arXiv subjects

F. Miletto Granozio

Publications and source records attributed to F. Miletto Granozio.

At least 19 recordsLinked to original sources

arXiv2025

Uncovering surface states of the Dirac semimetal BaMg2Bi2

BaMg2Bi2 is a Dirac semimetal characterized by a simple Dirac cone crossing the Fermi level at the center of the Brillouin zone, protected by C3 rotational symmetry. Together with its Sr-based analogue SrMg2Bi2, it has been proposed as a promising candidate for a chemically driven topological switch: while SrMg2Bi2 is an insulator, BaMg2Bi2 exhibits non-trivial topological features. A detailed understanding of its electronic structure is essential to elucidate its electronic and transport properties. Previous photoemission studies confirmed the Dirac nature of BaMg2Bi2, but were limited to high photon energies, which hindered direct comparison with density functional theory calculations (DFT), due to reduced resolution and higher-frequency matrix-element modulation in that regime. In this work, we combine high-resolution angle-resolved photoemission spectroscopy (ARPES) and DFT calculations to get full insight on the valence band states, providing a comprehensive picture of the low-energy electronic structure. Our measurements reveal the presence of previously unobserved surface states. We found that they are topologically trivial, but they unlock a more comprehensive understanding of the material's behavior, reconciling previous discrepancies between experiment and theory.

cond-mat.str-el↗

arXiv2021

Orbital selective switching of ferromagnetism in an oxide quasi two-dimensional electron gas

Multi-orbital physics in quasi-two-dimensional electron gases (q2DEGs) triggers unique phenomena not observed in bulk materials, such as unconventional superconductivity and magnetism. Here, we investigate the mechanism of orbital selective switching of the spin-polarization in the oxide q2DEG formed at the (001) interface between the LaAlO$_{3}$, EuTiO$_{3}$ and SrTiO$_{3}$ band insulators. By using density functional theory calculations, transport, magnetic and x-ray spectroscopy measurements, we find that the filling of titanium-bands with 3d$_{xz,yz}$ orbital character in the EuTiO3 layer and at the interface with SrTiO$_{3}$ induces an antiferromagnetic to ferromagnetic switching of the exchange interaction between Eu-4f$^{7}$ magnetic moments. The results explain the observation of the carrier density dependent ferromagnetic correlations and anomalous Hall effect in this q2DEG, and demonstrate how combined theoretical and experimental approaches can lead to a deeper understanding of novel electronic phases and serve as a guide for the materials design for advanced electronic applications.

cond-mat.mtrl-sci↗

arXiv2019

Electronic phase separation at LaAlO3/SrTiO3 interfaces tunable by oxygen deficiency

Electronic phase separation is crucial for the fascinating macroscopic properties of the LaAlO3/SrTiO3 (LAO/STO) paradigm oxide interface, including the coexistence of superconductivity and ferromagnetism. We investigate this phenomenon using angle-resolved photoelectron spectroscopy (ARPES) in the soft-X-ray energy range, where the enhanced probing depth combined with resonant photoexcitation allow access to fundamental electronic structure characteristics (momentum-resolved spectral function, dispersions and ordering of energy bands, Fermi surface) of buried interfaces. Our experiment uses X-ray irradiation of the LAO/STO interface to tune its oxygen deficiency, building up a dichotomic system where mobile weakly correlated Ti t2g-electrons co-exist with localized strongly correlated Ti eg-ones. The ARPES spectra dynamics under X-ray irradiation shows a gradual intensity increase under constant Luttinger count of the Fermi surface. This fact identifies electronic phase separation (EPS) where the mobile electrons accumulate in conducting puddles with fixed electronic structure embedded in an insulating host phase, and allows us to estimate the lateral fraction of these puddles. We discuss the physics of EPS invoking a theoretical picture of oxygen-vacancy clustering, promoted by the magnetism of the localized Ti eg-electrons, and repelling of the mobile t2g-electrons from these clusters. Our results on the irradiation-tuned EPS elucidate the intrinsic one taking place at the stoichiometric LAO/STO interfaces.

cond-mat.mtrl-sci↗

arXiv2018

Symmetry breaking at the (111) interfaces of SrTiO${_3}$ hosting a 2D-electron system

We used x-ray absorption spectroscopy to study the orbital symmetry and the energy band splitting of (111) LaAlO${_3}$/SrTiO${_3}$ and LaAlO${_3}$/EuTiO${_3}$/SrTiO${_3}$ heterostructures, hosting a quasi two-dimensional electron system (q2DES), and of a Ti-terminated (111) SrTiO${_3}$ single crystal, also known to form a q2DES at its surface. We demonstrate that the bulk tetragonal Ti-3d D${_4}$${_h}$ crystal field is turned into trigonal D${_3}$${_d}$ crystal field in all cases. The symmetry adapted a${_1}$${_g}$ and e${^π_g}$ orbitals are non-degenerate in energy and their splitting, Δ, is positive at the bare STO surface but negative in the heterostructures, where the a${_1}$${_g}$ orbital is lowest in energy. These results demonstrate that the interfacial symmetry breaking induced by epitaxial engineering of oxide interfaces has a dramatic effect on their electronic properties, and it can be used to manipulate the ground state of the q2DES.

cond-mat.mtrl-sci↗

arXiv2018

Infrared study of the quasi-two-dimensional electron system at the interface between SrTiO$_{3}$ and crystalline or amorphous LaAlO$_3$

We have used grazing-angle infrared spectroscopy to detect the Berreman effect (BE) in the quasi-two-dimensional electron system (q-2DES) which forms spontaneously at the interface between SrTiO$_{3}$ (STO) and a thin film of LaAlO$_3$ (LAO). From the BE, which allows one to study longitudinal optical excitations in ultrathin films like the q-2DES, we have extracted at different temperatures its thickness, the charge density and mobility of the carriers under crystalline LAO (sample A), and the charge density under amorphous LAO (sample B). This quantity turns out to be higher than in sample A, but a comparison with Hall measurements shows that under amorphous LAO the charges are partly localized at low $T$ with a low activation energy (about 190 K in $k_B$ units), and are thermally activated according to a model for large polarons. The thickness of the q-2DES extracted from our spectra turns out to be 4 $\pm 1$ nm for crystalline LAO, 7 $\pm 2$ nm for amorphous LAO.

cond-mat.mtrl-sci↗

arXiv2016

Octahedral rotation patterns in strained EuFeO3 and other Pbnm perovskite films: Implications for hybrid improper ferroelectricity

We report the relationship between epitaxial strain and the crystallographic orientation of the in-phase rotation axis and A-site displacements in Pbnm-type perovskite films. Synchrotron diffraction measurements of EuFeO3 films under strain states ranging from 2% compressive to 0.9% tensile on cubic or rhombohedral substrates exhibit a combination of a-a+c- and a+a-c- rotational patterns. We compare the EuFeO3 behavior with previously reported experimental and theoretical work on strained Pbnm-type films on non-orthorhombic substrates, as well as additional measurements from LaGaO3, LaFeO3, and Eu0.7Sr0.3MnO3 films on SrTiO3. Compiling the results from various material systems reveals a general strain dependence in which compressive strain strongly favors a-a+c- and a+a-c- rotation patterns and tensile strain weakly favors a-a-c+ structures. In contrast, EuFeO3 films grown on Pbnm-type GdScO3 under 2.3% tensile strain take on a uniform a-a+c- rotation pattern imprinted from the substrate, despite strain energy considerations that favor the a-a-c+ pattern. These results point to the use of substrate imprinting as a more robust route than strain for tuning the crystallographic orientations of the octahedral rotations and A-site displacements needed to realize rotation-induced hybrid improper ferroelectricity in oxide heterostructures.

cond-mat.mtrl-sci↗

arXiv2014

Growth and characterization of conducting LaAlO3/EuTiO3/SrTiO3 het-erostructures

We studied the structural, magnetic and transport properties of LaAlO3/EuTiO3/SrTiO3 heterostructures grown by Pulsed Laser Deposition. The samples have been characterized in-situ by electron diffraction and scanning probe mi-croscopy and ex-situ by transport measurements and x-ray absorption spectroscopy. LaAlO3/EuTiO3/SrTiO3 films show a ferromagnetic transition at T<7.5 K, related to the ordering of Eu2+ spins, even in samples characterized by just two EuTiO3 unit cells. A finite metallic conductivity is observed only in the case of samples composed by one or two EuTiO3 unit cells and, simultaneously, by a LaAlO3 thickness equal or above 4 unit cells. The role of ferromagnetic EuTiO3 on the transport properties of delta-doped LaAlO3/EuTiO3/SrTiO3 is critically discussed.

cond-mat.mtrl-sci↗

arXiv2013

Carrier-number fluctuations in the 2-dimensional electron gas at the LaAlO3/SrTiO3 interface

The voltage-spectral density SV(f) of the 2-dimensional electron gas formed at the interface of LaAlO3 /SrTiO3 has been thoroughly investigated. The low-frequency component has a clear 1/f behavior with a quadratic bias current dependence, attributed to resistance fluctuations. However, its temperature dependence is inconsistent with the classical Hooge model, based on carrier-mobility fluctuations. The experimental results are, instead, explained in terms of carrier-number fluctuations, due to an excitation-trapping mechanism of the 2-dimensional electron gas.

cond-mat.str-el↗

arXiv2012

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

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.

cond-mat.str-el↗

arXiv2012

Observation of a two-dimensional electron gas at the surface of annealed SrTiO3 single crystals by scanning tunneling spectroscopy

Scanning tunneling spectroscopy suggests the formation of a two dimensional electron gas (2DEG) on the TiO2 terminated surface of undoped SrTiO3 single crystals annealed at temperature lower than 400 °C in ultra high vacuum conditions. Low energy electron diffraction indicates that the 2D metallic SrTiO3 surface is not structurally reconstructed, suggesting that non-ordered oxygen vacancies created in the annealing process introduce carriers leading to an electronic reconstruction. The experimental results are interpreted in a frame of competition between oxygen diffusion from the bulk to the surface and oxygen loss from the surface itself.

cond-mat.mtrl-sci↗

arXiv2011

Revealing the ortho-II Band Folding in YBa2Cu3O7-delta Films

We present an angle-resolved photoelectron spectroscopy study of YBa2Cu3O7-delta films in situ grown by pulsed laser deposition. We have successfully produced underdoped surfaces with ordered oxygen vacancies within the CuO chains resulting in a clear ortho-II band folding of the Fermi surface. This indicates that order within the CuO chains affects the electronic properties of the CuO2 planes. Our results highlight the importance of having not only the correct surface carrier concentration, but also a very well ordered and clean surface in order that photoemission data on this compound be representative of the bulk.

cond-mat.supr-con↗

arXiv2011

In-situ Investigation of the Early Stage of TiO2 epitaxy on (001) SrTiO3

We report on a systematic study of the growth of epitaxial TiO2 films deposited by pulsed laser deposition on Ti-terminated (001) SrTiO3 single crystals. By using in-situ reflection high energy electron diffraction, low energy electron diffraction, x-ray photoemission spectroscopy and scanning probe microscopy, we show that the stabilization of the anatase (001) phase is preceded by the growth of a pseudomorphic Sr-Ti-O intermediate layer, with a thickness between 2 and 4 nm. The data demonstrate that the formation of this phase is related to the activation of long range Sr migration from the substrate to the film. The role of interface Gibbs energy minimization, as a driving force for Sr diffusion, is discussed. Our results enrich the phase diagram of the Sr-Ti-O system under epitaxial strain opening the roudeficient SrTiO phase.

cond-mat.mtrl-sci↗

arXiv2010

Energy and symmetry of $dd$ excitations in undoped layered cuprates measured by Cu $L_3$ resonant inelastic x-ray scattering

We measured high resolution Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS) of the undoped cuprates La$_2$CuO$_4$, Sr$_2$CuO$_2$Cl$_2$, CaCuO$_2$ and NdBa$_2$Cu$_3$O$_6$. The dominant spectral features were assigned to $dd$ excitations and we extensively studied their polarization and scattering geometry dependence. In a pure ionic picture, we calculated the theoretical cross sections for those excitations and used them to fit the experimental data with excellent agreement. By doing so, we were able to determine the energy and symmetry of Cu-3$d$ states for the four systems with unprecedented accuracy and confidence. The values of the effective parameters could be obtained for the single ion crystal field model but not for a simple two-dimensional cluster model. The firm experimental assessment of $dd$ excitation energies carries important consequences for the physics of high $T_c$ superconductors. On one hand, having found that the minimum energy of orbital excitation is always $\geq 1.4$ eV, i.e., well above the mid-infrared spectral range, leaves to magnetic excitations (up to 300 meV) a major role in Cooper pairing in cuprates. On the other hand, it has become possible to study quantitatively the effective influence of $dd$ excitations on the superconducting gap in cuprates.

cond-mat.supr-con↗

arXiv2010

Pulsed laser deposition of SrTiO3/LaGaO3 and SrTiO3/LaAlO3: plasma plume effects

Pulsed laser deposition of SrTiO3/LaGaO3 and SrTiO3/LaAlO3 interfaces has been analyzed with a focus on the kinetic energy of the ablated species. LaGaO3 and LaAlO3 plasma plumes were studied by fast photography and space-resolved optical emission spectroscopy. Reflection high energy electron diffraction was performed proving a layer-by-layer growth up to 10-1 mbar oxygen pressure. The role of the energetic plasma plume on the two-dimensional growth and the presence of interfacial defects at different oxygen growth pressure has been discussed in view of the conducting properties developing at such polar/non-polar interfaces.

cond-mat.mtrl-sci↗

arXiv2010

Magnetic properties of pseudomorphic epitaxial films of Pr_{0.7}Ca_{0.3}MnO_3 under different biaxial tensile stresses

In order to analyse the effect of strain on the magnetic properties of narrow-band manganites, the temperature and field dependent susceptibilities of about 8.5 nm thick epitaxial Pr0.7Ca0.3MnO3 films, respectively grown on (001) and (110) SrTiO3 substrates, have been compared. For ultrathin samples grown on (001) SrTiO3, a bulk-like cluster-glass magnetic behaviour is found, indicative of the possible coexistence of antiferromagnetic and ferromagnetic phases. On the contrary, ultrathin films grown on (110) substrates show a robust ferromagnetism, with a strong spontaneous magnetization of about 3.4 mB /Mn atom along the easy axis. On the base of high resolution reciprocal space mapping analyses performed by x-ray diffraction, the different behaviours are discussed in terms of the crystallographic constraints imposed by the epitaxy of Pr0.7Ca0.3MnO3 on SrTiO3. We suggest that for growth on (110) SrTiO3, the tensile strain on the film c-axis, lying within the substrate plane, favours the ferromagnetic phase, possibly by allowing a mixed occupancy and hybridization of both in-plane and out-of-plane eg orbitals. Our data allow to shed some physics of inhomogeneous states in manganites and on the nature of their ferromagnetic insulating state.

cond-mat.mtrl-sci↗

arXiv2009

Polar catastrophe and electronic reconstructions at the LaAlO3/SrTiO3 interface: evidence from optical second harmonic generation

The so-called "polar catastrophe", a sudden electronic reconstruction taking place to compensate for the interfacial ionic polar discontinuity, is currently considered as a likely factor to explain the surprising conductivity of the interface between the insulators LaAlO3 and SrTiO3. We applied optical second harmonic generation, a technique that a priori can detect both mobile and localized interfacial electrons, to investigating the electronic polar reconstructions taking place at the interface. As the LaAlO3 film thickness is increased, we identify two abrupt electronic rearrangements: the first takes place at a thickness of 3 unit cells, in the insulating state; the second occurs at a thickness of 4-6 unit cells, i.e., just above the threshold for which the samples become conducting. Two possible physical scenarios behind these observations are proposed. The first is based on an electronic transfer into localized electronic states at the interface that acts as a precursor of the conductivity onset. In the second scenario, the signal variations are attributed to the strong ionic relaxations taking place in the LaAlO3 layer.

cond-mat.mtrl-sci↗

arXiv2009

Charge density waves enhance the electronic noise of manganites

The transport and noise properties of Pr_{0.7}Ca_{0.3}MnO_{3} epitaxial thin films in the temperature range from room temperature to 160 K are reported. It is shown that both the broadband 1/f noise properties and the dependence of resistance on electric field are consistent with the idea of a collective electrical transport, as in the classical model of sliding charge density waves. On the other hand, the observations cannot be reconciled with standard models of charge ordering and charge melting. Methodologically, it is proposed to consider noise-spectra analysis as a unique tool for the identification of the transport mechanism in such highly correlated systems. On the basis of the results, the electrical transport is envisaged as one of the most effective ways to understand the nature of the insulating, charge-modulated ground states in manganites.

cond-mat.str-el↗

arXiv2008

Dispersing bimagnons and doping induced bimagnon-charge modes in superconducting cuprates

In the early days of high temperature superconductivity it was already recognized that magnetic properties of these materials are intimately related to the superconducting ones . When doped, the long-range ordered antiferromagnetic background of pristine copper-oxide insulators melts away and makes room for a spin liquid and superconductivity. By resonant inelastic x-ray scattering (RIXS) in the soft regime we probe the hitherto inaccessible dynamical multiple-spin correlations of the magnetic background in a series of parent compounds and in high Tc materials [NCCO (Nd2-xCexCuO4) and LSCO (La2-xSrxCuO4)]. High resolution measurements allows the clear observation of dispersing bimagnon excitations. In the undoped compounds the theory, fits the data on these coherent spin excitations without free parameters. In nearly optimally doped LSCO we observe the appearance of a new collective excitation at an energy of 250 +/- 60 meV having the signature of a coupled bimagnon-charge mode. It has a strongly reduced dispersion and lies in a so far unexplored region of momentum and energy space in the mid-infrared.

cond-mat.str-el↗