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Lopa Bhatt

Publications and source records attributed to Lopa Bhatt.

13 recordsLinked to original sources

Persistent structural distortions and absent superconductivity in trilayer nickelate thin films

A new family of high-temperature superconductors was recently discovered in the $n=2,3$ Ruddlesden-Popper nickelates, where superconductivity emerges concomitant with suppression of parent density waves and structural octahedral rotations under hydrostatic pressure. Intriguingly, compressive strain mimics the structural effects of pressure in the $n=2$ phase, yielding ambient-pressure superconductivity. However, analogous strain-stabilized superconductivity has not been realized in the $n=3$. Here, we use atomically-precise synthesis, transport, picoscale electron microscopy, and synchrotron X-ray diffraction to probe $n=3$ La$_4$Ni$_3$O$_{10}$ thin films. Although compressive strain suppresses density wave order, we do not observe superconductivity even under the largest strain state. Importantly, we identify a structural distortion unique to strained $n=3$ thin films that may inhibit superconductivity: persistent, layer-inequivalent octahedral rotations around the $c$-axis. Our results highlight key differences between the $n=3$ and $n=2$ systems, suggesting that ambient-pressure superconductivity in the $n=3$ may require new methods beyond epitaxial strain engineering.

cond-mat.mtrl-sci

Breaking symmetry to create a parallel-plate varactor dielectric with unparalleled microwave performance

Voltage-tunable capacitors (varactors) are key to microwave circuits. Tunable dielectric varactors outperform competing technologies in almost every relevant metric but usually suffer from high dielectric loss. In contrast, Ruddlesden-Popper (RPs) dielectric thin films have remarkably low microwave loss. Unfortunately, their crystallographic symmetry has until recently dictated an in-plane device structure, precluding the favorable out-of-plane parallel-plate varactor design for minimized size and maximized electric field in the tunable dielectric. Guided by theory, we report RPs akin to the widely studied tunable microwave dielectric BaxSr1-xTiO3. Assembling these same atoms into the first RP phase with broken out-of-plane symmetry, we achieve a low-loss, out-of-plane tunable dielectric thin film. The highest performing film, (ATiO3)nAO film with A = Ba0.45Sr0.55 and n = 8, unlocks a tenfold improvement in the figure of merit for out-of-plane tunable dielectrics at 10 GHz, paving the way for a new generation of tunable monolithic microwave integrated circuits.

cond-mat.mtrl-sci

Coherent spin waves in a maximal entropy phase

In solids, disorder is conventionally regarded as detrimental to coherence. It typically localizes and dampens collective excitations, as exemplified by Anderson localization or the broadening of magnetic modes in systems lacking long-range order. While high-entropy materials are specifically designed to harness disorder and stabilize homogeneous mixed-phase structures that can display unique properties, this same disorder is nonetheless expected to preclude the formation of coherent magnetic excitations. To test the limits of this picture, we selected the antiferromagnetic system YBaCuFeO5, as it features two distinct transition metal atoms with significantly different magnetic moments, rendering its spin dynamics exceptionally sensitive to local atomic ordering. Combining resonant inelastic x-ray scattering and linear spin wave theory, we reveal a surprising paradox: YBaCuFeO5 exhibits an unexpected, entropy-driven mixed phase, in which disorder, rather than reducing the lifetime of the collective excitations, favors coherence. In this mixed phase, the spin waves remain dispersive, markedly distinct from those expected for an ordered ground state, and exhibit well-defined acoustic and optical branches separated by a large optical gap. These results demonstrate that in entropy-stabilized magnets, disorder can favor coherent collective modes previously thought to be exclusive to low-entropy systems.

cond-mat.str-el

A superconducting half-dome in bilayer nickelates

Understanding how superconductivity emerges and collapses in correlated electron systems remains a central challenge in condensed matter physics. As a recently discovered member of the high temperature superconductor family, bilayer nickelates provide a new opportunity for examining this problem. Their pronounced sensitivity to oxygen stoichiometry, while posing challenges for stabilizing superconductivity, simultaneously offers an effective control parameter for tuning electronic phases. Here we report a superconducting half-dome in compressively strained bilayer nickelate thin films as a function of continuous tuning of oxygen stoichiometry. Starting from an optimally superconducting state, increasing oxygen stoichiometry gradually suppresses superconductivity toward a metallic phase, whereas decreasing oxygen stoichiometry drives a granular superconductor-to-insulator transition while leaving the superconducting onset intact. This half-dome structure can be understood to arise from the contrasting roles played by interstitial oxygen versus oxygen vacancies - namely the dominance of doping versus scattering. Notably, the half-dome emerges consistently across samples with different rare-earth combinations, with or without alkaline-earth doping, revealing a general feature of the bilayer nickelate phase diagram.

cond-mat.supr-con

Designing heterostructures to control oxygen stoichiometry in helimagnetic perovskite strontium ferrite

A large challenge in determining the physics of helimagnetic SrFeO3 is in stabilizing the stoichiometric chemical phase over long enough time scales to conduct extensive measurements. Degradation in SrFeO3 manifests mainly as a crossover from metallic to insulating behavior. Using a combination of electronic transport and density functional theory, we show that this degradation is dominated by oxygen loss, possibly on the order of one percent. We further demonstrate that high quality SrFeO3 thin films can be stabilized long-term by combining a nanoscale band insulator capping layer with an ex situ ozone anneal. We show that this produces a nearly-pristine cation sublattice and preserves metallicity for at least several weeks. These results establish a reliable pathway for producing chemically stable SrFeO3 thin films, enabling reproducible studies of its unusual helimagnetism.

cond-mat.mtrl-sci

Superconducting phase diagram of multi-layer square-planar nickelates

The discovery of superconductivity in square-planar nickelates has offered a rich materials platform to explore the origins of cuprate-like superconductivity. Experimental investigations however have largely been limited to the infinite-layer $R$NiO$_2$ ($R$=rare-earth) nickelates. Here, we construct a phase diagram of multi-layer square-planar Nd$_{n+1}$Ni$_n$O$_{2n+2}$ compounds and discover signatures of superconductivity for $n$ = 4 - 8. Upon decreasing the dimensionality $n$, the superconducting anisotropy evolves due to 4$f$ electron effects, and electronic structure characteristics approach cuprate-like behavior. Magnetic fluctuations persist from within the superconducting regime and into the over-doped, non-superconducting regime. Remarkably, the superconducting regime overlaps with that of chemically-doped infinite-layer nickelates, demonstrating underlying commonalities and distinct differences across varying structural realizations of square-planar nickelates. Our work establishes this layered template for creating new nickel-based superconductors.

cond-mat.supr-con

Melting point depression of charge density wave in 1T-TiSe$_2$ due to size effects

Classical nucleation theory predicts size-dependent nucleation and melting due to surface and confinement effects at the nanoscale. In correlated electronic states, observation of size-dependent nucleation and melting is rarely reported, likely due to the extremely small length scales necessary to observe such effects for electronic states. Here, using 1T-TiSe$_2$ nanoflakes as a prototypical two-dimensional (2D) charge density wave (CDW) system, we perform in-situ cryogenic electron microscopy with temperature down to 20 K and observe size-dependent nucleation and melting of CDWs. Specifically, we observe a melting point depression of CDW for 1T-TiSe$_2$ flakes with lateral sizes less than 100 nm. By fitting experimental data to a Ginzburg-Landau model, we estimate a zero-temperature correlation length of 10--50 nm, which matches the reported CDW domain size for 1T-TiSe$_2$. As the flake size approaches the correlation length, the divergence of the CDW correlation length near the transition is cut off by the finite flake size, limiting long-range order and thereby lowering the transition temperature. For very small flakes whose size is close to the correlation length, we also observe absence of CDWs, as predicted by the model. We thus show that an electronic phase transition follows classical nucleation theory.

cond-mat.mtrl-sci

Unconventional superlattice ordering in intercalated transition metal dichalcogenide V$_{1/3}$NbS$_2$

The interplay between symmetry and topology in magnetic materials makes it possible to engineer exotic phases and technologically useful properties. A key requirement for these pursuits is achieving control over local crystallographic and magnetic structure, usually through sample morphology (such as synthesis of bulk crystals versus thin-films) and application of magnetic or electric fields. Here we show that V$_{1/3}$NbS$_2$ can be crystallized in two ordered superlattices, distinguished by the periodicity of out-of-plane magnetic intercalants. Whereas one of these structures is metallic and displays the hallmarks of altermagnetism, the other superlattice, which has not been isolated before in this family of intercalation compounds, is a semimetallic noncollinear antiferromagnet that may enable access to topologically nontrivial properties. This observation of an unconventional superlattice structure establishes a powerful route for tailoring the tremendous array of magnetic and electronic behaviors hosted in related materials.

cond-mat.mtrl-sci

Quantitative approaches for multi-scale structural analysis with atomic resolution electron microscopy

Atomic-resolution imaging with scanning transmission electron microscopy is a powerful tool for characterizing the nanoscale structure of materials, in particular features such as defects, local strains, and symmetry-breaking distortions. In addition to advanced instrumentation, the effectiveness of the technique depends on computational image analysis to extract meaningful features from complex datasets recorded in experiments, which can be complicated by the presence of noise and artifacts, small or overlapping features, and the need to scale analysis over large representative areas. Here, we present image analysis approaches which synergize real and reciprocal space information to efficiently and reliably obtain meaningful structural information with picometer scale precision across hundreds of nanometers of material from atomic-resolution electron microscope images. Damping superstructure peaks in reciprocal space allows symmetry-breaking structural distortions to be disentangled from other sources of inhomogeneity and measured with high precision. Real space fitting of the wave-like signals resulting from Fourier filtering enables absolute quantification of lattice parameter variations and strain, as well as the uncertainty associated with these measurements. Implementations of these algorithms are made available as an open source Python package.

cond-mat.mtrl-sci

Resolving Structural Origins for Superconductivity in Strain-Engineered La$_3$Ni$_2$O$_7$ Thin Films

The discovery of high-temperature superconductivity in bulk La$_3$Ni$_2$O$_7$ under high hydrostatic pressure and, more recently, biaxial compression in epitaxial thin films has ignited significant interest in understanding the interplay between atomic and electronic structure in these compounds. Subtle changes in the nickel-oxygen bonding environment are thought to be key drivers for stabilizing superconductivity, but specific details of which bonds and which modifications are most relevant remains so far unresolved. While direct, atomic-scale structural characterization under hydrostatic pressure is beyond current experimental capabilities, static stabilization of strained La$_3$Ni$_2$O$_7$ films provides a platform well-suited to investigation with new picometer-resolution electron microscopy methods. Here, we use multislice electron ptychography to directly measure the atomic-scale structural evolution of La$_3$Ni$_2$O$_7$ thin films across a wide range of biaxial strains tuned via substrate. By resolving both the cation and oxygen sublattices, we study strain-dependent evolution of atomic bonds, providing the opportunity to isolate and disentangle the effects of specific structural motifs for stabilizing superconductivity. We identify the lifting of crystalline symmetry through modification of the nickel-oxygen octahedral distortions under compressive strain as a key structural ingredient for superconductivity. Rather than previously supposed $c$-axis compression, our results highlight the importance of in-plane biaxial compression in superconducting thin films, which suggests an alternative -- possibly cuprate-like -- understanding of the electronic structure. Identifying local regions of inhomogeneous oxygen stoichiometry and high internal strain near crystalline defects, we suggest potential pathways for improving the sharpness and temperature of the superconducting transition.

cond-mat.supr-con

Superconductivity and normal-state transport in compressively strained La$_2$PrNi$_2$O$_7$ thin films

The discovery of superconductivity under high pressure in Ruddlesden-Popper phases of bulk nickelates has sparked great interest in stabilizing ambient pressure superconductivity in thin-film form using epitaxial strain. Recently, signs of superconductivity have been observed in compressively strained bilayer nickelate thin films with an onset temperature exceeding 40 K, albeit with broad and two-step-like transitions. Here, we report intrinsic superconductivity and normal-state transport properties in compressively strained La$_2$PrNi$_2$O$_7$ thin films, achieved through a combination of isovalent Pr substitution, growth optimization, and precision ozone annealing. The superconducting onset occurs above 48 K, with zero resistance reached above 30 K, and the critical current density at 1.4 K is 100-fold larger than previous reports. The normal-state resistivity exhibits quadratic temperature dependence indicative of Fermi liquid behaviour, and other phenomenological similarities to transport in overdoped cuprates suggest parallels in their emergent properties.

cond-mat.supr-con

Millimeter-scale freestanding superconducting infinite-layer nickelate membranes

Progress in the study of infinite-layer nickelates has always been highly linked to materials advances. In particular, the recent development of superconductivity via hole-doping was predicated on the controlled synthesis of Ni in a very high oxidation state, and subsequent topotactic reduction to a very low oxidation state, currently limited to epitaxial thin films. Here we demonstrate a process to combine these steps with a heterostructure which includes an epitaxial soluble buffer layer, enabling the release of freestanding membranes of (Nd,Sr)NiO2 encapsulated in SrTiO3, which serves as a protective layer. The membranes have comparable structural and electronic properties to that of optimized thin films, and range in lateral dimensions from millimeters to ~100 micron fragments, depending on the degree of strain released with respect to the initial substrate. The changes in the superconducting transition temperature associated with membrane release are quite similar to those reported for substrate and pressure variations, suggestive of a common underlying mechanism. These membranes structures should provide a versatile platform for a range of experimental studies and devices free from substrate constraints.

cond-mat.mtrl-sci

Emergence of Layer Stacking Disorder in c-axis Confined MoTe$_2$

The layer stacking order in 2D materials strongly affects functional properties and holds promise for next generation electronic devices. In bulk, octahedral MoTe$_2$ possesses two stacking arrangements, the Weyl semimetal T$_d$ phase, and the higher-order topological insulator 1T' phase; however, it remains unclear if thin exfoliated flakes of MoTe$_2$ follow the T$_d$, 1T', or an alternative stacking sequence. Here, we resolve this debate using atomic-resolution imaging within the transmission electron microscope. We find that the layer stacking in thin flakes of MoTe$_2$ is highly disordered and pseudo-random, which we attribute to intrinsic confinement effects. Conversely, WTe$_2$, which is isostructural and isoelectronic to MoTe$_2$, displays ordered stacking even for thin exfoliated flakes. Our results are important for understanding the quantum properties of MoTe$_2$ devices, and suggest that thickness may be used to alter the layer stacking in other 2D materials.

cond-mat.mtrl-sci