scattering scenario. We find that conductivity corrections are modulated by the electrostatic field effect, that governs a competition between normal-state quasiparticle interference and superconducting fluctuations.

cond-mat.supr-con

Curvature-Controlled Polarization in Adaptive Ferroelectric Membranes

In this study, we explore the ferroelectric domain structure and mechanical properties of PbTiO$_3$-based membranes, which develops a well-ordered and crystallographic-oriented ripple pattern upon release from their growth substrate. The ferrolectric domain structure of the PbTiO$_3$ layer was examined at various length scales using optical second harmonic generation, piezoresponse force microscopy, and scanning transmission electron microscopy. These methods reveal the presence of purely in-plane domains organized into superdomains at the crest of the ripples, while an in-plane/out-of-plane domain structure was observed in the flat regions separating the ripples, in agreement with phase-field simulations. The mechanical properties of the membrane were assessed using contact resonance force microscopy, which identified distinct mechanical behaviors at the ripples compared to the flat regions. This study shows that the physical properties of the ferroelectric layer in membranes can be locally controlled within an ordered array of ripples, with well-defined geometric characteristics.

cond-mat.mtrl-sci

Engineering Symmetry Breaking Interfaces by Nanoscale Structural-Energetics in Orthorhombic Perovskite Thin Films

The atomic configuration of phases and their interfaces is fundamental to materials design and engineering. Here, we unveil a transition metal oxide interface, whose formation is driven by energetic influences - epitaxial tensile strain versus oxygen octahedra connectivity - that compete in determining the orientation of an orthorhombic perovskite film. We study this phenomenon in a system of LaVO$_3$ grown on (101) DyScO$_3$, using atomic-resolution scanning transmission electron microscopy to measure intrinsic markers of orthorhombic symmetry. We identify that the film resolves this energetic conflict by switching its orientation by 90 degrees at an atomically-flat plane within its volume, not at the film/substrate interface. At either side of this "switching plane", characteristic orthorhombic distortions tend to zero to couple mismatched oxygen octahedra rotations. The resulting boundary is highly energetic, which makes it a priori unlikely; by using second-principles atomistic modeling, we show how its formation requires structural relaxation of an entire film grown beyond a critical thickness measuring tens of unit cells. The switching plane breaks the inversion symmetry of the Pnma orthorhombic structure, and sharply joins two regions, a thin intermediate layer and the film bulk, that are held under different mechanical strain states. By therefore contacting two distinct phases of one compound that would never otherwise coexist, this alternative type of interface opens new avenues for nanoscale engineering of functional systems, such as a chemically-uniform but magnetically inhomogeneous heterostructure.

cond-mat.mtrl-sci

High-field superconductivity from atomic-scale confinement and spin-orbit coupling at (111)$\mathrm{LaAlO_3/KTaO_3}$ interfaces

We study the superconducting critical fields of two-dimensional electron systems at (111)$\mathrm{LaAlO_3/KTaO_3}$ interfaces as a function of electrostatic back-gating. Our work reveals inplane critical fields of unprecedented magnitudes at oxide interfaces. By comparing the critical fields in-plane and out-of-plane we discover an extremely anisotropic superconductor with an effective thickness below 1 nm and a 12-fold violation of the Chandrasekhar-Clogston paramagnetic limit. The analysis of magneto-transport indicates that the enhancement of the critical fields is due to an exceptionally thin superconducting layer and to a paramagnetic susceptibility suppressed by spin-orbit scattering.

cond-mat.supr-con

Electron-Beam Writing of Atomic-Scale Reconstructions at Oxide Interfaces

The epitaxial growth of complex oxides enables the production of high-quality films, yet substrate choice is restricted to certain symmetry and lattice parameters, thereby limiting the technological applications of epitaxial oxides. In comparison, the development of free-standing oxide membranes gives opportunities to create novel heterostructures by non-epitaxial stacking of membranes, opening new possibilities for materials design. Here, we introduce a method for writing, with atomic precision, ionically bonded crystalline material across the gap between an oxide membrane and a carrier substrate. The process involves a thermal pre-treatment, followed by localized exposure to the raster scan of a scanning transmission electron microscopy (STEM) beam. STEM imaging and electron energy-loss spectroscopy show that we achieve atomically sharp interface reconstructions between a 30 nm-thick SrTiO${_3}$ membrane and a niobium-doped SrTiO${_3}$(001)-oriented carrier substrate. These findings indicate new strategies for fabricating synthetic heterostructures with novel structural and electronic properties.

cond-mat.mtrl-sci

Thermal and electrostatic tuning of surface phonon-polaritons in LaAlO3/SrTiO3 heterostructures

Phonon polaritons are promising for infrared applications due to a strong light-matter coupling and subwavelength energy confinement they offer. Yet, the spectral narrowness of the phonon bands and difficulty to tune the phonon polariton properties hinder further progress in this field. SrTiO3 - a prototype perovskite oxide - has recently attracted attention due to two prominent far-infrared phonon polaritons bands, albeit without any tuning reported so far. Here we show, using cryogenic infrared near-field microscopy, that long-propagating surface phonon polaritons are present both in bare SrTiO3 and in LaAlO3/SrTiO3 heterostructures hosting a two-dimensional electron gas. The presence of the two-dimensional electron gas increases dramatically the thermal variation of the upper limit of the surface phonon polariton band due to temperature dependent polaronic screening of the surface charge carriers. Furthermore, we demonstrate a tunability of the upper surface phonon polariton frequency in LaAlO3/SrTiO3 via electrostatic gating. Our results suggest that oxide interfaces are a new platform bridging unconventional electronics and long-wavelength nanophotonics.

cond-mat.mtrl-sci

Anomalous T-dependence of phonon lifetimes in metallic VO2

We investigate phonon lifetimes in VO2 single crystals. We do so in the metallic state above the metal-insulator transition (MIT), where strong structural fluctuations are known to take place. By combining inelastic X-ray scattering and Raman spectroscopy, we track the temperature dependence of several acoustic and optical phonon modes up to 1000 K. Contrary to what is commonly observed, we find that phonon lifetimes decrease with decreasing temperature. Our results show that pre-transitional fluctuations in the metallic state give rise to strong electron-phonon scattering that onsets hundreds of degrees above the transition and increases as the MIT is approached. Notably, this effect is not limited to specific points of reciprocal space that could be associated with the structural transition.

cond-mat.str-el

Characteristic lengthscales of the electrically-induced insulator-to-metal transition

Some correlated materials display an insulator-to-metal transition as the temperature is increased. In most cases this transition can also be induced electrically, resulting in volatile resistive switching due to the formation of a conducting filament. While this phenomenon has attracted much attention due to potential applications, many fundamental questions remain unaddressed. One of them is its characteristic lengths: what sets the size of these filaments, and how does this impact resistive switching properties. Here we use a combination of wide-field and scattering-type scanning near-field optical microscopies to characterize filament formation in NdNiO3 and SmNiO3 thin films. We find a clear trend: smaller filaments increase the current density, yielding sharper switching and a larger resistive drop. With the aid of numerical simulations, we discuss the parameters controlling the filament width and, hence, the switching properties.

cond-mat.mtrl-sci

A Laser-ARPES View of the 2D Electron Systems at LaAlO3/SrTiO3 and Al/SrTiO3 Interfaces

We have measured the electronic structure of the two-dimensional electron system (2DES) found at the Al/SrTiO3 (Al/STO) and LaAlO3/SrTiO3 (LAO/STO) interfaces by means of laser angle resolved photoemission spectroscopy, taking advantage of the large photoelectron escape depth at low photon energy to probe these buried interfaces. We demonstrate the possibility of tuning the electronic density in Al/STO by varying the Al layer thickness and show that the electronic structure evolution is well described by self-consistent tight binding supercell calculations, but differs qualitatively from a rigid band shift model. We show that both 2DES are strongly coupled to longitudinal optical phonons, in agreement with previous reports of a polaronic ground state in similar STO based 2DESs. Tuning the electronic density in Al/STO to match that of LAO/STO and comparing both systems, we estimate that the intrinsic LAO/STO 2DES has a bare band width of ~ 60 meV and a carrier density of ~ 6 10^13 cm-2.

cond-mat.mtrl-sci

Layered Metals as Polarized Transparent Conductors

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Transparent conductors are compromises between electrical conductivity, requiring mobile electrons, and optical transparency based on immobile charges to avoid screening of visible light. Technological solutions reflect this trade-off, achieving the desired transparencies by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. Materials with a quasi-two-dimensional electronic structure have a plasma edge well below the range of visible light while maintaining excellent in-plane conductivity. We demonstrate that slabs of the layered oxides Sr$_2$RuO$_4$ and Tl$_2$Ba$_2$CuO$_{6+δ}$ are optically transparent even at macroscopic thicknesses >2$μ$m for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens, that advancements in a-axis thin film growth will enable.

cond-mat.mtrl-sci

Electronic transport in sub-micrometric channels at the LaAlO$_{3}$/SrTiO$_{3}$ interface

Nanoscale channels realized at the conducting interface between LaAlO$_{3}$ and SrTiO$_{3}$ provide a perfect playground to explore the effect of dimensionality on the electronic properties of complex oxides. Here we compare the electric transport properties of devices realized using the AFM-writing technique and conventional photo-lithography. We find that the lateral size of the conducting paths has a strong effect on their transport behavior at low temperature. We observe a crossover from metallic to insulating regime occurring at about 50 K for channels narrower than 100 nm. The insulating upturn can be suppressed by the application of a positive backgate. We compare the behavior of nanometric constrictions in lithographically patterned channels with the result of model calculations and we conclude that the experimental observations are compatible with the physics of a quantum point contact.

cond-mat.mes-hall

High sensitivity variable-temperature infrared nanoscopy of conducting oxide interfaces

Probing the local transport properties of two-dimensional electron systems (2DES) confined at buried interfaces requires a non-invasive technique with a high spatial resolution operating in a broad temperature range. In this paper, we investigate the scattering-type scanning near field optical microscopy as a tool for studying the conducting LaAlO3/SrTiO3 interface from room temperature down to 6 K. We show that the near-field optical signal, in particular its phase component, is highly sensitive to the transport properties of the electron system present at the interface. Our modelling reveals that such sensitivity originates from the interaction of the AFM tip with coupled plasmon-phonon modes with a small penetration depth. The model allows us to quantitatively correlate changes in the optical signal with the variation of the 2DES transport properties induced by cooling and by electrostatic gating. To probe the spatial resolution of the technique, we image conducting nano-channels written in insulating heterostructures with a voltage-biased tip of an atomic force microscope.

cond-mat.str-el

Artificial quantum confinement in LAO3/STO heterostructure

Heterostructures of transition metal oxides (TMO) perovskites represent an ideal platform to explore exotic phenomena involving the complex interplay between the spin, charge, orbital and lattice degrees of freedom available in these compounds. At the interface between such materials, this interplay can lead to phenomena that are present in none of the original constituents such as the formation of the interfacial 2D electron system (2DES) discovered at the LAO3/STO3 (LAO/STO) interface. In samples prepared by growing a LAO layer onto a STO substrate, the 2DES is confined in a band bending potential well, whose width is set by the interface charge density and the STO dielectric properties, and determines the electronic band structure. Growing LAO (2 nm) /STO (x nm)/LAO (2 nm) heterostructures on STO substrates allows us to control the extension of the confining potential of the top 2DES via the thickness of the STO layer. In such samples, we explore the dependence of the electronic structure on the width of the confining potential using soft X-ray ARPES combined with ab-initio calculations. The results indicate that varying the thickness of the STO film modifies the quantization of the 3d t2g bands and, interestingly, redistributes the charge between the dxy and dxz/dyz bands.

cond-mat.str-el

Modulation of superconductivity by quantum confinement in doped strontium titanate

Quantum confinement in a thin-film geometry offers viable routes for tuning the critical properties of superconductors through modification of both density of states and pairing interaction. Low-density systems like doped strontium titanate are especially susceptible to these confinement-induced effects. In this paper, we show that the superconducting critical temperature $T_c$ is enhanced through quantum confinement in SrTiO$_3$/SrTi$_{1-x}$Nb$_x$O$_3$/SrTiO$_3$ heterostructures at $x=1\%$ concentration, by measuring resistivity transitions and the Hall carrier density for different thicknesses of the doped layer. We observe a nonmonotonic raise of $T_c$ with decreasing layer thickness at constant carrier density as estimated from the Hall effect. We analyze the results by solving a two-band model with a pairing interaction reproducing the density-dependent $T_c$ of doped SrTiO$_3$ in the bulk, that we confine to a potential well established self-consistently by the charged Nb dopants. The evolution of the theoretical $T_c$ with thickness agrees well with experiments. We point out the possible role of density inhomogeneities and suggest novel methods for engineering superconductivity in epitaxial thin films.

cond-mat.supr-con

Probing Quantum Confinement and Electronic Structure at Polar Oxide Interfaces

Polar discontinuities occurring at interfaces between two different materials constitute both a challenge and an opportunity in the study and application of a variety of devices. In order to cure the large electric field occurring in such structures, a reconfiguration of the charge landscape sets in at the interface via chemical modifications, adsorbates or charge transfer. In the latter case, one may expect a local electronic doping of one material: one sparkling example is the two-dimensional electron liquid (2DEL) appearing in SrTiO$_3$ once covered by a polar LaAlO$_3$ layer. Here we show that tuning the formal polarisation of a (La,Al)$_{1-x}$(Sr,Ti)$_x$O$_3$ (LASTO:$x$) overlayer through chemical composition modifies the quantum confinement of the 2DEL in SrTiO$_3$ and its electronic band structure. The analysis of the behaviour in magnetic field of superconducting field-effect devices reveals, in agreement with $ab\ initio$ calculations and self-consistent Poisson-Schrödinger modelling, that quantum confinement and energy splitting between electronic bands of different symmetries strongly depend on interface charge densities. These results not only strongly support the polar discontinuity mechanisms with a full charge transfer to explain the origin of the 2DEL at the celebrated LaAlO$_3$/SrTiO$_3$ interface, but also demonstrate an effective tool for tailoring the electronic structure at oxide interfaces.

cond-mat.mtrl-sci