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T. Venkatesan

Publications and source records attributed to T. Venkatesan.

At least 19 recordsLinked to original sources

Epitaxial CeO2 Films as a Host for Quantum Applications

In highly purified host, the coherence of quantum emitters is ultimately limited by hyperfine interactions between the emitter and lattice nuclei possessing non-zero nuclear magnetic moments. This limitation can only be mitigated through isotopic purification. In this work, we investigate CeO2 as a host composed entirely of nuclei with zero nuclear moment. High-quality CeO2 thin films were grown by PLD and doped with Tm and Er ions. Structural characterization using X-ray diffraction, atomic force microscopy, and ion channeling confirms single-crystalline, atomically smooth films with dopants substitutionally incorporated at Ce lattice sites. Photoluminescence lifetime measurements show significantly longer lifetimes for Er-doped CeO2 (2.9 - 5.3 ms) compared with Tm-doped films (14 - 68 {\mu}s). Moreover, the Er-doped PLD films exhibit longer lifetimes at ~1% dopant concentration than previously reported for MBE-grown films. Density functional theory calculations reveal a substantial overlap between unoccupied O 2p and Tm 4f states near the valence band maximum, whereas Er 4f states remain well isolated. This electronic interaction likely introduces non-radiative recombination pathways in Tm-doped CeO2, explaining the reduced lifetimes. These findings highlight the importance of selecting appropriate dopant-host combinations and optimized growth conditions to minimize non-radiative channels for quantum applications.

quant-ph

Competition of electronic correlation and reconstruction in La1-xSrxTiO3/SrTiO3 heterostructures

Electronic correlation and reconstruction are two important factors that play a critical role in shaping the magnetic and electronic properties of correlated low-dimensional systems. Here, we report a competition between the electronic correlation and structural reconstruction in La1-xSrxTiO3/SrTiO3 heterostructures by modulating material polarity and interfacial strain, respectively. The heterostructures exhibit a critical thickness (tc) at which a metal-to-insulator transition (MIT) abruptly occurs at certain thickness, accompanied by the coexistence of two- and three-dimensional (2D and 3D) carriers. Intriguingly, the tc exhibits a V-shaped dependence on the doping concentration of Sr, with the smallest tc value at x = 0.5. We attribute this V-shaped dependence to the competition between the electronic reconstruction (modulated by the polarity) and the electronic correlation (modulated by strain), which are borne out by the experimental results, including strain-dependent electronic properties and the evolution of 2D and 3D carriers. Our findings underscore the significance of the interplay between electronic reconstruction and correlation in the realization and utilization of emergent electronic functionalities in low-dimensional correlated systems.

cond-mat.str-el

Large polaron evolution in anatase TiO2 due to carrier and temperature dependence of electron-phonon coupling

The electronic and magneto transport properties of reduced anatase TiO2 epitaxial thin films are analyzed considering various polaronic effects. Unexpectedly, with increasing carrier concentration, the mobility increases, which rarely happens in common metallic systems. We find that the screening of the electron-phonon (e-ph) coupling by excess carriers is necessary to explain this unusual dependence. We also find that the magnetoresistance (MR) could be decomposed into a linear and a quadratic component, separately characterizing the transport and trap behavior of carriers as a function of temperature. The various transport behaviors could be organized into a single phase diagram which clarifies the nature of large polaron in this material.

cond-mat.mes-hall

Skyrmionics in correlated oxides

While chiral magnets, metal-based magnetic multilayers, or Heusler compounds have been considered as the material workhorses in the field of skyrmionics, oxides are now emerging as promising alternatives, as they host special correlations between the spin-orbital-charge-lattice degrees of freedom and/or coupled ferroic order parameters. These interactions open new possibilities for practically exploiting skyrmionics. In this article, we review the recent advances in the observation and control of topological spin textures in various oxide systems. We start with the discovery of skyrmions and related quasiparticles in bulk and heterostructure ferromagnetic oxides. Next, we emphasize the shortcomings of implementing ferromagnetic textures, which have led to the recent explorations of ferrimagnetic and antiferromagnetic oxide counterparts, with higher Curie temperatures, stray-field immunity, low Gilbert damping, ultrafast magnetic dynamics, and/or absence of skyrmion deflection. Then, we highlight the development of novel pathways to control the stability, motion, and detection of topological textures using electric fields and currents. Finally, we present the outstanding challenges that need to be overcome to achieve all-electrical, nonvolatile, low-power oxide skyrmionic devices.

cond-mat.mtrl-sci

Effect of phonon anharmonicity on ferroelectricity in EuxBa1-xTiO3

Investigating the competition between ferroelectric ordering and quantum fluctuations is essential to tailor the desired functionalities of mixed ferroelectric and incipient ferroelectric systems, like, (Ba,Sr)TiO3 and (Eu,Ba)TiO3. Recently, it has been shown that suppression of quantum fluctuations increases ferroelectric ordering in (Eu,Ba)TiO3 and since these phenomena are coupled to crystallographic phase transitions it is essential to understand the role of phonons. Here, we observe that the unusual temperature dependence of phonons in BaTiO3 gets suppressed when Ba2+ is replaced by Eu2+. This manifests in a decrease in the cubic-to-tetragonal (i.e., para-to-ferroelectric) phase transition temperature (by 150 K) and a complete suppression of tetragonality of the lattice (at room temperature by 40% replacement of Ba2+ by Eu2+). We have quantified the anharmonicity of the phonons and observed that the replacement of Ba2+ by Eu2+ suppresses it (by 93%) with a resultant lowering of the ferroelectric ordering temperature in the EuxBa1-xTiO3. This suggests that tuning phonon anharmonicity can be an important route to novel ferroelectric materials.

cond-mat.mtrl-sci

Antiferromagnetic Half-skyrmions and Bimerons at room temperature

In the quest for post-CMOS technologies, ferromagnetic skyrmions and their anti-particles have shown great promise as topologically protected solitonic information carriers in memory-in-logic or neuromorphic devices. However, the presence of dipolar fields in ferromagnets, restricting the formation of ultra-small topological textures, and the deleterious skyrmion Hall effect when driven by spin torques have thus far inhibited their practical implementations. Antiferromagnetic analogues, which are predicted to demonstrate relativistic dynamics, fast deflection-free motion and size scaling have recently come into intense focus, but their experimental realizations in natural antiferromagnetic systems are yet to emerge. Here, we demonstrate a family of topological antiferromagnetic spin-textures in $α$-Fe$_2$O$_3$ - an earth-abundant oxide insulator - capped with a Pt over-layer. By exploiting a first-order analogue of the Kibble-Zurek mechanism, we stabilize exotic merons-antimerons (half-skyrmions), and bimerons, which can be erased by magnetic fields and re-generated by temperature cycling. These structures have characteristic sizes of the order ~100 nm that can be chemically controlled via precise tuning of the exchange and anisotropy, with pathways to further scaling. Driven by current-based spin torques from the heavy-metal over-layer, some of these AFM textures could emerge as prime candidates for low-energy antiferromagnetic spintronics at room temperature.

cond-mat.mtrl-sci

Evidence of Rotational Fröhlich Coupling in Polaronic Trions

Electrons commonly couple through Fröhlich interactions with longitudinal optical phonons to form polarons. However, trions possess a finite angular momentum and should therefore couple instead to rotational optical phonons. This creates a polaronic trion whose binding energy is determined by the crystallographic orientation of the lattice. Here, we demonstrate theoretically within the Fröhlich approach and experimentally by photoluminescence emission that the bare trion binding energy (20 meV) is significantly enhanced by the phonons at the interface between the two-dimensional semiconductor MoS$_2$ and the bulk transition metal oxide SrTiO$_3$. The low-temperature {binding energy} changes from 60 meV in [001]-oriented substrates to 90 meV for [111] orientation, as a result of the counter-intuitive interplay between the rotational axis of the MoS$_2$ trion and that of the SrTiO$_3$ phonon mode.

cond-mat.mes-hall

Artificial two-dimensional polar metal by charge transfer to a ferroelectric insulator

Integrating multiple properties in a single system is crucial for the continuous developments in electronic devices. However, some physical properties are mutually exclusive in nature. Here, we report the coexistence of two seemingly mutually exclusive properties-polarity and two-dimensional conductivity-in ferroelectric Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ thin films at the LaAlO$_3$/Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ interface at room temperature. The polarity of a ~3.2 nm Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ thin film is preserved with a two-dimensional mobile carrier density of ~0.05 electron per unit cell. We show that the electronic reconstruction resulting from the competition between the built-in electric field of LaAlO$_3$ and the polarization of Ba$_{0.2}$Sr$_{0.8}$TiO$_3$ is responsible for this unusual two-dimensional conducting polar phase. The general concept of exploiting mutually exclusive properties at oxide interfaces via electronic reconstruction may be applicable to other strongly-correlated oxide interfaces, thus opening windows to new functional nanoscale materials for applications in novel nanoelectronics.

cond-mat.mtrl-sci

Oxygen Electromigration and Energy Band Reconstruction Induced by Electrolyte Field Effect at Oxide Interfaces

Electrolyte gating is a powerful means for tuning the carrier density and exploring the resultant modulation of novel properties on solid surfaces. However, the mechanism, especially its effect on the oxygen migration and electrostatic charging at the oxide heterostructures, is still unclear. Here we explore the electrolyte gating on oxygen-deficient interfaces between SrTiO3 (STO) crystals and LaAlO3 (LAO) overlayer through the measurements of electrical transport, X-ray absorption spectroscopy (XAS) and photoluminescence (PL) spectra. We found that oxygen vacancies (Ovac) were filled selectively and irreversibly after gating due to oxygen electromigration at the amorphous LAO/STO interface, resulting in a reconstruction of its interfacial band structure. Because of the filling of Ovac, the amorphous interface also showed an enhanced electron mobility and quantum oscillation of the conductance. Further, the filling effect could be controlled by the degree of the crystallinity of the LAO overlayer by varying the growth temperatures. Our results reveal the different effects induced by electrolyte gating, providing further clues to understand the mechanism of electrolyte gating on buried interfaces and also opening a new avenue for constructing high-mobility oxide interfaces.

cond-mat.str-el

Strong spin-orbit coupling and magnetism in (111) (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35})$/SrTiO$_3$

Strong correlations, multiple lattice degrees of freedom, and the ease of doping make complex oxides a source of great research interest. Complex oxide heterointerfaces break inversion symmetry and can host a two dimensional carrier gas, which can display a variety of coexisting and competing phenomena. In the case of heterointerfaces based on SrTiO$_3$, many of these phenomena can be effectively tuned by using an electric gate, due to the large dielectric constant of SrTiO$_3$. Most studies so far have focused on (001) oriented heterostructures; however, (111) oriented heterostructures have recently gained attention due to the possibility of finding exotic physics in these systems due their hexagonal surface crystal symmetry. In this work, we use magnetoresistance to study the evolution of spin-orbit interaction and magnetism in a new system, (111) oriented (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)/SrTiO$_3$. At more positive values of the gate voltage, which correspond to high carrier densities, we find that transport is multiband, and dominated by high mobility carriers with a tendency towards weak localization. At more negative gate voltages, the carrier density is reduced, the high mobility bands are depopulated, and weak antilocalization effects begin to dominate, indicating that spin-orbit interaction becomes stronger. At millikelvin temperatures, and gate voltages corresponding to the strong spin-orbit regime, we observe hysteresis in magnetoresistance, indicative of ferromagnetism in the system. Our results suggest that in the (111) (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)/SrTiO$_3$ system, low mobility carriers which experience strong spin-orbit interactions participate in creating magnetic order in the system.

cond-mat.str-el

Low temperature magnetoresistance of (111) (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)/SrTiO$_3$

The two dimensional conducting interfaces in SrTiO$_3$-based systems are known to show a variety of coexisting and competing phenomena in a complex phase space. Magnetoresistance measurements, which are typically used to extract information about the various interactions in these systems, must be interpreted with care, since multiple interactions can contribute to the resistivity in a given range of magnetic field and temperature. Here we review all the phenomena that can contribute to transport in SrTiO$_3$-based conducting interfaces at low temperatures, and discuss possible ways to distinguish between various phenomena. We apply this analysis to the magnetoresistance data of (111) oriented (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)/STO (LSAT/STO) heterostructures in perpendicular field, and find an excess negative magnetoresistance contribution which cannot be explained by weak localization alone. We argue that contributions from magnetic scattering as well as electron-electron interactions can provide a possible explanation for the observed magnetoresistance.

cond-mat.mes-hall

Room Temperature Giant Charge-to-Spin Conversion at SrTiO3/LaAlO3 Oxide Interface

Two-dimensional electron gas (2DEG) formed at the interface between SrTiO3 (STO) and LaAlO3 (LAO) insulating layer is supposed to possess strong Rashba spin-orbit coupling. To date, the inverse Edelstein effect (i.e. spin-to-charge conversion) in the 2DEG layer is reported. However, the direct effect of charge-to-spin conversion, an essential ingredient for spintronic devices in a current induced spin-orbit torque scheme, has not been demonstrated yet. Here we show, for the first time, a highly efficient spin generation with the efficiency of ~6.3 in the STO/LAO/CoFeB structure at room temperature by using spin torque ferromagnetic resonance. In addition, we suggest that the spin transmission through the LAO layer at high temperature range is attributed to the inelastic tunneling via localized states in the LAO band gap. Our findings may lead to potential applications in the oxide insulator based spintronic devices.

cond-mat.mtrl-sci

Control of magnetic anisotropy by orbital hybridization in (La0.67Sr0.33MnO3)n/(SrTiO3)n superlattice

The asymmetry of chemical nature at the hetero-structural interface offers an unique opportunity to design desirable electronic structure by controlling charge transfer and orbital hybridization across the interface. However, the control of hetero-interface remains a daunting task. Here, we report the modulation of interfacial coupling of (La0.67Sr0.33MnO3)n/(SrTiO3)n superlattices by manipulating the periodic thickness with n unit cells of SrTiO3 and n unit cells La0.67Sr0.33MnO3. The easy axis of magnetic anisotropy rotates from in-plane (n = 10) to out-of-plane (n = 2) orientation at 150 K. Transmission electron microscopy reveals enlarged tetragonal ratio > 1 with breaking of volume conservation around the (La0.67Sr0.33MnO3)n/(SrTiO3)n interface, and electronic charge transfer from Mn to Ti 3d orbitals across the interface. Orbital hybridization accompanying the charge transfer results in preferred occupancy of 3d3z2-r2 orbital at the interface, which induces a stronger electronic hopping integral along the out-of-plane direction and corresponding out-of-plane magnetic easy axis for n = 2. We demonstrate that interfacial orbital hybridization in superlattices of strongly correlated oxides may be a promising approach to tailor electronic and magnetic properties in device applications.

cond-mat.mtrl-sci

Electron Accumulation and Emergent Magnetism in LaMnO3/SrTiO3 Heterostructures

Emergent phenomena at polar-nonpolar oxide interfaces have been studied intensely in pursuit of next-generation oxide electronics and spintronics. Here we report the disentanglement of critical thicknesses for electron reconstruction and the emergence of ferromagnetism in polar-mismatched LaMnO3/SrTiO3 (001) heterostructures. Using a combination of element-specific X-ray absorption spectroscopy and dichroism, and first-principles calculations, interfacial electron accumulation and ferromagnetism have been observed within the polar, antiferromagnetic insulator LaMnO3. Our results show that the critical thickness for the onset of electron accumulation is as thin as 2 unit cells (UC), significantly thinner than the observed critical thickness for ferromagnetism of 5 UC. The absence of ferromagnetism below 5 UC is likely induced by electron over-accumulation. In turn, by controlling the doping of the LaMnO3, we are able to neutralize the excessive electrons from the polar mismatch in ultrathin LaMnO3 films and thus enable ferromagnetism in films as thin as 3 UC, extending the limits of our ability to synthesize and tailor emergent phenomena at interfaces and demonstrating manipulation of the electronic and magnetic structures of materials at the shortest length scales.

cond-mat.mtrl-sci

Signatures of Electronic Nematicity in (111) LaAlO$_3$/SrTiO$_3$ Interfaces

Symmetry breaking is a fundamental concept in condensed matter physics whose presence often heralds new phases of matter. For instance, the breaking of time reversal symmetry is traditionally linked to magnetic phases in a material, while the breaking of gauge symmetry can lead to superfluidity/superconductivity. Nematic phases are phases in which rotational symmetry is broken while maintaining translational symme- try, and are traditionally associated with liquid crystals. Electronic nematic states where the or- thogonal in-plane crystal directions have different electronic properties have garnered a great deal of attention after their discovery in Sr$_3$Ru$_2$O$_7$, multiple iron based superconductors, and in the superconducting state of CuBiSe. Here we demonstrate the existence of an electronic ne- matic phase in the two-dimensional carrier gas that forms at the (111) LaAlO$_3$ (LAO)/SrTiO$_3$ (STO) interface that onsets at low temperatures, and is tunable by an electric field.

cond-mat.str-el

Experimental study of extrinsic spin Hall effect in CuPt alloy

We have experimentally studied the effects on the spin Hall angle due to systematic addition of Pt into the light metal Cu. We perform spin torque ferromagnetic resonance measurements on Py/CuPt bilayer and find that as the Pt concentration increases, the spin Hall angle of CuPt alloy increases. Moreover, only 28% Pt in CuPt alloy can give rise to a spin Hall angle close to that of Pt. We further extract the spin Hall resistivity of CuPt alloy for different Pt concentrations and find that the contribution of skew scattering is larger for lower Pt concentrations, while the side-jump contribution is larger for higher Pt concentrations. From technological perspective, since the CuPt alloy can sustain high processing temperatures and Cu is the most common metallization element in the Si platform, it would be easier to integrate the CuPt alloy based spintronic devices into existing Si fabrication technology.

cond-mat.mtrl-sci

Magnetoresistance in the superconducting state at the (111) LaAlO$_3$/SrTiO$_3$ interface

Condensed matter systems that simultaneously exhibit superconductivity and ferromagnetism are rare due the antagonistic relationship between conventional spin-singlet superconductivity and ferromagnetic order. In materials in which superconductivity and magnetic order is known to coexist (such as some heavy-fermion materials), the superconductivity is thought to be of an unconventional nature. Recently, the conducting gas that lives at the interface between the perovskite band insulators LaAlO$_3$ (LAO) and SrTiO$_3$ (STO) has also been shown to host both superconductivity and magnetism. Most previous research has focused on LAO/STO samples in which the interface is in the (001) crystal plane. Relatively little work has focused on the (111) crystal orientation, which has hexagonal symmetry at the interface, and has been predicted to have potentially interesting topological properties, including unconventional superconducting pairing states. Here we report measurements of the magnetoresistance of (111) LAO/STO heterostructures at temperatures at which they are also superconducting. As with the (001) structures, the magnetoresistance is hysteretic, indicating the coexistence of magnetism and superconductivity, but in addition, we find that this magnetoresistance is anisotropic. Such an anisotropic response is completely unexpected in the superconducting state, and suggests that (111) LAO/STO heterostructures may support unconventional superconductivity.

cond-mat.str-el

Electrical Properties and Subband Occupancy at the (La,Sr)(Al,Ta)O$_3$/SrTiO$_3$ Interface

The quasi two-dimensional electron gas (q-2DEG) at oxide interfaces provides a platform for investigating quantum phenomena in strongly correlated electronic systems. Here, we study the transport properties at the high-mobility (La$_{0.3}$Sr$_{0.7}$)(Al$_{0.65}$Ta$_{0.35}$)O$_{0.3}$/SrTiO$_{0.3}$ (LSAT/STO) interface. Before oxygen annealing, the as-grown interface exhibits a high electron density and electron occupancy of two subbands: higher-mobility electrons ($μ_1\approx{10^4}$ cm$^2$V$^{-1}$s$^{-1}$ at 2 K) occupy the lower-energy $3d_{xy}$ subband, while lower-mobility electrons ($μ_1\approx{10^3}$ cm$^{2}$V$^{-1}$s$^{-1}$ at 2 K) propagate in the higher-energy $3d_{xz/yz}$-dominated subband. After removing oxygen vacancies by annealing in oxygen, only a single type of 3dxy electrons remain at the annealed interface, showing tunable Shubnikov-de Haas (SdH) oscillations below 9 T at 2 K and an effective mass of $0.7m_e$. By contrast, no oscillation is observed at the as-grown interface even when electron mobility is increased to $50,000$ cm$^{2}$V$^{-1}$s$^{-1}$ by gating voltage. Our results reveal the important roles of both carrier mobility and subband occupancy in tuning the quantum transport at oxide interfaces.

cond-mat.str-el