arXiv subjects

Bharat Jalan

Publications and source records attributed to Bharat Jalan.

At least 55 records · Page 3Linked to original sources

arXiv2021

Hysteretic Magnetoresistance in a Non-Magnetic SrSnO3 Film via Thermal Coupling to Dynamic Substrate Behavior

Hysteretic magnetoresistance (MR) is often used as a signature of ferromagnetism in conducting oxide thin films and heterostructures. Here, magnetotransport is investigated in a non-magnetic uniformly La-doped SrSnO3 film grown using hybrid molecular beam epitaxy. A 12 nm La:SrSnO3/2 nm SrSnO3/GdScO3 (110) film with insulating behavior exhibited a robust hysteresis loop in the MR at T < 5 K accompanied by an anomaly at ~ +/- 3 T at T < 2.5 K. Furthermore, MR with the field in-plane yielded a value exceeded 100% at 1.8 K. Using detailed temperature-, angle- and magnetic field-dependent resistance measurements, we illustrate the origin of hysteresis is not due to magnetism in the film but rather is associated with the magnetocaloric effect of the GdScO3 substrate. Given GdScO3 and similar substrates are commonly used in complex oxide research, this work highlights the importance of thermal coupling to processes in the substrates which must be carefully accounted for in the data interpretation for thin films and heterostructures utilizing these substrates.

cond-mat.mtrl-sci↗

arXiv2021

Solid Source Metal-Organic Molecular Beam Epitaxy of Epitaxial RuO2

A seemingly simple oxide with a rutile structure, RuO2 has been shown to possess several intriguing properties ranging from strain-stabilized superconductivity to a strong catalytic activity. Much interest has arisen surrounding the controlled synthesis of RuO2 films but, unfortunately, utilizing atomically-controlled deposition techniques like molecular beam epitaxy (MBE) has been difficult due to the ultra-low vapor pressure and low oxidation potential of Ru. Here, we demonstrate the growth of epitaxial, single-crystalline RuO2 films on different substrate orientations using the novel solid-source metal-organic (MO) MBE. This approach circumvents these issues by supplying Ru using a pre-oxidized solid metal-organic precursor containing Ru. High-quality epitaxial RuO2 films with bulk-like room-temperature resistivity of 55 micro-ohm-cm were obtained at a substrate temperature as low as 300 C. By combining X-ray diffraction, transmission electron microscopy, and electrical measurements, we discuss the effect of substrate temperature, orientation, film thickness, and strain on the structure and electrical properties of these films. Our results illustrating the use of novel solid-source MOMBE approach paves the way to the atomic-layer controlled synthesis of complex oxides of stubborn metals, which are not only difficult to evaporate but also hard to oxidize.

cond-mat.mtrl-sci↗

arXiv2021

Direct observation and consequences of dopant segregation inside and outside dislocation cores in perovskite BaSnO3

Distinct dopant behaviors inside and outside dislocation cores are identified by atomic-resolution electron microscopy in perovskite BaSnO3 with considerable consequences on local atomic and electronic structures. Driven by elastic strain, when A-site designated La dopants segregate near a dislocation core, the dopant atoms accumulate at the Ba sites in compressively strained regions. This triggers formation of Ba-vacancies adjacent to the core atomic sites resulting in reconstruction of the core. Notwithstanding the presence of extremely large tensile strain fields, when La atoms segregate inside the dislocation core, they become B-site dopants, replacing Sn atoms and compensating the positive charge of the core oxygen vacancies. Electron energy-loss spectroscopy shows that the local electronic structure of these dislocations changes dramatically due to the segregation of the dopants inside and around the core ranging from formation of strong La-O hybridized electronic states near the conduction band minimum to insulator-to-metal transition.

cond-mat.mtrl-sci↗

arXiv2021

Surface state at $BaSnO_3$ evidenced by angle-resolved photoemission spectroscopy and ab initio calculations

Perovskite alkaline earth stannates, such as $BaSnO_3$ and $SrSnO_3$, showing light transparency and high electrical conductivity (when doped), have become promising candidates for novel optoelectrical devices. Such devices are mostly based on hetero-structures and understanding of their electronic structure, which usually deviates from the bulk, is mandatory for exploring a full application potential. Employing angle-resolved photoemission spectroscopy and ab initio calculations we reveal the existence of a 2-dimensional metallic state at the $SnO_2$-terminated surface of a 1\% La-doped $BaSnO_3$ thin film. The observed surface state is characterized by distinct carrier density and a smaller effective mass in comparison with the corresponding bulk values. The small surface effective mass of about $0.12m_e$ can cause an improvement of the electrical conductivity of BSO based heterostructures.

cond-mat.mtrl-sci↗

arXiv2020

Strain Relaxation via Phase Transformation in SrSnO3

SrSnO3 (SSO) is an emerging ultra-wide bandgap (UWBG) semiconductor with potential for highpower applications. In-plane compressive strain was recently shown to stabilize the high temperature tetragonal phase of SSO at room temperature (RT) which exists at T > 1062 K in bulk. Here, we report on the study of strain relaxation in epitaxial, tetragonal phase of Nd-doped SSO films grown on GdScO3 (110) (GSO) substrates using radical-based hybrid molecular beam epitaxy. The thinnest SSO film (thickness, t = 12 nm) yielded a fully coherent tetragonal phase at RT. At 12 nm < t < 110 nm, the tetragonal phase first transformed into orthorhombic phase and then at t > 110 nm, the orthorhombic phase began to relax by forming misfit dislocations. Remarkably, the tetragonal phase remained fully coherent until it completely transformed into the orthorhombic phase. Using thickness- and temperature-dependent electronic transport measurements, we discuss the important roles of the surface, phase coexistence, and misfit dislocations on carrier density and mobility in Nd-doped SSO. This study provides unprecedented insights into the strain relaxation behavior and its consequences for electronic transport in doped SSO with implications in the development of high-power electronic devices.

cond-mat.mtrl-sci↗

arXiv2020

Impurity Band Conduction in Si-doped \b{eta}-Ga2O3 Films

By combining temperature-dependent resistivity and Hall effect measurements, we investigate donor state energy in Si-doped \b{eta}-Ga2O3 films grown using metal-organic vapor phase epitaxy (MOVPE). High magnetic field Hall effect measurements (H = +/-90 kOe) showed non-linear Hall resistance for T < 150 K revealing two-band conduction. Further analyses revealed carrier freeze-out characteristics in both bands yielding donor state energies of ~ 33.7 and ~ 45.6 meV. The former is consistent with the donor energy of Si in \b{eta}-Ga2O3 whereas the latter suggests a residual donor state, likely associated with a DX center. This study provides a critical insight into the impurity band conduction and the defect energy states in \b{eta}-Ga2O3 using high-field magnetotransport measurements.

cond-mat.mtrl-sci↗

arXiv2020

Self-Assembled Periodic Nanostructures Using Martensitic Phase Transformations

We describe a novel approach for the rational design and synthesis of self-assembled periodic nanostructures using martensitic phase transformations. We demonstrate this approach in a thin film of perovskite SrSnO3 with reconfigurable periodic nanostructures consisting of regularly spaced regions of sharply contrasted dielectric properties. The films can be designed to have different periodicities and relative phase fractions via chemical doping or strain engineering. The dielectric contrast within a single film can be tuned using temperature and laser wavelength, effectively creating a variable photonic crystal. Our results show the realistic possibility of designing large-area self-assembled periodic structures using martensitic phase transformations with the potential of implementing "built-to-order" nanostructures for tailored optoelectronic functionalities.

cond-mat.mtrl-sci↗

arXiv2020

Electronic Structure and Small Hole Polarons in YTiO3

As a prototypical Mott insulator with ferromagnetic ordering, YTiO3 (YTO) is of great interest in the study of strong electron correlation effects and orbital ordering. Here we report the first molecular beam epitaxy (MBE) growth of YTO films, combined with theoretical and experimental characterization of the electronic structure and charge transport properties. The obstacles of YTO MBE growth are discussed and potential routes to overcome them are proposed. DC transport and Seebeck measurements on thin films and bulk single crystals identify p-type Arrhenius transport behavior, with an activation energy of ~ 0.17 eV in thin films, consistent with the energy barrier for small hole polaron migration from hybrid density functional theory (DFT) calculations. Hard X-ray photoelectron spectroscopy measurements (HAXPES) show the lower Hubbard band (LHB) at 1.1 eV below the Fermi level, whereas a Mott-Hubbard band gap of ~1.5 eV is determined from photoluminescence (PL) measurements. These findings provide critical insight into the electronic band structure of YTO and related materials.

cond-mat.mtrl-sci↗

arXiv2020

Precursor Selection in Hybrid Molecular Beam Epitaxy of Alkaline-Earth Stannates

One of the challenges of oxide molecular beam epitaxy (MBE) is the synthesis of oxides containing metals with high electronegativity (metals that are hard to oxidize). The use of reactive organometallic precursors can potentially address this issue. To investigate the formation of radicals in MBE, we explored three carefully chosen metal-organic precursors of tin for SnO2 and BaSnO3 growth: tetramethyltin (TMT), tetraethyltin (TET), and hexamethylditin (HMDT). All three precursors produced single-crystalline, atomically smooth, and epitaxial SnO2 (101) films on r-Al2O3 in the presence of an oxygen plasma. The study of growth kinetics revealed reaction-limited and flux-limited regimes except for TET, which also exhibited a decrease in deposition rate with increasing temperature above 800 C. Contrary to these similarities, the performance of these precursors was dramatically different for BaSnO3 growth. TMT and TET were ineffective in supplying adequate tin whereas HMDT yielded phase-pure, stoichiometric BaSnO3 films. Significantly, HMDT resulted in phase-pure and stoichiometric BaSnO3 films even without the use of an oxygen plasma (i.e., with molecular oxygen alone). These results are discussed using the ability of HMDT to form tin radicals and therefore, assisting with Sn to Sn4+ oxidation reaction. Structural and electronic transport properties of films grown using HMDT with and without oxygen plasma are compared. This study provides guideline for the choice of precursors that will enable synthesis of metal oxides containing hard-to-oxidize metals using reactive radicals in MBE.

cond-mat.mtrl-sci↗

arXiv2020

From Weak Antilocalization to Kondo Scattering in a Magnetic Complex Oxide Interface

Quantum corrections to electrical resistance can serve as sensitive probes of the magnetic landscape of a material. For example, interference between time-reversed electron paths gives rise to weak localization effects, which can provide information about the coupling between spins and orbital motion, while the Kondo effect is sensitive to the presence of spin impurities. Here we use low-temperature magnetotransport measurements to reveal a transition from weak antilocalization (WAL) to Kondo scattering in the quasi-two-dimensional electron gas formed at the interface between SrTiO$_3$ and the Mott insulator NdTiO$_3$. This transition occurs as the thickness of the NdTiO$_3$ layer is increased. Analysis of the Kondo scattering and WAL points to the presence of atomic-scale magnetic impurities coexisting with extended magnetic regions that affect transport via a strong magnetic exchange interaction. This leads to distinct magnetoresistance behaviors that can serve as a sensitive probe of magnetic properties in two dimensions.

cond-mat.mtrl-sci↗

arXiv2020

Effects of paramagnetic pair-breaking and spin-orbital coupling on multi-band superconductivity

The BCS picture of superconductivity describes pairing between electrons originating from a single band. A generalization of this picture occurs in multi-band superconductors, where electrons from two or more bands contribute to superconductivity. The contributions of the different bands can result in an overall enhancement of the critical field and can lead to qualitative changes in the temperature dependence of the upper critical field when compared to the single-band case. While the role of orbital pair-breaking on the critical field of multi-band superconductors has been explored extensively, paramagnetic and spin-orbital scattering effects have received comparatively little attention. Here we investigate this problem using thin films of Nd-doped SrTiO$_3$. We furthermore propose a model for analyzing the temperature-dependence of the critical field in the presence of orbital, paramagnetic and spin-orbital effects, and find a very good agreement with our data. Interestingly, we also observe a dramatic enhancement in the out-of-plane critical field to values well in excess of the Chandrasekhar-Clogston (Pauli) paramagnetic limit, which can be understood as a consequence of multi-band effects in the presence of spin-orbital scattering.

cond-mat.supr-con↗

arXiv2020

Machine Learning Analysis of Perovskite Oxides Grown by Molecular Beam Epitaxy

Reflection high-energy electron diffraction (RHEED) is a ubiquitous in situ molecular beam epitaxial (MBE) characterization tool. Although RHEED can be a powerful means for crystal surface structure determination, it is often used as a static qualitative surface characterization method at discrete intervals during a growth. A full analysis of RHEED data collected during the entirety of MBE growths is made possible using principle component analysis (PCA) and k-means clustering to examine significant boundaries that occur in the temporal clusters grouped from RHEED data and identify statistically significant patterns. This process is applied to data from homoepitaxial SrTiO$_{3}$ growths, heteroepitaxial SrTiO$_{3}$ grown on scandate substrates, BaSnO$_{3}$ films grown on SrTiO$_{3}$ substrates, and LaNiO$_{3}$ films grown on LaAlO$_{3}$ substrates. This analysis may provide additional insights into the surface evolution and transitions in growth modes at precise times and depths during growth, and that video archival of an entire RHEED image sequence may be able to provide more insight and control over growth processes and film quality.

cond-mat.mtrl-sci↗

arXiv2019

Disentangling spin-orbit coupling and local magnetism in a quasi-two-dimensional electron system

Quantum interference between time-reversed electron paths in two dimensions leads to the well-known weak localization correction to resistance. If spin-orbit coupling is present, the resistance correction is negative, termed weak anti-localization (WAL). Here we report the observation of WAL coexisting with exchange coupling between itinerant electrons and localized magnetic moments. We use low-temperature magneto-transport measurements to investigate the quasi-two-dimensional, high-electron-density interface formed between SrTiO$_3$ (STO) and the anti-ferromagnetic Mott insulator NdTiO$_3$ (NTO). As the magnetic field angle is gradually tilted away from the sample normal, the data reveals the interplay between strong $k$-cubic Rashba-type spin-orbit coupling and a substantial magnetic exchange interaction from local magnetic regions. The resulting quantum corrections to the conduction are in excellent agreement with existing models and allow sensitive determination of the small magnetic moments (22 $μ_B$ on average), their magnetic anisotropy and mutual coupling strength. This effect is expected to arise in other 2D magnetic materials systems.

cond-mat.mes-hall↗

arXiv2019

Dopant Solubility, and Charge Compensation in La-doped SrSnO3 Films

We investigate lanthanum (La) as an n-type dopant in the strain-stabilized tetragonal phase of SrSnO3 grown on GdScO3 (110) using a radical-based hybrid molecular beam epitaxy approach. Fully coherent, epitaxial films with atomically smooth film surface were obtained irrespective of doping density. By combining secondary ion mass spectroscopy and Hall measurements, we demonstrate that each La atom contributes to one electron to the film confirming it occupies Sr-site in SrSnO3 and that it is completely activated. Carrier density exceeding 1 x 10^20 cm-3 was achieved in LSSO films, which is in excellent agreement with the dopant-solubility limit predicted by the density functional theory calculations. A record-high room-temperature mobility of 70 cm2V-1s-1 at 1 x 10^20 cm-3 was obtained in 12 nm La-doped SrSnO3 film making this the thinnest perovskite oxide semiconductor with a reasonably high electron mobility at room temperature. We discuss the structure-dopant-transport property relationships providing essential knowledge for the design of electronic devices using these materials.

cond-mat.mtrl-sci↗

arXiv2019

STEM beam channeling in BaSnO3/LaAlO3 perovskite bilayers and visualization of 2D misfit dislocation network

A study of the STEM probe channeling in a heterostructures crystalline specimen is presented here with a goal to guide appropriate STEM-based characterization for complex structures. STEM analysis of perovskite BaSnO3/LaAlO3 bilayers is performed and the dominating effects of beam channeling on HAADF- and LAADF-STEM are illustrated. To study the electron beam propagating through BaSnO3/LaAlO3 bilayers, probe intensity depth profiles are calculated, and the effects of probe defocus and atomic column alignment are discussed. Characteristics of the beam channeling are correlated to resulting ADF-STEM images, which is then tested by comparing focal series of plan-view HAADF-STEM images to those recorded experimentally. Additionally, discussions on how to visualize the misfit dislocation network at the BaSnO3/LaAlO3 interface using HAADF- and LAADF-STEM images are provided.

cond-mat.mtrl-sci↗

arXiv2019

Unraveling the Effect of Electron-Electron Interaction on Electronic Transport in High-Mobility Stannate Films

Contrary to the common belief that electron-electron interaction (EEI) should be negligible in s-orbital-based conductors, we demonstrated that the EEI effect could play a significant role on electronic transport leading to the misinterpretation of the Hall data. We show that the EEI effect is primarily responsible for an increase in the Hall coefficient in the La-doped SrSnO3 films below 50 K accompanied by an increase in the sheet resistance. The quantitative analysis of the magnetoresistance (MR) data yielded a large phase coherence length of electrons exceeding 450 nm at 1.8 K and revealed the electron-electron interaction being accountable for breaking of electron phase coherency in La-doped SrSnO3 films. These results while providing critical insights into the fundamental transport behavior in doped stannates also indicate the potential applications of stannates in quantum coherent electronic devices owing to their large phase coherence length.

cond-mat.mtrl-sci↗

arXiv2019

Separating Electrons and Donors in BaSnO3 via Band Engineering

Through a combination of thin film growth, hard X-ray photoelectron spectroscopy (HAXPES), scanning transmission electron microscopy/electron energy loss spectroscopy (STEM/EELS), magneto-transport measurements, and transport modeling, we report on the demonstration of modulation-doping of BaSnO3 (BSO) using a wider bandgap La-doped SrSnO3 (LSSO) layer. Hard X-ray photoelectron spectroscopy (HAXPES) revealed a valence band offset of 0.71 +/- 0.02 eV between LSSO and BSO resulting in a favorable conduction band offset for remote doping of BSO using LSSO. Nonlinear Hall effect of LSSO/BSO heterostructure confirmed two-channel conduction owing to electron transfer from LSSO to BSO and remained in good agreement with the results of self-consistent solution to one-dimensional Poisson and Schrödinger equations. Angle-dependent HAXPES measurements revealed a spatial distribution of electrons over 2-3 unit cells in BSO. These results bring perovskite oxides a step closer to room-temperature oxide electronics by establishing modulation-doping approaches in non-SrTiO3-based oxide heterostructure.

cond-mat.mtrl-sci↗

arXiv2018

Hopping Transport in SrTiO3/Nd1-xTiO3/SrTiO3 Heterostructures

Electronic transport near the insulator-metal transition is investigated in the molecular beam epitaxy-grown SrTiO3/Nd1-xTiO3/SrTiO3 heterostructures using temperature dependent magnetotransport measurements. It was found that Nd-vacancies introduce localized electronic states resulting in the variable range hopping transport at low temperatures. At a fixed Nd-vacancies concentration, a crossover from Mott to Efros-Shklovskii (ES) variable range hopping transport was observed with decreasing temperature. With increasing disorder, a sign reversal of magnetoresistance from positive to negative was observed revealing interplay between intra-state interaction and the energy dependence of the localization length as a function of disorder. These findings highlight the important role of stoichiometry when exploring intrinsic effect using heterostructure and interfaces in addition to offering broad opportunity to tailor low temperature transport using non-stoichiometry defects.

cond-mat.mtrl-sci↗