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Thirumalai Venkatesan

Publications and source records attributed to Thirumalai Venkatesan.

17 recordsLinked to original sources

Pulsed Laser Template Engineering- PLATEN

Thin films of functional inorganic materials, particularly oxides, play a vital role in optoelectronics, enabling applications that range from active optical components to MEMS-based architectures. Achieving high aspect ratio patterning of these functional materials remains a significant challenge, as many of their constituent elements do not readily form volatile compounds required for conventional reactive ion etch processes. We introduce a novel approach, Pulsed Laser Template ENgineering (PLATEN), which offers a more accessible route for patterning materials that are typically difficult to etch. This technique involves depositing functional films using the Pulsed Laser Deposition (PLD) process onto silicon substrates that have been pre-patterned using reactive ion etching to create high aspect ratio features. Due to the highly forward-directed nature of the PLD process, the deposited films replicate closely the topography of the patterned silicon, without coatings the sidewalls. This process remains effective even at feature sizes down to approximately 50 nm. The oxide films replicate the underlying silicon pattern to a thickness of 80 nm. For thickness beyond 80 nm the patterns develop a waist at the midpoint which scales with film thickness and is not dependent on the feature size. In this paper, we present a detailed analysis of the PLATEN process, including deviations from ideal pattern replication in sub-micron features as a function of film thickness, and demonstrate near single crystalline growth of oxides on the patterned silicon substrate, demonstrating the potential of PLATEN technique for active opto-electronic materials.

cond-mat.mtrl-sci↗

Small polarons mediated near-room-temperature metal-insulator transition in vanadium dioxide and their hopping dynamics

Researchers pursuing advanced photoelectric devices have discovered near room-temperature metal-insulator transitions (MIT) in non-volatile VO2. Despite theoretical investigations suggesting that polaron dynamics mediate the MIT, direct experimental evidence remains scarce. In this study, we present direct evidence of the polaron state in insulating VO2 through high-resolution spectroscopic ellipsometry measurements and first-principles calculations. We illustrate the complementary role of polaron dynamics in facilitating Peierls and Mott transitions, thereby contributing to the MIT processes. Furthermore, our observations and characterizations of conventional metallic and correlated plasmons in the respective phases of the VO2 film offer valuable insights into their electron structures. This investigation enhances comprehension of the MIT mechanism in correlated systems and underscores the roles of polarons, lattice distortions, and electron correlations in facilitating phase transition processes in strongly-correlated systems. Additionally, the detailed detection of small polarons and plasmons serves as inspiration for the development of new device functionalities.

physics.app-ph↗

Direct observation of two-dimensional small polarons at correlated oxide interface

Two-dimensional (2D) perovskite oxide interfaces are ideal systems where diverse emergent properties can be uncovered.The formation and modification of polaronic properties due to short-range strong charge-lattice interactions of 2D interfaces remains hugely intriguing.Here, we report the direct observation of small-polarons at the LaAlO3/SrTiO3 (LAO/STO) conducting interface using high-resolution spectroscopic ellipsometry.First-principles investigations further reveals that strong coupling between the interfacial electrons and the Ti-lattice result in the formation of localized 2D small polarons.These findings resolve the longstanding issue where the excess experimentally measured interfacial carrier density is significantly lower than theoretically predicted values.The charge-phonon induced lattice distortion further provides an analogue to the superconductive states in magic-angle twisted bilayer graphene attributed to the many-body correlations induced by broken periodic lattice symmetry.Our study sheds light on the multifaceted complexity of broken periodic lattice induced quasi-particle effects and its relationship with superconductivity.

cond-mat.str-el↗

Coexistence of surface oxygen vacancy and interface conducting states in LaAlO3/SrTiO3 revealed by low-angle resonant soft X-ray scattering

Oxide heterostructures have shown rich physics phenomena, particularly in the conjunction of exotic insulator-metal transition (IMT) at the interface between polar insulator LaAlO3 and non-polar insulator SrTiO3 (LaAlO3/SrTiO3). Polarization catastrophe model has suggested an electronic reconstruction yielding to metallicity at both the interface and surface. Another scenario is the occurrence of surface oxygen vacancy at LaAlO3 (surface-Ov), which has predicted surface-to-interface charge transfer yielding metallic interface but insulating surface. To clarify the origin of IMT, one should probe surface-Ov and the associated electronic structures at both the surface and the buried interface simultaneously. Here, using low-angle resonant soft X-ray scattering (LA-RSXS) supported with first-principles calculations, we reveal the co-existence of the surface-Ov state and the interface conducting state only in conducting LaAlO3/SrTiO3 (001) films. Interestingly, both the surface-Ov state and the interface conducting state are absent for the insulating film. As a function of Ov density, while the surface-Ov state is responsible for the IMT, the spatial charge distribution is found responsible for a transition from two-dimensional-like to three-dimensional-like conducting accompanied by spectral weight transfer, revealing the importance of electronic correlation. Our results show the importance of surface-Ov in determining interface properties and provides a new strategy in utilizing LA-RSXS to directly probe the surface and buried interface electronic properties in complex oxide heterostructures.

cond-mat.mtrl-sci↗

Experimental Evidence of t2g Electron-Gas Rashba Interaction Induced by Asymmetric Orbital Hybridization

We report the control of Rashba spin-orbit interaction by tuning asymmetric hybridization between Ti-orbitals at the LaAlO3/SrTiO3 interface. This asymmetric orbital hybridization is modulated by introducing a LaFeO3 layer between LaAlO3 and SrTiO3, which alters the Ti-O lattice polarization and traps interfacial charge carriers, resulting in a large Rashba spin-orbit effect at the interface in the absence of an external bias. This observation is verified through high-resolution electron microscopy, magneto-transport and first-principles calculations. Our results open hitherto unexplored avenues of controlling Rashba interaction to design next-generation spin-orbitronics.

cond-mat.mtrl-sci↗

Charge Carrier Transport in Iron Pyrite Thin Films: Disorder Induced Variable Range Hopping

The origin of p-type conductivity and the mechanism responsible for low carrier mobility was investigated in pyrite (FeS2) thin films. Temperature dependent resistivity measurements were performed on polycrystalline and nanostructured thin films prepared by three different methods. Films have a high hole density and low mobility regardless of the method used for their preparation. The charge transport mechanism is determined to be nearest neighbour hopping (NNH) at near room temperature with Mott-type variable range hopping (VRH) of holes via localized states occurring at lower temperatures. Density functional theory (DFT) predicts that sulfur vacancy induced localized defect states will be situated within the band gap with the charge remaining localized around the defect. The data indicate that the electronic properties including hopping transport in pyrite thin films can be correlated to sulfur vacancy related defect. The results provide insights on electronic properties of pyrite thin films and its implications for charge transport

cond-mat.mtrl-sci↗

Large Microwave Inductance of Granular Boron-Doped Diamond Superconducting Films

Boron-doped diamond granular thin films are known to exhibit superconductivity with an optimal critical temperature of Tc = 7.2K. Here we report the measured complex surface impedance of Boron-doped diamond films in the microwave frequency range using a resonant technique. Experimentally measured inductance values are in good agreement with estimates obtained from the normal state sheet resistance of the material. The magnetic penetration depth temperature dependence is consistent with that of a fully-gapped s-wave superconductor. Boron-doped diamond films should find application where high kinetic inductance is needed, such as microwave kinetic inductance detectors and quantum impedance devices.

cond-mat.supr-con↗

Topological Hall Effect and Skyrmion-like Bubbles at a Charge-transfer Interface

Exploring exotic interface magnetism due to charge transfer and strong spin-orbit coupling has profound application in future development of spintronic memory. Here, the emergence, tuning and interpretation of hump-shape Hall Effect from a CaMnO3/CaIrO3/CaMnO3 trilayer structure are studied in detail. The hump signal can be recognized as Topological Hall Effect suggesting the presence of Skyrmion-like magnetic bubbles; but the debated alternative interpretation where the signal being an artefact between two cancelling Anomalous Hall Effect loops is also discussed. Firstly, by tilting the magnetic field direction, the evolution of Hall signal suggests transformation of the bubbles topology into a more trivial kind. Secondly, by varying the thickness of CaMnO3, the optimal thicknesses for the hump signal emergence are found, suggesting a tuning of charge transfer fraction. Using high-resolution transmission electron microscopy, a stacking fault is also identified, which distinguishes the top and bottom CaMnO3/CaIrO3 interfaces in terms of charge transfer fraction and possible interfacial Dzyaloshinskii-Moriya Interaction. Finally, a spin-transfer torque experiment revealed a low threshold current density of ~10^9 A/m^2 for initiating the motion of bubbles. This discovery opens a possible route for integrating Skyrmions with antiferromagnetic spintronics.

cond-mat.mes-hall↗

Tunable and Enhanced Rashba Spin-Orbit Coupling in Iridate-Manganite Heterostructures

Tailoring spin-orbit interactions and Coulomb repulsion are the key features to observe exotic physical phenomena such as magnetic anisotropy and topological spin texture at oxide interfaces. Our study proposes a novel platform for engineering the magnetism and spin-orbit coupling at LaMnO3/SrIrO3 (3d-5d oxide) interfaces by tuning the LaMnO3 growth conditions which controls the lattice displacement and spin-correlated interfacial coupling through charge transfer. We report on a tunable and enhanced interface-induced Rashba spin-orbit coupling and Elliot-Yafet spin relaxation mechanism in LaMnO3/SrIrO3 bilayer with change in the underlying magnetic order of LaMnO3. We also observed enhanced spin-orbit coupling strength in LaMnO3/SrIrO3 compared to previously reported SrIrO3 layers. The X-Ray spectroscopy measurement reveals the quantitative valence of Mn and their impact on charge transfer. Further, we performed angle-dependent magnetoresistance measurements, which show signatures of magnetic proximity effect in SrIrO3 while reflecting the magnetic order of LaMnO3. Our work thus demonstrates a new route to engineer the interface induced Rashba spin-orbit coupling and magnetic proximity effect in 3d-5d oxide interfaces which makes SrIrO3 an ideal candidate for spintronics applications.

cond-mat.str-el↗

Characteristic Lengths of Interlayer Charge-Transfer in Correlated Oxide Heterostructures

Using interlayer interaction to control functional heterostructures with atomic-scale designs has become one of the most effective interface-engineering strategies nowadays. Here, we demonstrate the effect of a crystalline LaFeO3 buffer layer on amorphous and crystalline LaAlO3/SrTiO3 heterostructures. The LaFeO3 buffer layer acts as an energetically favored electron acceptor in both LaAlO3/SrTiO3 systems, resulting in modulation of interfacial carrier density and hence metal-to-insulator transition. For amorphous and crystalline LaAlO3/SrTiO3 heterostructures, the metal-to-insulator transition is found when the LaFeO3 layer thickness crosses 3 and 6 unit cells, respectively. Such different critical LaFeO3 thicknesses are explained in terms of distinct characteristic lengths of the redox-reaction-mediated and polar-catastrophe-dominated charge transfer, controlled by the interfacial atomic contact and Thomas-Fermi screening effect, respectively. Our results not only shed light on the complex interlayer charge transfer across oxide heterostructures but also provides a new route to precisely tailor the charge-transfer process at a functional interface.

cond-mat.mtrl-sci↗

Phase change-photonic framework for terahertz wave control

The advancement in capabilities enabled by handheld devices and the prospective internet of things has led to an explosion of wireless data consumption in the last decade. The ever-increasing demand for high speed data transfer has projected the unprecedented importance of terahertz spectral range for next generation wireless communication systems. However, versatile interaction and active manipulation of terahertz waves required for a wide-range of terahertz technologies are either unavailable or unscalable. Here, we report on an integrated platform of chalcogenide phase change material, germanium antimony telluride (GST), with metamaterials for multidimensional manipulation of terahertz waves. The thermal, electrical and optical stimulation of GST provide multilevel non-volatility, sub-wavelength spatial selectivity and variable ultrafast switching of terahertz waves, respectively. These multifaceted response of phase change material can be used in tandem with metamaterial that enables strong field confinement along with on-demand spectral response and frequency selectivity. The unique and multifarious properties of GST combined with the versatility and scalability of metamaterial design and ease of fabrication could aid in the development of advanced devices operating in terahertz range, such as spatio-temporal light modulators, neuromorphic photonic devices, compressive imagers, and switchable holograms, vital for the next generation wireless communication systems.

physics.app-ph↗

The Mechanism of Electrolyte Gating on High-Tc Cuprates: The Role of Oxygen Migration and Electrostatics

Electrolyte gating is widely used to induce large carrier density modulation on solid surfaces to explore various properties. Most of past works have attributed the charge modulation to electrostatic field effect. However, some recent reports have argued that the electrolyte gating effect in VO2, TiO2 and SrTiO3 originated from field-induced oxygen vacancy formation. This gives rise to a controversy about the gating mechanism, and it is therefore vital to reveal the relationship between the role of electrolyte gating and the intrinsic properties of materials. Here, we report entirely different mechanisms of electrolyte gating on two high-Tc cuprates, NdBa2Cu3O7-δ (NBCO) and Pr2-xCexCuO4 (PCCO), with different crystal structures. We show that field-induced oxygen vacancy formation in CuO chains of NBCO plays the dominant role while it is mainly an electrostatic field effect in the case of PCCO. The possible reason is that NBCO has mobile oxygen in CuO chains while PCCO does not. Our study helps clarify the controversy relating to the mechanism of electrolyte gating, leading to a better understanding of the role of oxygen electro migration which is very material specific.

cond-mat.str-el↗

Interfacial Rashba magnetoresistance of two-dimensional electron gas at LaAlO$_3$/SrTiO$_3$ interface

We report the angular dependence of magnetoresistance in two-dimensional electron gas at LaAlO$_3$/SrTiO$_3$ interface. We find that this interfacial magnetoresistance exhibits a similar angular dependence to the spin Hall magnetoresistance observed in ferromagnet/heavy metal bilayers, which has been so far discussed in the framework of bulk spin Hall effect of heavy metal layer. The observed magnetoresistance is in qualitative agreement with theoretical model calculation including both Rashba spin-orbit coupling and exchange interaction. Our result suggests that magnetic interfaces subject to spin-orbit coupling can generate a nonnegligible contribution to the spin Hall magnetoresistance and the interfacial spin-orbit coupling effect is therefore key to the understanding of various spin-orbit-coupling-related phenomena in magnetic/non-magnetic bilayers.

cond-mat.mtrl-sci↗

High field magneto-transport in two-dimensional electron gas LaAlO3/SrTiO3

Transport properties of the complex oxide LaAlO3/SrTiO3 interface are investigated under high magnetic field (55T). By rotating the sample with respect to the magnetic field, the two-dimensional nature of charge transport is clearly established. Small oscillations of the agnetoresistance with altered periodicity are observed when plotted versus inverse magnetic field. We attribute this effect to Rashba spin-orbit coupling which remains consistent with large negative magnetoresistance when the field is parallel to the sample plane. A large inconsistency between the carrier density extracted from Shubnikov-de Haas analysis and from the Hall effect is explained by the contribution to transport of at least two bands with different mobility.

cond-mat.str-el↗

Extremely large magnetoresistance in few-layer graphene/boron-nitride heterostructures

Understanding magnetoresistance, the change in electrical resistance upon an external magnetic field, at the atomic level is of great interest both fundamentally and technologically. Graphene and other two-dimensional layered materials provide an unprecedented opportunity to explore magnetoresistance at its nascent stage of structural formation. Here, we report an extremely large local magnetoresistance of ~ 2,000% at 400 K and a non-local magnetoresistance of > 90,000% in 9 T at 300 K in few-layer graphene/boron-nitride heterostructures. The local magnetoresistance is understood to arise from large differential transport parameters, such as the carrier mobility, across various layers of few-layer graphene upon a normal magnetic field, whereas the non-local magnetoresistance is due to the magnetic field induced Ettingshausen-Nernst effect. Non-local magnetoresistance suggests the possibility of a graphene based gate tunable thermal switch. In addition, our results demonstrate that graphene heterostructures may be promising for magnetic field sensing applications.

cond-mat.mtrl-sci↗

Emergent nanoscale superparamagnetism at oxide interfaces

Atomically sharp oxide heterostructures exhibit a range of novel physical phenomena that do not occur in the parent bulk compounds. The most prominent example is the appearance of highly conducting and superconducting states at the interface between the band insulators LaAlO3 and SrTiO3. Here we report a new emergent phenomenon at the LaMnO3/SrTiO3 interface in which an antiferromagnetic insulator abruptly transforms into a magnetic state that exhibits unexpected nanoscale superparamagnetic dynamics. Upon increasing the thickness of LaMnO3 above five unit cells, our scanning nanoSQUID-on-tip microscopy shows spontaneous formation of isolated magnetic islands of 10 to 50 nm diameter, which display random moment reversals by thermal activation or in response to an in-plane magnetic field. Our charge reconstruction model of the polar LaMnO3/SrTiO3 heterostructure describes the sharp emergence of thermodynamic phase separation leading to nucleation of metallic ferromagnetic islands in an insulating antiferromagnetic matrix. The model further suggests that the nearby superparamagnetic-ferromagnetic transition can be gate tuned, holding potential for applications in magnetic storage and spintronics.

cond-mat.str-el↗

Current-driven spin orbit field in LaAlO3/SrTiO3 heterostructures

We demonstrate a current tunable Rashba spin orbit interaction in LaAlO3/SrTiO3 (LAO/STO) quasi two dimensional electron gas (2DEG) system. Anisotropic magnetoresistance (AMR) measurements are employed to detect and understand the current-induced Rashba field. The effective Rashba field scales with the current and a value of 2.35 T is observed for a dc-current of 200 uA. The results suggest that LAO/STO heterostructures can be considered for spin orbit torque based magnetization switching.

cond-mat.mtrl-sci↗