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Oxygen deficient titanium dioxide (TiO$_{2-x}$) is a very attractive material for several applications ranging from photocatalysis to resistive switching. Oxygen vacancies turn insulating anatase titanium dioxide into a polaronic conductor, while creating a defect state band below the ultraviolet semiconducting gap. Here we employ a combination of broadband infrared (IR) reflectivity and THz-pump/IR-probe measurements to investigate the relationship between localized defect states and delocalized conducting polaronic states. We show that the THz pump allows to convert deeply localized electrons into metastable polarons with a lifetime in the ns range. These long-lived metastable states may find application in novel opto-electronic applications exploiting the interplay of dc resistivity, with terahertz and infrared signals.

Metallic ferromagnetic transition metal dichalcogenides have emerged as important building blocks for scalable magnonics and memory applications. Downscaling such systems to the ultra-thin limit is critical to integrate them into technology. Here, we achieved layer-by-layer control over the transition metal dichalcogenide Cr$_{1.6}$Te$_{2}$ by using pulsed laser deposition, and we uncovered the minimum critical thickness above which room temperature magnetic order is maintained. The electronic and magnetic structure is explored experimentally and theoretically and it is shown that the films exhibit strong in-plane magnetic anisotropy as a consequence of large spin-orbit effects. Our study elucidates both magnetic and electronic properties of Cr$_{1.6}$Te$_{2}$, and corroborates the importance of intercalation to tune the magnetic properties of nanoscale materials architectures., Comment: 21 pages, 4 figures

The relation between crystal symmetries, electron correlations, and electronic structure steers the formation of a large array of unconventional phases of matter, including magneto-electric loop currents and chiral magnetism. Detection of such hidden orders is a major goal in condensed matter physics. However, to date, nonstandard forms of magnetism with chiral electronic ordering have been experimentally elusive. Here, we develop a theory for symmetry-broken chiral ground states and propose a methodology based on circularly polarized spin-selective angular-resolved photoelectron spectroscopy to probe them. We exploit the archetypal quantum material Sr2RuO4 and reveal spectroscopic signatures which, even though subtle, may be reconciled with the formation of spin-orbital chiral currents at the material surface. As we shed light on these chiral regimes, our findings pave the way for a deeper understanding of ordering phenomena and unconventional magnetism.

Knowledge of atomic-level details of structure, chemistry, and electronic states is paramount for a comprehensive understanding of emergent properties at oxide interfaces. We utilise a novel methodology based on atomic-scale electron energy loss spectroscopy (EELS) to spatially map the electronic states tied to the formation of a two-dimensional electron gas (2DEG) at the prototypical non-polar/polar $TiO_2$/$LaAlO_3$ interface. Combined with differential phase contrast analysis we directly visualise the microscopic locations of ions and charge and find that 2DEG states and $Ti^{3+}$ defect states exhibit different spatial distributions. Supported by density functional theory (DFT) and inelastic scattering simulations we examine the role of oxygen vacancies in 2DEG formation. Our work presents a general pathway to directly image emergent phenomena at interfaces using this unique combination of arising microscopy techniques with machine learning assisted data analysis procedures., Comment: 17 pages, 10 figures

Engineering surfaces and interfaces of materials promises great potential in the field of heterostructures and quantum matter designer, with the opportunity of driving new many-body phases that are absent in the bulk compounds. Here, we focus on the magnetic Weyl kagome system Co$_3$Sn$_2$S$_2$ and show how for different sample's terminations the Weyl-points connect also differently, still preserving the bulk-boundary correspondence. Scanning-tunnelling microscopy has suggested such a scenario indirectly. Here, we demonstrate this directly for the fermiology of Co$_3$Sn$_2$S$_2$, by linking it to the system real space surfaces distribution. By a combination of micro-ARPES and first-principles calculations, we measure the energy-momentum spectra and the Fermi surfaces of Co$_3$Sn$_2$S$_2$ for different surface terminations and show the existence of topological features directly depending on the top-layer electronic environment. Our work helps to define a route to control bulk-derived topological properties by means of surface electrostatic potentials, creating a realistic and reliable methodology to use Weyl kagome metals in responsive magnetic spintronics.

Intermetallics are an important playground to stabilize a large variety of physical phenomena, arising from their complex crystal structure. The ease of their chemical tuneabilty makes them suitable platforms to realize targeted electronic properties starting from the symmetries hidden in their unit cell. Here, we investigate the family of the recently discovered intermetallics MCo$_2$Al$_9$ (M: Sr, Ba) and we unveil their electronic structure for the first time. By using angle-resolved photoelectron spectroscopy and density functional theory calculations, we discover the existence of Dirac-like dispersions as ubiquitous features in this family, coming from the hidden kagome and honeycomb symmetries embedded in the unit cell. Finally, from calculations, we expect that the spin-orbit coupling is responsible for opening energy gaps in the electronic structure spectrum, which also affects the majority of the observed Dirac-like states. Our study constitutes the first experimental observation of the electronic structure of MCo$_2$Al$_9$ and proposes these systems as hosts of Dirac-like physics with intrinsic spin-orbit coupling. The latter effect suggests MCo$_2$Al$_9$ as a future platform for investigating the emergence of non-trivial topology.

Kagome materials have emerged as a setting for emergent electronic phenomena that encompass different aspects of symmetry and topology. It is debated whether the XV$_6$Sn$_6$ kagome family (where X is a rare earth element), a recently discovered family of bilayer kagome metals, hosts a topologically non-trivial ground state resulting from the opening of spin-orbit coupling gaps. These states would carry a finite spin-Berry curvature, and topological surface states. Here, we investigate the spin and electronic structure of the XV$_6$Sn$_6$ kagome family. We obtain evidence for a finite spin-Berry curvature contribution at the center of the Brillouin zone, where the nearly flat band detaches from the dispersing Dirac band because of spin-orbit coupling. In addition, the spin-Berry curvature is further investigated in the charge density wave regime of ScV$_6$Sn$_6$, and it is found to be robust against the onset of the temperature-driven ordered phase. Utilizing the sensitivity of angle resolved photoemission spectroscopy to the spin and orbital angular momentum, our work unveils the spin-Berry curvature of topological kagome metals, and helps to define its spectroscopic fingerprint., Comment: 21 pages, 4 figures

Long-range electronic order descending from a metallic parent state constitutes a rich playground to study the intricate interplay of structural and electronic degrees of freedom. With dispersive and correlation features as multifold as topological Dirac-like itinerant states, van-Hove singularities, correlated flat bands, and magnetic transitions at low temperature, kagome metals are located in the most interesting regime where both phonon and electronically mediated couplings are significant. Several of these systems undergo a charge density wave (CDW) transition, and the van-Hove singularities, which are intrinsic to the kagome tiling, have been conjectured to play a key role in mediating such an instability. However, to date, the origin and the main driving force behind this charge order is elusive. Here, we use the topological bilayer kagome metal ScV6Sn6 as a platform to investigate this puzzling problem, since it features both kagome-derived nested Fermi surface and van-Hove singularities near the Fermi level, and a CDW phase that affects the susceptibility, the neutron scattering, and the specific heat, similarly to the siblings AV3Sb5 (A = K, Rb, Cs) and FeGe. We report on our findings from high-resolution angle-resolved photoemission, density functional theory, and time-resolved optical spectroscopy to unveil the dynamics of its CDW phase. We identify the structural degrees of freedom to play a fundamental role in the stabilization of charge order. Along with a comprehensive analysis of the subdominant impact from electronic correlations, we find ScV6Sn6 to feature an instance of charge density wave order that predominantly originates from phonons. As we shed light on the emergent phonon profile in the low-temperature ordered regime, our findings pave the way for a deeper understanding of ordering phenomena in all CDW kagome metals.

Phase transitions are key in determining and controlling the quantum properties of correlated materials. Here, by using the powerful combination of precise material synthesis and angle resolved photoelectron spectroscopy, we show evidence for a genuine Mott transition undressed of any symmetry breaking side effects in the thin-films of V$_{2}$O$_{3}$. In particular, and in sharp contrast with the bulk V$_{2}$O$_{3}$ crystals, we unveil the purely electronic dynamics approaching the metal-insulator transition, disentangled from the structural transformation that is prevented by the residual substrate-induced strain. On approaching the transition, the spectral signal evolves surprisingly slowly over a wide temperature range, the Fermi wave-vector does not change, and the critical temperature appears to be much lower than the one reported for the bulk. Our findings are on one side fundamental in demonstrating the universal benchmarks of a genuine non-symmetry breaking Mott transition, extendable to a large array of correlated quantum systems and, on the other, given that the fatal structural breakdown is avoided, they hold promise of exploiting the metal-insulator transition by implementing V$_{2}$O$_{3}$ thin films in devices.

$V_2O_3$ has long been studied as a prototypical strongly correlated material. The difficulty in obtaining clean, well ordered surfaces, however, hindered the use of surface sensitive techniques to study its electronic structure. Here we show by mean of X-ray diffraction and electrical transport that thin films prepared by pulsed laser deposition can reproduce the functionality of bulk $V_2O_3$. The same films, when transferred in-situ, show an excellent surface quality as indicated by scanning tunnelling microscopy and low energy electron diffraction, representing a viable approach to study the metal-insulator transition (MIT) in $V_2O_3$ by means of angle-resolved photoemission spectroscopy. Combined, these two aspects pave the way for the use of $V_2O_3$ thin films in device-oriented heterostructures.

Two-dimensional (2D) metallic states induced by oxygen vacancies at oxide surfaces and interfaces provide new opportunities for the development of advanced applications, but the ability to control the behavior of these states is still limited. We used Angle Resolved Photoelectron Spectroscopy combined with density functional theory to study the reactivity of states induced by the oxygen vacancies at the (001)-(1x4) surface of anatase TiO2, where both 2D metallic and deeper lying in-gap states (IGs) are observed. Remarkably, the two states exhibit very different evolution when the surface is exposed to molecular O2: while IGs are almost completely quenched, the metallic states are only weakly affected. The energy scale analysis for the vacancy migration and recombination resulting from the DFT calculations confirms indeed that only the IGs originate from and remain localized at the surface, whereas the metallic states originate from subsurface vacancies, whose migration and recombination at the surface is energetically less favorable rendering them therefore insensitive to oxygen dosing.

We have grown untwinned YBa$_2$Cu$_3$O$_{7-\delta}$ (YBCO) films on (110) MgO substrates that were pre-annealed at high temperature in oxygen atmosphere. The annealing results in surface reconstruction with shallow facets, which induce the suppression of the YBCO twinning domains, and the preferential alignment of the CuO chains along one of the in-plane directions of the substrate. Because of the large mismatch between the in-plane lattice parameters of film and substrate, the strain induced by the MgO into the YBCO layer is strong and very peculiar. The YBCO film is compressed, with respect to the bulk, and presents a unidirectional buckling of the atomic planes, along the chains' direction, due to a deformation of the copper-oxygen octahedra. The YBCO films, which can be grown with thicknesses down to few unit cells and oxygen doping levels spanning most of the superconducting dome, are patterned into nanowires with dimensions down to 50 nm. The anisotropies due to the untwinning state are preserved in these structures; moreover, additional anisotropies appear, in ultrathin structures where strain effects become more pronounced. Such untwinned and compressively strained films can therefore be used as a platform to study the interplay between strain and the various local orders in the normal state of YBCO., Comment: 11 pages, 8 figures

We combine time resolved pump-probe Magneto-Optical Kerr Effect and Photoelectron Spectroscopy experiments supported by theoretical analysis to determine the relaxation dynamics of delocalized electrons in half-metallic ferromagnetic manganite $La_{1-x}Sr_{x}MnO_{3}$. We observe that the half-metallic character of $La_{1-x}Sr_{x}MnO_{3}$ determines the timescale of both the electronic phase transition and the quenching of magnetization, revealing a quantum isolation of the spin system in double exchange ferromagnets extending up to hundreds of picoseconds. We demonstrate the use of time-resolved hard X-ray photoelectron spectroscopy (TR-HAXPES) as a unique tool to single out the evolution of strongly correlated electronic states across a second-order phase transition in a complex material., Comment: Article 25 pages, 6 figures

Spintronics exploits the magnetoresistance effects to store or sense the magnetic information. Since the magnetoresistance strictly depends on the magnetic anisotropy of the system, it is fundamental to set a defined anisotropy to the system. Here, we investigate by means of vectorial Magneto-Optical Kerr Magnetometry (v-MOKE), half-metallic La0.67Sr0.33MnO3 (LSMO) thin films that exhibit at room temperature pure biaxial magnetic anisotropy if grown onto MgO (001) substrate with a thin SrTiO3 (STO) buffer. In this way, we can avoid unwanted uniaxial magnetic anisotropy contributions that may be detrimental for specific applications. The detailed study of the angular evolution of the magnetization reversal pathways, critical fields (coercivity and switching) allows for disclosing the origin of the magnetic anisotropy, which is magnetocrystalline in nature and shows four-fold symmetry at any temperature.

We report on the growth and characterization of ultrathin YBa$_2$Cu$_3$O$_{7-\delta}$ (YBCO) films on MgO (110) substrates, which exhibit superconducting properties at thicknesses down to 3 nm. YBCO nanowires, with thicknesses down to 10 nm and widths down to 65 nm, have been also successfully fabricated. The nanowires protected by a Au capping layer show superconducting properties close to the as-grown films, and critical current densities, which are only limited by vortex dynamics. The 10 nm thick YBCO nanowires without the Au capping present hysteretic current voltage characteristics, characterized by a voltage switch which drives the nanowires directly from the superconducting to the normal state. Such bistability is associated in NbN nanowires to the presence of localized normal domains within the superconductor. The presence of the voltage switch, in ultrathin nanostructures characterized by high sheet resistance values, though preserving high quality superconducting properties, make our nanowires very attractive devices to engineer single photon detectors., Comment: 12 pages, 8 figures