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Varun Harbola

Publications and source records attributed to Varun Harbola.

10 recordsLinked to original sources

Reconfigurable Strain Gradient Polarity in Crystalline Oxide Nanomembranes for Controlled Bending of Functional Materials

We report the fabrication and mechanical characterization of a "bubble" geometry for accessing local strain gradients using freestanding, single-crystalline manganite nanomembranes: a switchable bistable nanodrum, with opposite strain gradient polarities. By leveraging epitaxial strain as a source of pre-strain and with control of geometrical and mechanical boundary conditions, the fabricated device can support strain gradients with strain variation ranging from 0.01% to 1%. Switching energetics can be designed to configure the bubble morphology. By providing a mechanical framework for sustained strain gradients, this platform supports scalable oxide membrane applications such as the mechanical manipulation of magnetism, coupled to local probes.

cond-mat.mtrl-sci

Optical Signature of Moir\'e Superlattices Formed by Twisted SrTiO$_3$ Membranes

Moir\'e superlattices formed at the interfaces of mismatched lattices have attracted significant interest over the past decade due to their large tunability of band parameters and interactions among electrons, spins, and lattices. Superlattices made from twisted perovskite oxides may have strong structure and potential modulation, but evidence of such modulation over macroscopic areas, particularly at large twisting angles, has not been clearly demonstrated so far. Here, we fabricated millimeter-scale twisted oxide bilayers at $36^\circ$ angle, close to the simple coincidence site lattice condition $\Sigma5$, from freestanding SrTiO$_3$ membranes. We discovered new low-frequency vibrational modes whose Raman activity, according to molecular dynamics simulations, is greatly enhanced by an asymmetric, twisted interface between the SrO and TiO$_2$ layers. Such an interface is energetically favorable from first-principles calculations and is corroborated by the observation of strong second harmonic generation from the interface comparable to that from the SrTiO$_3$ surface throughout the bilayer region. The results are consistent with interlayer coupling enhanced by high-temperature annealing and confirmed by cross-sectional scanning transmission electron microscopy imaging. Our work sheds light on the structural behavior of twisted oxides and provides directions for tuning their phononic and nonlinear optical properties in future studies.

cond-mat.mtrl-sci

Instability-driven mechanically locked states in functional oxide membranes

Mechanical instabilities in thin solids offer a powerful route to engineer nonlinear responses, yet their controlled use in functional crystalline oxides has remained largely unexplored. Notably, by changing the aspect ratio of solids, the energy landscape around equilibrium can be modified to induce non-linearities under lateral stresses through non-lateral deformations. These nonlinear systems can develop multiple local energy minima where the system can settle and switch between states through the application of a driving force. Crucially, recent advances in oxide thin film growth have enabled the fabrication of freestanding oxide membranes, paving a viable path for their use in bistable architecture, particularly at the nanoscale. Here, we demonstrate that freestanding oxide membranes, such as SrTiO3 (STO) and BaTiO3 (BTO), relax into well-defined metastable buckling states when transferred onto lithographically defined cavities. The membrane deformation is determined by the interplay between built-in residual strain, bending stiffness, and cavity geometry, resulting in reproducible bistable states with distinct strain distributions. Using a combination of atomic force microscopy, in-contact Kelvin probe measurements, and finite-element modelling, we reveal that these mechanically locked states directly shape the electromechanical potential landscape of ferroelectric BaTiO3. We further demonstrate reversible snapthrough transitions between mechanically degenerate states, establishing complex oxides as deterministic, geometry-tunable building blocks for nonlinear nanoelectromechanical architectures. Our results illustrate a general strategy for exploiting mechanical instabilities to encode and manipulate functional responses in ultrathin crystalline membranes.

cond-mat.mtrl-sci

Microscopic mechanisms of flexoelectricity in oxide membranes

Modern electromechanical actuators and sensors rely on the piezoelectric effect that linearly couples strain and electric polarization. However, this effect is restricted to materials that lack inversion symmetry. In contrast, the flexoelectric effect couples strain gradients to electric polarization, and is a universal property in insulating materials of arbitrary symmetry. Flexoelectricity becomes prominent at the nanoscale from the inverse scaling of strain gradients with material dimensions. Here, we measure the strain-gradient-induced structural distortions in strontium titanate using multislice electron ptychography. This technique enables reliable picometer-scale measurements of the dominant oxygen-titanium distortions, correcting for artifacts that limited conventional imaging methods. This enables us to directly measure the sign of the net ionic contribution to the flexoelectric polarization. Guided by the experimental measurements, first-principles calculations show how the sign and magnitude of the bulk contribution to the flexoelectric coefficient in strontium titanate can be switched by tuning the strain state. Hybridization between the optical soft phonon and acoustic phonon modes drives this transition, yielding a large response and a polarity switch across the resonance. This strain-dependence might explain the sign discrepancy and orders of magnitude variation in the values of previously reported flexoelectric coefficients for strontium titanate. As the strain state of curved membranes can be tuned, our approach also suggests an approach to engineer nanoscale flexoelectric polarization using strain as a control parameter.

cond-mat.mtrl-sci

alpha-Ta Films on c-plane Sapphire with Enhanced Microstructure

Superconducting films of alpha-Ta are promising candidates for the fabrication of advanced superconducting qubits. However, alpha-Ta films suffer from many growth-induced structural inadequacies that negatively affect their performance. We have therefore explored a new synthesis method for alpha-Ta films which allows the growth of these films with unprecedented quality. Using this method, high quality alpha-Ta films are deposited at a comparably high substrate temperature of 1150 C. They are single-phase alpha-Ta and have a single out-of-plane (110) orientation. They consist of grains above 2 um that have one of three possible in-plane orientations. As shown by scanning transmission electron microscopy and electron energy loss studies the substrate-film interfaces are sharp with no observable intermixing. The obtained insights into the epitaxial growth of body-centered-cubic films on quasi-hexagonal substrates lay the basis for harnessing the high structural coherence of such films in various applications.

cond-mat.supr-con

Vector-substrate-based Josephson junctions

We present a way to We present a way to fabricate bicrystal Josephson junctions of high-Tc cuprate superconductors that does not require bulk bicrystalline substrates. Based on vector substrate technology, this novel approach makes use of a few tens-of-nanometers-thick bicrystalline membranes transferred onto conventional substrates.We demonstrate 24° YBa2Cu3O7-x Josephson junctions fabricated on sapphire single crystals by utilizing 10-nm-thick bicrystalline membranes of SrTiO3. This technique allows one to manufacture bicrystalline Josephson junctions of high-Tc superconductors on a large variety of bulk substrate materials, providing novel degrees of freedom in designing the junctions and their electronic properties. It furthermore offers the capability to replace the fabrication of bulk bicrystalline substrates with thin-film growth methods

cond-mat.supr-con

Interface Design Beyond Epitaxy: Oxide Heterostructures Comprising Symmetry-forbidden Interfaces

Epitaxial growth of thin-film heterostructures is generally considered the most successful procedure to obtain interfaces of excellent structural and electronic quality between three-dimensional materials. However, these interfaces can only join material systems with crystal lattices of matching symmetries and lattice constants. We present a novel category of interfaces, the fabrication of which is membrane-based and does not require epitaxial growth. These interfaces therefore overcome limitations imposed by epitaxy. Leveraging the additional degrees of freedom gained, we demonstrate atomically clean interfaces between three-fold symmetric sapphire and four-fold symmetric SrTiO3. Atomic-resolution imaging reveals structurally well-defined interfaces with a novel moiré-type reconstruction.

cond-mat.mtrl-sci

Fracture and Fatigue of Thin Crystalline SrTiO$_3$ Membranes

The increasing availability of a variety of two-dimensional materials has generated enormous growth in the field of nanoengineering and nanomechanics. Recent developments in thin film synthesis have enabled the fabrication of freestanding functional oxide membranes that can be readily incorporated in nanomechanical devices. While many oxides are extremely brittle in bulk, recent studies have shown that, in thin membrane form, they can be much more robust to fracture as compared to their bulk counterparts. Here, we investigate the ultimate tensile strength of SrTiO$_3$ membranes by probing freestanding SrTiO$_3$ drumheads using an atomic force microscope. We demonstrate that SrTiO$_3$ membranes can withstand an elastic deformation with an average strain of ~6% in the sub-20 nm thickness regime, which is more than an order of magnitude beyond the bulk limit. We also show that these membranes are highly resilient upon a high cycle fatigue test, surviving up to a billion cycles of force modulation at 85% of their fracture strain, demonstrating their high potential for use in nanomechanical applications.

physics.app-ph

Giant strain gradient elasticity in SrTiO3 membranes: bending versus stretching

Young's modulus determines the mechanical loads required to elastically stretch a material, and also, the loads required to bend it, given that bending stretches one surface while compressing the opposite one. Flexoelectric materials have the additional property of becoming electrically polarized when bent. While numerous studies have characterized this flexoelectric coupling, its impact on the mechanical response, due to the energy cost of polarization upon bending, is largely unexplored. This intriguing contribution of strain gradient elasticity is expected to become visible at small length scales where strain gradients are geometrically enhanced, especially in high permittivity insulators. Here we present nano-mechanical measurements of freely suspended SrTiO3 membrane drumheads. We observe a striking non-monotonic thickness dependence of Young's modulus upon small deflections. Furthermore, the modulus inferred from a predominantly bending deformation is three times larger than that of a predominantly stretching deformation for membranes thinner than 20 nm. In this regime we extract a giant strain gradient elastic coupling of ~2.2e-6 N, which could be used in new operational regimes of nano-electro-mechanics.

cond-mat.mtrl-sci

Strain-Induced Room-Temperature Ferroelectricity in SrTiO$_3$ Membranes

Advances in complex oxide heteroepitaxy have highlighted the enormous potential of utilizing strain engineering via lattice mismatch to control ferroelectricity in thin-film heterostructures. This approach, however, lacks the ability to produce large and continuously variable strain states, thus limiting the potential for designing and tuning the desired properties of ferroelectric films. Here, we observe and explore dynamic strain-induced ferroelectricity in SrTiO$_3$ by laminating freestanding oxide films onto a stretchable polymer substrate. Using a combination of scanning probe microscopy, optical second harmonic generation measurements, and atomistic modeling, we demonstrate robust room-temperature ferroelectricity in SrTiO$_3$ with 2.0% uniaxial tensile strain, corroborated by the notable features of 180° ferroelectric domains and an extrapolated transition temperature of 400 K. Our work reveals the enormous potential of employing oxide membranes to create and enhance ferroelectricity in environmentally benign lead-free oxides, which hold great promise for applications ranging from non-volatile memories and microwave electronics.

cond-mat.mtrl-sci