arXiv subjects

Bharat Jalan

Publications and source records attributed to Bharat Jalan.

At least 37 records · Page 2Linked to original sources

arXiv2025

Ferroelectric Switching in Hybrid Molecular Beam Epitaxy-Grown BaTiO3 Films

Molecular beam epitaxy (MBE) is a promising synthesis technique for both heterostructure growth and epitaxial integration of ferroelectric BaTiO3. However, a direct measurement of the remnant polarization (P_r) has not been previously reported in MBE-grown BaTiO3 films. We report the in-situ growth of an all-epitaxial SrRuO3/BaTiO3/SrRuO3 heterostructure on Nb-doped SrTiO3 (001) substrates by hybrid MBE using metal-organic precursors. This capacitor structure consisting of 16 nm SrRuO3/40 nm BaTiO3/16 nm SrRuO3 shows hysteretic polarization-electric field (P-E) curves with P_r = 15 μC cm-2 at frequencies ranging from 500 Hz to 20 kHz, after isolating the intrinsic ferroelectric response from non-ferroelectric contributions using the Positive-Up-Negative-Down (PUND) method. We hypothesize that the asymmetry in switching behavior and current leakage has origins in structural defects.

cond-mat.mtrl-sci↗

arXiv2025

Coexistence of unconventional spin Hall effect and antisymmetric planar Hall effect in IrO$_2$

Crystal symmetry plays an important role in the Hall effects. Unconventional spin Hall effect (USHE), characterized by Dresselhaus and out-of-plane spins, has been observed in materials with low crystal symmetry. Recently, antisymmetric planar Hall effect (APHE) was discovered in rutile RuO2 and IrO2 (101) thin films, which also exhibit low crystal symmetry. In this study, we report the observation of both USHE and APHE in IrO2 (111) films, using spin-torque ferromagnetic resonance (ST-FMR) and harmonic Hall measurements, respectively. Notably, the unconventional spin torque efficiency from Dresselhaus spin was more than double that of a previous report. Additionally, the temperature dependence of APHE suggests that it arises from the Lorentz force, constrained by crystal symmetry. Symmetry analysis supports the coexistence of USHE and APHE and demonstrates that both originate from the crystal symmetry of IrO2 (111), paving the way for a deeper understanding of Hall effects and related physical phenomena.

cond-mat.mes-hall↗

arXiv2025

Altermagnetic Polar Metallic phase in Ultra-Thin Epitaxially-Strained RuO2 Films

Altermagnetism refers to a wide class of magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetries, resulting in non-trivial spin splitting and magnetic multipoles. However, the direct observation of the altermagnetic order parameter remains elusive. Here, by combining theoretical analysis, electrical transport, X-ray and optical spectroscopies, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO2/TiO2 (110) films, mapping symmetries along with altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This features a novel altermagnetic metallic polar phase in epitaxially-strained 2 nm films, extending the concept of multiferroicity to altermagnets. Such a clear signature of a magnetic phase transition at ~500 K is observed exclusively in ultrathin strained films, unlike in bulk RuO2 single crystals. These results demonstrate the potential of epitaxial heterostructure design to induce altermagnetism, paving the way for emergent novel phases with multifunctional properties.

cond-mat.mtrl-sci↗

arXiv2025

Absence of two-phonon quasi-elastic scattering in the normal state of doped--SrTiO$_3$ by THz pump-probe spectroscopy

Multi-pulse nonlinear THz spectroscopies enable a new understanding of interacting metallic systems via their sensitivity to novel correlation functions. Here, we investigated the THz nonlinear properties of the dilute metallic phase of doped-SrTiO$_3$ thin films using nonlinear terahertz 2D coherent spectroscopy. We observed a large $χ^{(3)}$ response in the low temperature region where the dc electrical resistivity follows a T$^2$-dependence. This is largely a pump-probe response, which we find is governed by a single energy relaxation rate that is much smaller at all temperatures than the momentum relaxation rates obtained from the optical conductivity. This indicates that the processes that dominate the resistive scattering are not the same as those that remove energy from the electronic system. Moreover the fact that the energy relaxation rate is an increasing function of temperature indicates that the excitations that do carry away energy from the electronic system cannot be considered as quasi-elastic and as such soft two-phonon electron scattering does not play a major role in the physics as proposed. This indicates that these materials' resistive T$^2$ scattering likely originates in electron-electron interactions despite the very small Fermi wave vectors at the lowest dopings.

cond-mat.str-el↗

arXiv2025

Metallicity and Anomalous Hall Effect in Epitaxially-Strained, Atomically-thin RuO2 Films

The anomalous Hall effect (AHE), a hallmark of time-reversal symmetry breaking, has been reported in rutile RuO2, a debated metallic altermagnetic candidate. Previously, AHE in RuO2 was observed only in strain-relaxed thick films under extremely high magnetic fields (~50 T). Yet, in ultrathin strained films with distinctive anisotropic electronic structures, there are no reports, likely due to disorder and defects suppressing metallicity thus hindering its detection. Here, we demonstrate that ultrathin, fully-strained 2 nm TiO2/t nm RuO2/TiO2 (110) heterostructures, grown by hybrid molecular beam epitaxy, retain metallicity and exhibit a sizeable AHE at a significantly lower magnetic field (< 9 T). Density functional theory calculations reveal that epitaxial strain stabilizes a non-compensated magnetic ground state and reconfigures magnetic ordering in RuO2 (110) thin films. These findings establish ultrathin RuO2 as a platform for strain-engineered magnetism and underscore the transformative potential of epitaxial design in advancing spintronic technologies.

cond-mat.mtrl-sci↗

arXiv2024

High-Mobility Carriers in Epitaxial IrO2 Films Grown using Hybrid Molecular Beam Epitaxy

Binary rutile oxides of 5d metals such as IrO2, stand out as a paradox due to limited experimental studies despite the rich predicted quantum phenomena. Here, we investigate the electrical transport properties of IrO2 by engineering epitaxial thin films grown via hybrid molecular beam epitaxy. Our findings reveal phonon-limited carrier transport and thickness-dependent anisotropic in-plane resistance in IrO2 (110) films, the latter suggesting a complex relationship between strain relaxation and orbital hybridization. Magneto-transport measurements reveal a previously unobserved non-linear Hall effect. A two-carrier analysis of this effect shows the presence of minority carriers with mobility exceeding 3000 cm2/Vs at 1.8 K. These results point towards emergent properties in 5d metal oxides that can be controlled using dimensionality and epitaxial strain.

cond-mat.mtrl-sci↗

arXiv2024

Epitaxially Grown Single-Crystalline SrTiO3 Membranes Using a Solution-Processed, Amorphous SrCa2Al2O6 Sacrificial Layer

Water-soluble sacrificial layers based on epitaxially-grown, single crystalline (Ca, Sr, Ba)3Al2O6 layer are widely used for creating free-standing perovskite oxide membranes. However, obtaining these sacrificial layers with intricate stoichiometry remains a challenge, especially for molecular beam epitaxy (MBE). In this study, we demonstrate the hybrid MBE growth of epitaxial, single crystalline SrTiO3 films using a solution processed, amorphous SrCa2Al2O6 sacrificial layer onto SrTiO3 (001) substrates. Prior to the growth, the oxygen plasma exposure was used to first create the crystalline SrCa2Al2O6 layer with well-defined surface crystallinity. Utilizing reflection high energy electron diffraction, x-ray diffraction, and atomic force microscopy, we observe an atomic layer-by-layer growth of epitaxial, single crystalline SrTiO3 film on the SrCa2Al2O6 layer with atomically smooth surfaces. The SrCa2Al2O6 layer was subsequently dissolved in de-ionized water to create free-standing SrTiO3 membranes that were transferred onto a metal-coated Si wafer. Membranes created with Sr-deficiency revealed ferroelectric-like behavior measured using piezo force microscopy whereas stoichiometric films remained paraelectric-like. These findings underscore the viability of using ex-situ deposited amorphous SrCa2Al2O6 for epitaxial, single crystalline growth, as well as the importance of point defects in determining the ferroic properties in membranes.

cond-mat.mtrl-sci↗

arXiv2024

Deep-ultraviolet transparent conducting SrSnO3 via heterostructure design

Exploration and advancements in ultra-wide bandgap (UWBG) semiconductors are pivotal for next-generation high-power electronics and deep-ultraviolet (DUV) optoelectronics. A critical challenge lies in finding a semiconductor that is highly transparent to DUV wavelengths yet conductive with high mobility at room temperature. Here, we achieved both high transparency and high conductivity by employing a thin heterostructure design. The heterostructure facilitated high conductivity by screening phonons using free carriers, while the atomically thin films ensured high transparency. We utilized a heterostructure comprising SrSnO3/La:SrSnO3/GdScO3 (110) and applied electrostatic gating to effectively separate electrons from their dopant atoms. This led to a modulation of carrier density from 1018 cm-3 to 1020 cm-3, with room temperature mobilities ranging from 40 to 140 cm2V-1s-1. The phonon-limited mobility, calculated from first principles, closely matched experimental results, suggesting that room-temperature mobility could be further increased with higher electron density. Additionally, the sample exhibited 85% optical transparency at a 300 nm wavelength. These findings highlight the potential of heterostructure design for transparent UWBG semiconductor applications, especially in deep-ultraviolet regime.

cond-mat.mtrl-sci↗

arXiv2024

Moiré polar vortex, flat bands and Lieb lattice in twisted bilayer BaTiO$_3$

Advances in material fabrication techniques and growth methods have opened up a new chapter for twistronics, in the form of twisted freestanding three-dimensional material membranes. Through first-principles calculations based on density functional theory, we investigate the crystal and electronic structures of twisted bilayer BaTiO$_3$. Our findings reveal that large stacking fault energy leads to chiral in-plane vortex pattern that was recently observed in experiments. Moreover, we also found non-zero out-of-plane local dipole moments, indicating that the strong interlayer interaction might offer promising strategy to stabilize ferroelectric order in the two-dimensional limit. Remarkably, the vortex pattern in the twisted BaTiO$_3$ bilayer support localized electronic states with quasi-flat bands, associated with the interlayer hybridization of oxygen $p_z$ orbitals. We found that the associated band width reaches a minimum at $\sim$19$^{\circ}$ twisting, configuring the largest magic angle in moiré systems reported so far. Further, the moiré vortex pattern bears a striking resemblance to two interpenetrating Lieb lattices and corresponding tight-binding model provides a comprehensive description of the evolution the moiré bands with twist angle and reveals the topological nature of these states.

cond-mat.mtrl-sci↗

arXiv2024

Anomalous frequency and temperature dependent scattering in the dilute metallic phase in lightly doped-SrTiO$_3$

The mechanism of superconductivity in materials with aborted ferroelectricity and the emergence of a dilute metallic phase in systems like doped-SrTiO$_3$ are outstanding issues in condensed matter physics. This dilute metal has features both similar and different to those found in the normal state of other unconventional superconductors. We have investigated the optical properties of the dilute metallic phase in doped-SrTiO$_3$ using THz time-domain spectroscopy. At low frequencies the THz response exhibits a Drude-like form as expected for typical metal-like conductivity. We observed the frequency and temperature dependencies to the low energy scattering rate $Γ(ω, T) \propto (\hbarω)^2 + (p πk_BT)^2 $ expected in a conventional Fermi liquid, despite the fact that densities are too small to allow current decay through electron-electron scattering. However we find the lowest known $p$ values of 0.39-0.72. As $p$ is 2 in a canonical Fermi liquid and existing models based on energy dependent elastic scattering bound $p$ from below to 1, our observation lies outside current explanation. Our data also gives insight into the high temperature regime and shows that the temperature dependence of the resistivity derives in part from strong T dependent mass renormalizations.

cond-mat.str-el↗

arXiv2024

Site-Specific Plan-view (S)TEM Sample Preparation from Thin Films using a Dual-Beam FIB-SEM

Plan-view transmission electron microscopy (TEM) samples are key to understand the atomic structure and associated properties of materials along their growth orientation, especially for thin films that are stain-engineered onto different substrates for property tuning. In this work, we present a method to prepare high-quality plan-view samples for analytical STEM study from thin-films using a dual-beam focused ion beam scanning electron microscope (FIB-SEM) system. The samples were prepared from thin films of perovskite oxides and metal oxides ranging from 20-80 nm thicknesses, grown on different substrates using molecular beam epitaxy. A site-specific sample preparation from the area of interest is described, which includes sample attachment and thinning techniques to minimize damage to the final TEM samples. While optimized for the thin film-like geometry, this method can be extended to other site-specific plan-view samples from bulk materials. Aberration-corrected scanning (S)TEM was used to access the quality of the thin film in each sample. This enabled direct visualization of line defects in perovskite BaSnO3 and Ir particle formation and texturing in IrO2 films.

physics.app-ph↗

arXiv2023

Thickness-dependent insulator-to-metal transition in epitaxial RuO2 films

Epitaxially grown RuO2 films on TiO2 (110) exhibit significant in-plane strain anisotropy, with a compressive strain of - 4.7% along the [001] crystalline direction and a tensile strain of +2.3% along [1-10]. As the film thickness increases, anisotropic strain relaxation is expected. By fabricating Hall bar devices with current channels along two in-plane directions <001> and <1-10>, we revealed anisotropic in-plane transport in RuO2/TiO2 (110) films grown via solid-source metal-organic molecular beam epitaxy approach. For film thicknesses (t_film) < 3.6 nm, the resistivity along <001> exceeds that along <1-10> direction at all temperatures. With further decrease in film thicknesses, we uncover a transition from metallic to insulating behavior at t_film <2.1 nm. Our combined temperature- and magnetic field-dependent electrical transport measurements reveal that this transition from metallic to insulating behavior is driven by electron-electron interactions.

cond-mat.mtrl-sci↗

arXiv2023

Fast and Facile Synthesis Route to Epitaxial Oxide Membrane Using a Sacrificial Layer

The advancement in thin-film exfoliation for synthesizing oxide membranes has opened up new possibilities for creating artificially-assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques like Molecular Beam Epitaxy (MBE). This is where easy-to-grow binary alkaline earth metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of single-crystalline perovskite SrTiO3 (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba1-xCaxO films, employing a hybrid MBE method. Our results highlight the rapid (< 5 minutes) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution x-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate epitaxial STO membranes with bulk-like intrinsic dielectric properties. The employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding research possibilities.

physics.app-ph↗

arXiv2023

Mending Cracks in Rutile TiO$_{2}$ with Electron Beam

Restructuring of rutile TiO$_{2}$ under electron beam irradiation driven by radiolysis was observed and analyzed using a combination of atomic-resolution imaging and electron energy loss spectroscopy (EELS) in scanning transmission electron microscopy (STEM). It was determined that a high-energy (80-300 keV) electron beam at high doses ($\gtrapprox 10^7 \ e/nm^2$) can constructively restructure rutile TiO$_{2}$ with an efficiency of $6\times 10^{-6}$. These observations were realized using rutile TiO$_{2}$ samples with atomically sharp nanometer-wide cracks. Based on atomic-resolution STEM imaging and quantitative EELS analysis, we propose a $"$ 2-step $"$ rolling model of the octahedral building blocks of the crystal to account for observed radiolysis-driven atomic migration.

cond-mat.mtrl-sci↗

arXiv2023

Effect of Pt vacancies on magnetotransport of Weyl semimetal candidate GdPtSb epitaxial films

We examine the effects of Pt vacancies on the magnetotransport properties of Weyl semimetal candidate GdPtSb films, grown by molecular beam epitaxy on c-plane sapphire. Rutherford backscattering spectrometry (RBS) and x-ray diffraction measurements suggest that phase pure GdPt$_{x}$Sb films can accommodate up to $15\%$ Pt vacancies ($x=0.85$), which act as acceptors as measured by Hall effect. Two classes of electrical transport behavior are observed. Pt-deficient films display a metallic temperature dependent resistivity (d$ρ$/dT$>$0). The longitudinal magnetoresistance (LMR, magnetic field $\mathbf{B}$ parallel to electric field $\mathbf{E}$) is more negative than transverse magnetoresistance (TMR, $\mathbf{B} \perp \mathbf{E}$), consistent with the expected chiral anomaly for a Weyl semimetal. The combination of Pt-vacancy disorder and doping away from the expected Weyl nodes; however, suggests conductivity fluctuations may explain the negative LMR rather than chiral anomaly. Samples closer to stoichiometry display the opposite behavior: semiconductor-like resistivity (d$ρ$/dT$<$0) and more negative transverse magnetoresistance than longitudinal magnetoresistance. Hysteresis and other nonlinearities in the low field Hall effect and magnetoresistance suggest that spin disorder scattering, and possible topological Hall effect, may dominate the near stoichiometric samples. Our findings highlight the complications of transport-based identification of Weyl nodes, but point to possible topological spin textures in GdPtSb.

cond-mat.mtrl-sci↗

arXiv2022

Free-Standing Epitaxial SrTiO$_3$ Nanomembranes via Remote Epitaxy using Hybrid Molecular Beam Epitaxy

The epitaxial growth of functional materials using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining free-standing epitaxial nano-membranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically employed to grow epitaxial perovskite oxides can damage graphene. Here, we demonstrate a technique based on hybrid molecular beam epitaxy that does not require an independent oxygen source to achieve epitaxial growth of complex oxides without damaging the underlying graphene. The technique produces films with self-regulating cation stoichiometry control and epitaxial orientation to the oxide substrate. Furthermore, the films can be exfoliated and transferred to foreign substrates while leaving the graphene on the original substrate. These results open the door to future studies of previously unattainable free-standing nano-membranes grown in an adsorption-controlled manner by hybrid molecular beam epitaxy, and has potentially important implications for the commercial application of perovskite oxides in flexible electronics.

cond-mat.mtrl-sci↗

arXiv2022

Hybrid Molecular Beam Epitaxy of Ge-based Oxides

Germanium-based oxides such as rutile GeO2 are garnering attention owing to their wide band gaps and the prospects for ambipolar doping for application in high-power devices. Here, we present the use of germanium tetraisopropoxide (GTIP) (an organometallic chemical precursor) as a source of Ge for the demonstration of hybrid molecular beam epitaxy (MBE) for Ge-containing compounds. We use Sn1-xGexO2 and SrSn1-xGexO3 as model systems to demonstrate this new synthesis method. A combination of high-resolution X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy confirms the successful growth of epitaxial rutile Sn1-xGexO2 on TiO2(001) substrates up to x = 0.54 and coherent perovskite SrSn1-xGexO3 on GdScO3(110) substrates up to x = 0.16. Characterization and first-principles calculations corroborate that Ge preferentially occupies the Sn site, as opposed to the Sr site. These findings confirm the viability of the GTIP precursor for the growth of germanium-containing oxides by hybrid MBE, and thus open the door to high-quality perovskite germanate films.

cond-mat.mtrl-sci↗

arXiv2021

Anomalous Transport in High-Mobility Superconducting SrTiO$_3$ Thin Films

The study of subtle effects on transport in semiconductors requires high-quality epitaxial structures with low defect density. Using hybrid molecular beam epitaxy (MBE), SrTiO$_3$ films with low-temperature mobility exceeding 42,000 cm$^2$V$^{-1}$s$^{-1}$ at low carrier density of 3 x 10$^{17}$ cm$^{-3}$ were achieved. A sudden and sharp decrease in residual resistivity accompanied by an enhancement in the superconducting transition temperature were observed across the second Lifshitz transition (LT) where the third band becomes occupied, revealing dominant intra-band scattering. These films further revealed an anomalous behavior in the Hall carrier density as a consequence of the antiferrodistortive (AFD) transition and the temperature-dependence of the Hall scattering factor. Using hybrid MBE growth, phenomenological modeling, temperature-dependent transport measurements, and scanning superconducting quantum interference device imaging, we provide critical insights into the important role of inter- vs intra-band scattering and of AFD domain walls on normal-state and superconducting properties of SrTiO$_3$.

cond-mat.supr-con↗