For years, itinerant charge carriers in ferroelectric insulators were believed to completely quench ferroelectricity. Recent breakthroughs, however, demonstrated the existence of a novel class of quasi-two-dimensional polar metals with promising applications in nonvolatile electronics and spintronics. Here, by combining temperature-dependent magnetotransport measurements, optical second harmonic generation (SHG), resonant photoemission spectroscopy (ResPES), and X-ray absorption spectroscopy (XAS), we report on the properties of a BaTiO3-based oxide heterostructure, sustaining a persistent polar displacement in the BaTiO3 layer while supporting a two-dimensional electron gas. This suggests that the oxide heterostructure may operate as a polar metal system, paving the way for new developments in oxide-based electronics.
Several reports about infinite-layer nickelate thin films suggest that the superconducting critical temperature versus chemical doping phase diagram has a dome-like shape, similar to cuprates. Here, a highly reproducible superconducting state in undoped PrNiO2 thin films grown on SrTiO3 are demonstrated. Scanning transmission electron microscopy measurements show coherent infinite-layer phase with no visible stacking-fault defects, an overall high structural quality where possible unintentional chemical doping or interstitial oxygen, if present, sum well below the measurable threshold of the technique. X-ray absorption measurements show very sharp features at the Ni L3,2-edges with a large linear dichroism, indicating the preferential hole occupation of Ni1+-3 d x 2 - y 2 ${\rm d}_{x^2-y^2}$ orbitals in a square planar geometry. Resonant inelastic X-ray scattering measurements reveal sharp magnon excitations of 200 meV energy at the magnetic Brillouin zone boundary, highly resonant at the Ni1 + absorption peak. The results indicate that, when properly stabilized, infinite-layer nickelate thin films are superconducting without chemical doping.
We report scanning tunnelling microscopy (STM) and x-ray photoemission spectroscopy (XPS) measurements on uncapped and SrTiO3 (STO) capped NdNiO2 realized by pulsed-laser deposition and topotactic reduction process. We find that untreated NdNiO2 surfaces are insulating and contain Ni mostly in a nominal Ni2+ oxidation state. Room temperature STM shows signatures of a striped-like topographic pattern, possibly compatible with recent reports of ordered oxygen vacancies in uncapped nickelates due to incomplete oxygen de-intercalation of the upper layers. A metallic surface and a full Ni1+ oxidation state is recovered by ultra high vacuum annealing at 250 C, as shown by STM and XPS. STO-capped NdNiO2 films, on the other hand, show Ni mostly in Ni1+ configuration, but Nd 3d5/2 core level spectra have a relevant contribution from ligand 4f 4L states, suggesting the formation of a NdTiNiOx layer at the interface with the STO. By in situ unit-cell by unit-cell Ar-ion sputtering removal of the STO capping and of the non stoichiometric interface layer, we were able to address the surface electronic properties of these samples, as shown by high resolution valence band photoemission spectroscopy. The results provide insights in the properties of infinite-layer NdNiO2 thin films prepared by the CaH2 topotactic reduction of perovskite NdNiO3 and suggest methods to improve their surface quality.
We report an experimental study of the magnetic properties of infinite-layer Nd1-xSrxNiO2 thin films by x-ray magnetic circular dichroism (XMCD) at Ni L3,2 and Nd M5,4 edges. We show that at low temperatures the out-of-plane component of the Ni1+ spin-moment is characterized by a rapid increase for magnetic fields below 1T , followed by a slower linear increase reaching a spin-moment value of 0.25uB/Ni at 9T in the case of superconducting Nd0.8Sr0.2NiO2. On the other hand, the Nd M5,4 XMCD shows a clear paramagnetic behaviour, which make both Ni- and Nd-spin-sublattices fully uncorrelated.The magnetic field and temperature dependencies of the Ni L3,2 XMCD data can be explained by assuming an out-of-plane canting of the strongly in-plane anti-ferromagnetic ordered Ni1+ spins. A symmetry lowering of the NiO2 planes observed via four-dimensional scanning transmission electron microscopy, triggering a DMI, can be responsible of the proposed Ni1+ spin-canting at zero-field. The resulting out-of-plane weak-ferromagnetic coupling under magnetic field explains the relatively large spin-moment and its magnetic field and temperature dependence.
We use Resonant Inelastic X-ray Scattering (RIXS) to compare the doping dependence of magnetic excitations of an Infinite-Layer nickelate to those of a prototypical superconducting cuprate. The polarization analysis of RIXS spectra establishes the dominant spin-flip nature of the mid-infrared peak in both cases. Hole doping leads to opposite behavior of the magnetic energy in the two materials. By fitting the data with an original Hubbard-based model for dynamic susceptibility, we find that t is comparable in the two materials while U is about twice larger in the nickelate. This finding accounts for the smaller magnetic bandwidth of nickelates and for its decrease upon doping.
In a 2D electron system (2DES) the breaking of the inversion, time-reversal and bulk crystal-field symmetries is interlaced with the effects of spin-orbit coupling (SOC) triggering exotic quantum phenomena. Here, epitaxial engineering is used to design and realize a 2DES characterized simultaneously by ferromagnetic order, large Rashba SOC and hexagonal band warping at the (111) interfaces between LaAlO3, EuTiO3, and SrTiO3 insulators. The 2DES displays anomalous quantum corrections to the magneto-conductance driven by the time-reversal-symmetry breaking occurring below the magnetic transition temperature. The results are explained by the emergence of a non-trivial Berry phase and competing weak anti-localization/weak localization back-scattering of Dirac-like fermions, mimicking the phenomenology of gapped topological insulators. These findings open perspectives for the engineering of novel spin-polarized functional 2DES holding promises in spin-orbitronics and topological electronics.
The dataset contains X-ray absorption spectroscopy (XAS), electric polarization and magnetotransport measurements obtained on LaAlO3/EuTiO3/Ca:SrTiO3 heterostructures, at which interface a two-dimensional electron gas appears. X-ray magnetic circular dichroism (XMCD) extracted from the XAS data are also included, as well as X-ray linear dichroism (XLD) alongside atomic multiplet calculations for two sets of parameters corresponding to "up" and "down" remanent polarization states (data of Fig. 1 and 2).
We report on the effects of visible light on the low temperature electronic properties of the spin-polarized two dimensional electron system (2DES) formed at the interfaces between LaAlO $$_{3}$$ , EuTiO $$_{3}$$ and (001) SrTiO $$_{3}$$ . A strong, persistent modulation of both longitudinal and transverse conductivity was obtained using light emitting diodes (LEDs) with emissions at different wavelengths in the visible spectrum range. In particular, Hall effect data show that visible light induces a non-volatile electron filling of bands with mainly 3d $$_{xz,yz}$$ character, and at the same time an enhancement of the anomalous Hall effect associated to the magnetic properties of the system. Accordingly, a suppression of the weak-anti localization corrections to the magneto-conductance is found, which correlates with an enhancement of the spin-polarization and of the ferromagnetic character of 2DES. The results establish the LED-induced photo-doping as a viable route for the control of the ground state properties of artificial spin-polarized oxide 2DES.
We compute the spin-Hall conductance in a multiband model describing the two-dimensional electron gas formed at a LaAlO3/SrTiO3 interface in the presence of a finite concentration of impurities. Combining linear response theory with a systematic calculation of the impurity contributions to the self-energy, as well as to the vertex corrections of the relevant diagrams, we recover the full spin-Hall vs. sheet conductance dependence of LaAlO3/SrTiO3 as reported in Trier et al. [Nano Lett. 20, 395 (2020)], finding a very good agreement with the experimental data below and above the Lifshitz transition. In particular, we demonstrate that the multiband electronic structure leads to only a partial, instead of a complete, screening of the spin-Hall conductance, which decreases with increasing the carrier density. Our method can be generalized to other two-dimensional systems characterized by a broken inversion symmetry and multiband physics.
Multi-orbital physics in quasi-two-dimensional electron gases (q2DEGs) triggers intriguing 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 LaAlO3, EuTiO3 and SrTiO3 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)/3d(yz) orbital character in the EuTiO3 layer and at the interface with SrTiO3 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 emerging electronic phases and serve as a guide for the materials design of advanced electronic applications.
We present a 'top-down' patterning technique based on ion milling performed at low-temperature, for the realization of oxide two-dimensional electron system devices with dimensions down to 160 nm. Using electrical transport and scanning Superconducting QUantum Interference Device measurements we demonstrate that the low-temperature ion milling process does not damage the 2DES properties nor creates oxygen vacancies-related conducting paths in the STO substrate. As opposed to other procedures used to realize oxide 2DES devices, the one we propose gives lateral access to the 2DES along the in-plane directions, finally opening the way to coupling with other materials, including superconductors.
While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-Tc superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen K edge, we study the EPC in Bi2Sr2CaCu2O8+delta(Bi2212) and Nd1+xBa2-xCu3O7-delta (NBCO) at different doping levels ranging from heavily underdoped (p = 0.07) to overdoped (p = 0.21). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO chains and the CuO2 planes. Combining the results from the two families, we find the EPC strength decreases with doping at q(parallel to) = (-0.25, 0) r.l.u., but has a nonmonotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in d-wave pairing.
Interfacial inversion symmetry breaking gives rise to electronic properties that differ substantially from those of the bulk constituent materials. Here, we report on the realization of an artificial ferromagnetic quasi-two-dimensional electron gas (q2DEG) at the (111) interfaces between LaAlO3, EuTiO3, and SrTiO3 characterized by a reconstruction of the bulk quasioctahedral crystal field into a trigonal one. The q2DEG is created through a transfer of electrons to the EuTiO3 layers at the interface with LaAlO3, extending into the first layers of SrTiO3, as shown by an electron-energy-loss spectroscopy map of the titanium valence with atomic column resolution. Interestingly, polarized X-ray absorption spectroscopy shows that the Eu-4f and the Ti-3d magnetic moments order ferromagnetically and exhibit the same magnetic field dependence at low temperature. In addition, the q2DEG presents a sizable in -plane orbital moment even at low magnetic field (0.1 T) possibly related to Ti-3d electrons occupying bands with the main a1g orbital character. The results show an intriguing interplay between ferromagnetism, spin-orbit coupling, and trigonal crystal field splitting in the (111) LaAlO3/EuTiO3/SrTiO3 q2DEG.
Multiferroics are compounds in which at least two ferroic orders coexist - typically (anti)ferromagnetism and ferroelectricity. While magnetic order can arise in both insulating and conducting compounds, ferroelectricity is in principle not allowed in metals although a few two-dimensional (semi)metals were reported to behave as ferroelectrics. Yet, the combination with magnetic order to realize multiferroic metals remains elusive. Here, by combining x-ray spectroscopy and magnetotransport, we show the coexistence of ferroelectricity and magnetism in an oxide-based two-dimensional electron gas (2DEG). The data evidence a non-volatile switching of the polar displacements and of the anomalous Hall effect by the polarization direction, demonstrating a magnetoelectric coupling. Our findings provide new opportunities in quantum matter stemming from the interplay between ferroelectricity, ferromagnetism and Rashba spin-orbit coupling in a 2DEG.
Superconductivity in infinite-layer nickelates holds exciting analogies with that of cuprates, with similar structures and 3d-electron count. Using resonant inelastic x-ray scattering, we studied electronic and magnetic excitations and charge density correlations in Nd_{1-x}Sr_{x}NiO_{2} thin films with and without an SrTiO_{3} capping layer. We observe dispersing magnons only in the capped samples, progressively dampened at higher doping. We detect an elastic resonant scattering peak in the uncapped x=0 compound at wave vector (∼⅓,0), remindful of the charge order signal in hole doped cuprates. The peak weakens at x=0.05 and disappears in the superconducting x=0.20 film. The role of the capping on the electronic reconstruction far from the interface remains to be understood.
Studies on oxide quasi-two dimensional electron gas (q2DEG) have been a playground for the discovery of novel and sometimes unexpected phenomena, like the reported magnetism at the surface and at the interface between LaAlO$_{3}$ and SrTiO$_{3}$ non-magnetic materials. However, magnetism in this system is weak and there are evidences of a not intrinsic origin. Here, by using in-situ high-resolution angle resolved photoemission we demonstrate that ferromagnetic EuTiO$_{3}$, the magnetic counterpart of SrTiO$_{3}$ in the bulk, hosts a q2DEG at its (001) surface. This is confirmed by density functional theory calculations with Hubbard U terms in the presence of oxygen divacancies in various configurations, all of them leading to a spin-polarized q2DEG related to the ferromagnetic order of Eu-4f magnetic moments. The results suggest EuTiO$_{3}$(001) as a new material platform for oxide q2DEGs, characterized by broken inversion and time reversal symmetries.
The development of “fault-tolerant” quantum computers, unaffected by noise and decoherence, is one of the fundamental challenges in quantum technology. One of the approaches currently followed is the realization of “topologically protected” qubits which make use of quantum systems characterized by a degenerate ground state of composite particles, known as “non-Abelian anyons”, able to encode and manipulate quantum information in a non-local manner. In this paper, we discuss the potential of quasi-two-dimensional electron gas (q2DEG) at the interface between band insulating oxides, like LaAlO3 and SrTiO3, as an innovative technological platform for the realization of topological quantum systems. Being characterized by a unique combination of unconventional spin-orbit coupling, magnetism, and 2D-superconductivity, these systems naturally possess most of the fundamental characteristics needed for the realization of a topological superconductor. These properties can be widely tuned by electric field effect acting on the orbital splitting and occupation of the non-degenerate 3d xy and 3d xz, yz bands. The topological state in oxide q2DEGs quasi-one-dimensional nanochannels could be therefore suitably controlled, leading to conceptual new methods for the realization of a topological quantum electronics based on the tuning of the orbital degrees of freedom.
The electric-field control of d-electron magnetism in multiferroic transition metal oxides is attracting widespread interest for the underlying fundamental physics and for next generation spintronic devices. Here, we report an extensive study of the 3d magnetism in magnetoelectric Ga0.6Fe1.4O3 (GFO) epitaxial films by polarization dependent x-ray absorption spectroscopy. We found a non-zero integral of the x-ray magnetic circular dichroism, with a sign depending upon the relative orientation between the external magnetic field and the crystallographic axes. This finding translates in a sign-reversal between the average Fe magnetic orbital and spin moments. Large Fe-displacements, among some of the octahedral sites, lower the symmetry of the system producing anisotropic paths for the Fe-O bondings giving rise to a large orbital-lattice interaction akin to a preferential crystallographic direction for the magnetic orbital moment. The latter may lead to a partial re-orientation of the magnetic orbital moment under an external magnetic field that, combined to the ferrimagnetic nature of the GFO, can qualitatively explain the observed sign-reversal of the XMCD integral. The results suggest that a control over the local symmetry of the oxygen octahedra in transition metal oxides can offer a suitable leverage over the manipulation of the effective orbital and spin moments in magnetoelectric systems.
Studies on oxide quasi-two-dimensional electron gas (q2DEG) have been a playground for the discovery of novel and sometimes unexpected phenomena, like the reported magnetism at the surface of SrTiO3 (001) and at the interface between nonmagnetic LaAlO3 and SrTiO3 band insulators. However, magnetism in this system is weak and there is evidence of a nonintrinsic origin. Here, by using in situ high-resolution angle-resolved photoemission, we demonstrate that ferromagnetic EuTiO3, the magnetic counterpart of SrTiO3 in the bulk, hosts a q2DEG at its (001) surface. This is confirmed by density functional theory calculations with Hubbard U terms in the presence of oxygen divacancies in various configurations, all of them leading to a spin-polarized q2DEG related to the ferromagnetic order of Eu-4f magnetic moments. The results suggest EuTiO3(001) as a new material platform for oxide q2DEGs, characterized by broken inversion and time-reversal symmetries.
Electric-field effect control of two-dimensional electron gases (2-DEG) has enabled the exploration of nanoscale electron quantum transport in semiconductors. Beyond these classical materials, transition metal-oxide-based structures have d-electronic states favoring the emergence of novel quantum orders absent in conventional semiconductors. In this context, the LaAlO3/SrTiO3 interface that combines gate-tunable superconductivity and sizeable spin-orbit coupling is emerging as a promising platform to realize topological superconductivity. However, the fabrication of nanodevices in which the electronic properties of this oxide interface can be controlled at the nanoscale by field-effect remains a scientific and technological challenge. Here, we demonstrate the quantization of conductance in a ballistic quantum point contact (QPC), formed by electrostatic confinement of the LaAlO3/SrTiO3 2-DEG with a split-gate. Through finite source-drain voltage, we perform a comprehensive spectroscopic investigation of the 3d energy levels inside the QPC, which can be regarded as a spectrometer able to probe Majorana states in an oxide 2-DEG.