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.
Sandeep Kumar Chaluvadi, Shyni Punathum Chalil, Anupam Jana, Deepak Dagur, Giovanni Vinai, Federico Motti, Jun Fujii, Moussa Mezhoud, Ulrike Lüders, Vincent Polewczyk, Ivana Vobornik, Giorgio Rossi, Chiara Bigi, Younghun Hwang, Thomas Olsen, Pasquale Orgiani, Federico Mazzola 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.
Federico Mazzola, Wojciech Brzezicki, Maria Teresa Mercaldo, Anita Guarino, Chiara Bigi, Jill A. Miwa, Domenico De Fazio, Alberto Crepaldi, Jun Fujii, Giorgio Rossi, Pasquale Orgiani, Sandeep Kumar Chaluvadi, Shyni Punathum Chalil, Giancarlo Panaccione, Anupam Jana, Vincent Polewczyk, Ivana Vobornik, Changyoung Kim, Fabio Miletto Granozio, Rosalba Fittipaldi, et al (3) 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.
F. Mazzola, H. Hassani, D. Amoroso, S.K. Chaluvadi, J. Fujii, V. Polewczyk, P. Rajak, Max Koegler, R. Ciancio, B. Partoens, G. Rossi, I. Vobornik, P. Ghosez, P. Orgiani WO$_3$ is a binary 5d compound which has attracted remarkable attention due to the vast array of structural transitions that it undergoes in its bulk form. In the bulk, a wide range of electronic properties has been demonstrated, including metal-insulator transitions and superconductivity upon doping. In this context, the synthesis of WO$_3$ thin films holds considerable promise for stabilizing targeted electronic phase diagrams and embedding them in technological applications. However, to date, the electronic structure of WO$_3$ thin films is experimentally unexplored, and only characterized by numerical calculations. Underpinning such properties experimentally would be important to understand not only the collective behavior of electrons in this transition metal oxide, but also to explain and engineer both the observed optical responses to carriers' concentration and its prized catalytic activity. Here, by means of tensile strain, we stabilize WO$_3$ thin films into a stable phase, which we call pseudo-tetragonal, and we unveil its electronic structure by combining photoelectron spectroscopy and density functional theory calculations. This study constitutes the experimental demonstration of the electronic structure of WO$_3$ thin-films and allows us to pin down the first experimental benchmarks of the fermiology of this system.
Federico Mazzola, Sandeep Kumar Chaluvadi, Vincent Polewczyk, Debashis Mondal, Jun Fujii, Piu Rajak, Mahabul Islam, Regina Ciancio, Luisa Barba, Michele Fabrizio, Giorgio Rossi, Pasquale Orgiani, Ivana Vobornik 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.
Marco Caputo, Jasmin Jandke, Edoardo Cappelli, Sandeep Kumar Chaluvadi, Eduardo Bonini Guedes, Muntaser Naamneh, Giovanni Vinai, Jun Fujii, Piero Torelli, Ivana Vobornik, Andrea Goldoni, Pasquale Orgiani, Felix Baumberger, Milan Radovic, Giancarlo Panaccione $V_2O_3$ has long been studied as a prototypical strongly correlated material. The difficulty in ob- taining 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.
Sandeep Kumar Chaluvadi, Fernando Ajejas, Pasquale Orgiani, Olivier Rousseau, Giovanni Vinai, Aleksandr Yu Petrov, Piero Torelli, Alain Pautrat, Julio Camarero, Paolo Perna, Laurence Mechin 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.