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Sandeep Kumar Chaluvadi

Publications and source records attributed to Sandeep Kumar Chaluvadi.

11 recordsLinked to original sources

Tracking the local order parameter through the Hubbard exciton decoherence time in the Mott-Hubbard insulator LaVO3

The prototypical Mott-Hubbard insulator LaVO3 undergoes a structural phase transition accompanied by the onset of spin and orbital ordering below 140 K. By combining ultrafast optical pump-probe spectroscopy and two-dimensional electronic spectroscopy, we investigate the interplay between fluctuations of the local spin and orbital order parameter and the lifetime of high-energy electron-hole excitations. Specifically, we demonstrate that the pump-induced perturbation of the order parameter leads to a change of the Hubbard exciton decoherence time and, consequently, of its homogeneous linewidth. Dynamical mean-field theory calculations confirm that the exciton scattering rate is crucially affected by the degree of order of the spin and orbital lattices in LaVO3. Our results demonstrate that multi-dimensional ultrafast optical spectroscopy can be used to track the dynamics of the order parameter, thus opening new routes in the study of correlated quantum materials characterized by intertwined orders.

cond-mat.str-el

Interfacial properties of MoS2 thin films grown on functional substrates

Interface chemistry and defect formation in MoS2 thin films grown on single crystal substrates critically determine the electronic structure of MoS2 and thus can strongly modify material functionality relevant for many applications, including electronics, optoelectronics, and energy related catalysis. We investigate MoS2 grown on three technologically relevant substrates, namely SrTiO3(111), c-axis Al2O3(0001) and 6H-SiC(0001). Experimental investigations by temperature dependent resistivity, photoemission spectroscopy and scanning transmission electron microscopy with coupled energy dispersive spectroscopy, with the support of theoretical calculation by Density Functional Theory, allow the identification of the substrate induced specific defects and their correlation with the electronic properties. Ti interdiffusion in SrTiO3/MoS2 generates donor like states near the Fermi level, leading to metallic transport. Al2O3/MoS2 exhibits a high density of sulfur related defects that introduce localized states and yield nearly temperature independent conductivity. SiC/MoS2 exhibits significant interface disorder resulting in a semiconducting temperature dependent resistivity, yet deviating from the ideal bulk like behavior. These results demonstrate how substrate choice governs defect formation and ultimately dominates the electronic behavior of MoS2 thin films, making the control of film substrate interactions essential for the engineering of new functional devices.

cond-mat.mtrl-sci

Substrate induced optimization of the Electrocatalytic Hydrogen Evolution Reaction (HER) performances of MoS2 thin film

Molybdenum disulfide (MoS2) has emerged as a promising, cost-effective catalyst for hydrogen production via water splitting. We investigate the structural and electrocatalytic properties of MoS2 thin films deposited on different substrates (Al2O3, SiC, STO) to study their hydrogen evolution reaction (HER) activity. In particular, in order to study the substrate influence on the stabilization of different polymorphic MoS2 phases, the films are synthesised using pulsed laser deposition on substrates with different crystal symmetries and lattice parameters. All the deposited samples are characterized by X-Ray Diffraction, Raman Spectroscopy, Linear Sweep Voltammetry and Electrochemical Impedance Spectroscopy analyses. The films grown on Al2O3 substrates exhibit the best HER performance, likely due to the stabilization of the metastable 1T phase through the interfacial interactions between film and substrate. Presence of the 1T phase in the samples grown on Al2O3 improves the charge transfer efficiency and the electrochemically active surface with a better response to the applied potential, demonstrating their enhanced catalytic behaviour for hydrogen evolution.

cond-mat.mtrl-sci

Bilayer orthogonal ferromagnetism in CrTe$_2$-based van der Waals system

Systems with pronounced spin anisotropy play a pivotal role in advancing magnetization switching and spin-wave generation mechanisms, which are fundamental for spintronic technologies. Quasi-van der Waals ferromagnets, particularly Cr$_{1+δ}$Te$_2$ compounds, represent seminal materials in this field, renowned for their delicate balance between frustrated layered geometries and magnetism. Despite extensive investigation, the precise nature of their magnetic ground state, typically described as a canted ferromagnet, remains contested, as does the mechanism governing spin reorientation under external magnetic fields and varying temperatures. In this work, we leverage a multimodal approach, integrating complementary techniques, to reveal that Cr$_{1+δ}$Te$_2$ ($δ= 0.25 - 0.50$) hosts a previously overlooked magnetic phase, which we term orthogonal-ferromagnetism. This single phase consists of alternating atomically sharp single layers of in-plane and out-of-plane ferromagnetic blocks, coupled via exchange interactions and as such, it differs significantly from crossed magnetism, which can be achieved exclusively by stacking multiple heterostructural elements together. Contrary to earlier reports suggesting a gradual spin reorientation in CrTe$_2$-based systems, we present definitive evidence of abrupt spin-flop-like transitions. This discovery, likely due to the improved crystallinity and lower defect density in our samples, repositions Cr$_{1+δ}$Te$_2$ compounds as promising candidates for spintronic and orbitronic applications, opening new pathways for device engineering.

cond-mat.str-el

Impact of terahertz short pulses on the oxygen defect state in TiO$_{2-x}$

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.

cond-mat.mtrl-sci

Uncovering the lowest thickness limit for room-temperature ferromagnetism of Cr$_{1.6}$Te$_{2}$

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.

cond-mat.mtrl-sci

Signatures of a surface spin-orbital chiral metal

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.

cond-mat.str-el

Visualising emergent phenomena at oxide interfaces

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.

cond-mat.mtrl-sci

Disentangling structural and electronic properties in V$_{2}$O$_{3}$ thin films: a genuine non-symmetry breaking Mott transition

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.

cond-mat.str-el

Metal to insulator transition at the surface of $V_2O_3$ thin films: an in-situ view

$V_2O_3$ 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.

cond-mat.str-el

Room temperature biaxial magnetic anisotropy in La0.67Sr0.33MnO3 thin films on SrTiO3 buffered MgO (001) substrates for spintronic applications

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.

cond-mat.mtrl-sci