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Harold Y. Hwang

Publications and source records attributed to Harold Y. Hwang.

At least 73 records · Page 4Linked to original sources

Nickelate superconductivity without rare-earth magnetism: (La,Sr)NiO$_{2}$

The observation of superconductivity in infinite layer nickelate (Nd,Sr)NiO$_{2}$ thin films has led to rapid theoretical and experimental investigations of these copper-oxide-analogue systems [1-15]. Superconductivity has also been found in (Pr,Sr)NiO$_{2}$ [16,17], but not previously in (La,Sr)NiO$_{2}$ [2], raising a fundamental question whether superconductivity is associated with the presence of rare-earth moments [18,19]. Here we show that with significant materials optimization, substantial portions of the La$_{1-x}$Sr$_{x}$NiO$_{2}$ phase diagram can enter the regime of coherent low-temperature transport ($x$ = 0.14 - 0.20), with subsequent superconducting transitions and a maximum onset of ~ 9 K at $x$ = 0.20. Additionally, we observe the unexpected indication of a superconducting ground state in undoped LaNiO$_{2}$, which likely reflects the self-doped nature of the electronic structure. Combining the results of (La/Pr/Nd)$_{1-x}$Sr$_{x}$NiO$_{2}$ reveals a generalized superconducting dome, characterized by systematic shifts in the unit cell volume and in the relative electron-hole populations across the lanthanides.

cond-mat.supr-con↗

Non-universal current flow near the metal-insulator transition in an oxide interface

In systems near phase transitions, macroscopic properties often follow algebraic scaling laws, determined by the dimensionality and the underlying symmetries of the system. The emergence of such universal scaling implies that microscopic details are irrelevant. Here, we locally investigate the scaling properties of the metal-insulator transition at the LaAlO3/SrTiO3 interface. We show that, by changing the dimensionality and the symmetries of the electronic system, coupling between structural and electronic properties prevents the universal behavior near the transition. By imaging the current flow in the system, we reveal that structural domain boundaries modify the filamentary flow close to the transition point, preventing a fractal with the expected universal dimension from forming. Our results offer a generic platform to engineer electronic transitions on the nanoscale.

cond-mat.mes-hall↗

Electronic Structure Trends Across the Rare-Earth Series in Superconducting Infinite Layer Nickelates

The recent discovery of superconductivity in oxygen-reduced monovalent nickelates has raised a new platform for the study of unconventional superconductivity, with similarities and differences with the cuprate high temperature superconductors. In this paper we investigate the family of infinite-layer nickelates $R$NiO$_2$ with rare-earth $R$ spanning across the lanthanide series, introducing a new and non-trivial "knob" with which to tune nickelate superconductivity. When traversing from La to Lu, the out-of-plane lattice constant decreases dramatically with an accompanying increase of Ni $ d_{x^2-y^2}$ bandwidth; however, surprisingly, the role of oxygen charge transfer diminishes. In contrast, the magnetic exchange grows across the lanthanides which may be favorable to superconductivity. Moreover, compensation effects from the itinerant $5d$ electrons present a closer analogy to Kondo lattices, indicating a stronger interplay between charge transfer, bandwidth renormalization, compensation, and magnetic exchange. We also obtain the microscopic Hamiltonian using Wannier downfolding technique, which will provide the starting point for further many-body theoretical studies.

cond-mat.supr-con↗

Universal behavior of the bosonic metallic ground state in a two-dimensional superconductor

Anomalous metallic behavior, marked by a saturating finite resistivity much lower than the Drude estimate, has been observed in a wide range of two-dimensional superconductors. Utilizing the electrostatically gated LaAlO3/SrTiO3 interface as a versatile platform for superconductor-metal quantum phase transitions, we probe variations in the gate, magnetic field, and temperature to construct a phase diagram crossing from superconductor, anomalous metal, vortex liquid, to Drude metal states, combining longitudinal and Hall resistivity measurements. We find that the anomalous metal phases induced by gating and magnetic field, although differing in symmetry, are connected in the phase diagram and exhibit similar magnetic field response approaching zero temperature. Namely, within a finite regime of the anomalous metal state, the longitudinal resistivity linearly depends on field while the Hall resistivity diminishes, indicating an emergent particle-hole symmetry. The universal behavior highlights the uniqueness of the quantum bosonic metallic state, distinct from bosonic insulators and vortex liquids.

cond-mat.supr-con↗

Universal bound to the amplitude of the vortex Nernst signal in superconductors

A liquid of superconducting vortices generates a transverse thermoelectric response. This Nernst signal has a tail deep in the normal state due to superconducting fluctuations. Here, we present a study of the Nernst effect in two-dimensional hetero-structures of Nb-doped strontium titanate (STO) and in amorphous MoGe. The Nernst signal generated by ephemeral Cooper pairs above the critical temperature has the magnitude expected by theory in STO. On the other hand, the peak amplitude of the vortex Nernst signal below $T_c$ is comparable in both and in numerous other superconductors despite the large distribution of the critical temperature and the critical magnetic fields. In four superconductors belonging to different families, the maximum Nernst signal corresponds to an entropy per vortex per layer of $\approx$ k$_Bln2$.

cond-mat.supr-con↗

Phase Diagram of Infinite Layer Praseodymium Nickelate Pr$_{1-x}$Sr$_{x}$NiO$_2$ Thin Films

We report the phase diagram of infinite layer Pr$_{1-x}$Sr$_{x}$NiO$_2$ thin films synthesized via topotactic reduction from the perovskite precursor phase using CaH$_2$. Based on the electrical transport properties, we find a doping-dependent superconducting dome extending between $x$ = 0.12 and 0.28, with a maximum superconducting transition temperature $T_{\rm{c}}$ of 14 K at $x$ = 0.18, bounded by weakly insulating behavior on both sides. In contrast to the narrower dome observed in Nd$_{1-x}$Sr$_{x}$NiO$_2$, a local $T_{\rm{c}}$ suppression near $x$ = 0.2 was not observed for the Pr$_{1-x}$Sr$_{x}$NiO$_2$ system. Normal state Hall effect measurements indicate mixed carrier contributions of both electrons and holes, and show a sign change in the Hall coefficient as functions of temperature and $x$, quite similar to that in Nd$_{1-x}$Sr$_{x}$NiO$_2$. Also similar is the observation of a minimum in the normal state resistivity associated with the superconducting compositions. These findings indicate an infinite layer nickelate phase diagram that is relatively insensitive to the rare-earth element, but suggest that disorder arising from the variations of the ionic radii on the rare-earth site affects the superconducting dome.

cond-mat.supr-con↗

Isotropic Pauli-Limited Superconductivity in the Infinite Layer Nickelate Nd$_{0.775}$Sr$_{0.225}$NiO$_{2}$

The recent observation of superconductivity in thin film infinite-layer nickelates$^{1-3}$ offers a different angle to investigate superconductivity in layered oxides$^{4}$. A wide range of candidate models have been proposed$^{5-10}$, emphasizing single- or multi-orbital electronic structure, Kondo or Hund's coupling, and analogies to cuprates. Clearly, further experimental characterization of the superconducting state is needed to develop a full understanding of the nickelates. Here we use magnetotransport measurements to probe the superconducting anisotropy in Nd$_{0.775}$Sr$_{0.225}$NiO$_{2}$. We find that the upper critical field is surprisingly isotropic at low temperatures despite the layered crystal structure. In a magnetic field the superconductivity is strongly Pauli-limited, such that the paramagnetic effect dominates over orbital de-pairing. Underlying this isotropic response is a substantial anisotropy in the superconducting coherence length, which is at least four times longer in-plane than out-of-plane. A prominent low-temperature upturn in the upper critical field indicates the presence of an unconventional ground state.

cond-mat.supr-con↗

Charge order textures induced by non-linear lattice coupling in a half-doped manganite

The self-organization of strongly interacting electrons into superlattice structures underlies the properties of many quantum materials. How these electrons arrange within the superlattice dictates what symmetries are broken and what ground states are stabilized. Here we show that cryogenic scanning transmission electron microscopy enables direct mapping of local symmetries and order at the intra-unit-cell level in the model charge-ordered system Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$. In addition to imaging the prototypical site-centered charge order, we discover the nanoscale coexistence of an exotic intermediate state which mixes site and bond order and breaks inversion symmetry. We further show that nonlinear coupling of distinct lattice modes controls the selection between competing ground states. The results demonstrate the importance of lattice coupling for understanding and manipulating the character of electronic self-organization and highlight a novel method for probing local order in a broad range of strongly correlated systems.

cond-mat.str-el↗

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↗

A superconducting praseodymium nickelate with infinite layer structure

A variety of nickel oxide compounds have long been studied for their manifestation of various correlated electron phenomena. Recently, superconductivity was observed in nanoscale infinite layer nickelate thin films of Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, epitaxially stabilized on SrTiO$_3$ substrates via topotactic reduction from the perovskite precursor phase. Here we present the synthesis and properties of PrNiO$_2$ thin films on SrTiO$_3$. Upon doping in Pr$_{0.8}$Sr$_{0.2}$NiO$_2$, we observe superconductivity with a transition temperature of 7-12 K, and robust critical current density at 2 K of 334 kA/cm$^2$. These findings indicate that superconductivity in the infinite layer nickelates is relatively insensitive to the details of the rare earth 4$f$ configuration. Furthermore, they motivate the exploration of a broader family of compounds based on two-dimensional NiO$_2$ planes, which will enable systematic investigation of the superconducting and normal state properties and their underlying mechanisms.

cond-mat.supr-con↗

Superconducting Dome in Nd$_{1-x}$Sr$_x$NiO$_2$ Infinite Layer Films

We report the phase diagram of Nd$_{1-x}$Sr$_x$NiO$_2$ infinite layer thin films grown on SrTiO$_3$. A superconducting dome spanning $0.125 < x < 0.25$ is found, remarkably similar to cuprates, albeit over a narrower doping window. However, while cuprate superconductivity is bounded by an insulator for underdoping and a metal for overdoping, here we observe weakly insulating behavior on either side of the dome. Furthermore, the normal state Hall coefficient is always small and proximate to a continuous zero crossing in doping and in temperature, in contrast to the $\sim 1/x$ dependence observed for cuprates. This suggests the presence of both electron- and hole-like bands, consistent with band structure calculations.

cond-mat.supr-con↗

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↗

Aspects of the Synthesis of Thin Film Superconducting Infinite-Layer Nickelates

The recent observation of superconductivity in Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$ calls for further investigation and optimization of the synthesis of this metastable infinite-layer nickelate structure. Here, we present our current understanding of important aspects of the growth of the parent perovskite compound via pulsed laser deposition on SrTiO$_{3}$ (001) substrates, and the subsequent topotactic reduction. We find that to achieve single-crystalline, single-phase superconducting Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$, it is essential that the precursor perovskite Nd$_{0.8}$Sr$_{0.2}$NiO$_{3}$ thin film is stabilized with high crystallinity and no impurity phases; in particular, a Ruddlesden-Popper-type secondary phase is often observed. We have further investigated the evolution of the soft-chemistry topotactic reduction conditions to realize full transformation to the infinite-layer structure with no film decomposition or formation of other phases. We find that capping the nickelate film with a subsequent SrTiO$_{3}$ layer provides an epitaxial template to the top region of the nickelate film, much like the substrate. Thus, for currently optimized growth conditions, we can stabilize superconducting single-phase Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$ (001) epitaxial thin films up to ~ 10 nm.

cond-mat.mtrl-sci↗

Doping evolution of the Mott-Hubbard landscape in infinite-layer nickelates

The recent observation of superconductivity in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ has raised fundamental questions about the hierarchy of the underlying electronic structure. Calculations suggest that this system falls in the Mott-Hubbard regime, rather than the charge-transfer configuration of other nickel oxides and the superconducting cuprates. Here, we use state-of-the-art, locally-resolved electron energy loss spectroscopy to directly probe the Mott-Hubbard character of Nd$_{1-x}$Sr$_x$NiO$_2$. Upon doping, we observe emergent hybridization reminiscent of the Zhang-Rice singlet via the oxygen-projected states, modification of the Nd 5$d$ states, and the systematic evolution of Ni 3$d$ hybridization and filling. These results clearly evidence the multiband nature of this system and the distinct electronic landscape for infinite-layer nickelates despite their formal similarity to the cuprates.

cond-mat.supr-con↗

Robust $d_{x^2-y^2}$-wave superconductivity of infinite-layer nickelates

Motivated by the recent observation of superconductivity in strontium doped NdNiO$_2$, we study the superconducting instabilities in this system from various vantage points. Starting with first-principles calculations, we construct two distinct tight-binding models, a simpler single-orbital as well as a three-orbital model, both of which capture the key low energy degrees of freedom to varying degree of accuracy. We study superconductivity in both models using the random phase approximation (RPA). We then analyze the problem at stronger coupling, and study the dominant pairing instability in the associated t-J model limit. In all instances, the dominant pairing tendency is in the $d_{x^2-y^2}$ channel, analogous to the cuprate superconductors.

cond-mat.supr-con↗

Electrostatic modulation of the lateral carrier density profile in field effect devices with non-linear dielectrics

We study the effects of electrostatic gating on the lateral distribution of charge carriers in two dimensional devices, in a non-linear dielectric environment. We compute the charge distribution using the Thomas-Fermi approximation to model the electrostatics of the system. The electric field lines generated by the gate are focused at the edges of the device, causing an increased depletion near the edges, compared to the center of the device. This effect strongly depends on the dimensions of the device, and the non-linear dielectric constant of the substrate. We experimentally demonstrate this effect using scanning superconducting interference device (SQUID) microscopy images of current distributions in gated LaAlO$_3$/SrTiO$_3$ heterostructures.

cond-mat.mes-hall↗

Observation of the signatures of sub-resolution defects in two-dimensional superconductors with scanning SQUID

The diamagnetic susceptibility of a superconductor is directly related to its superfluid density. Mutual inductance is a highly sensitive method for characterizing thin films; however, in traditional mutual inductance measurements, the measured response is a non-trivial average over the area of the mutual inductance coils, which are typically of millimeter size. Here we image localized, isolated features in the diamagnetic susceptibility of δ-doped SrTiO3, the 2-DES at the interface between LaAlO3 and SrTiO3, and Nb superconducting thin film systems using scanning superconducting quantum interference device susceptometry, with spatial resolution as fine as 0.7 μm. We show that these features can be modeled as locally suppressed superfluid density, with a single parameter that characterizes the strength of each feature. This method provides a systematic means of finding and quantifying submicron defects in two-dimensional superconductors.

cond-mat.supr-con↗

Dual-Gate Modulation of Carrier Density and Disorder in an Oxide Two-Dimensional Electron System

Carrier density and disorder are two crucial parameters that control the properties of correlated two-dimensional electron systems. In order to disentangle their individual contributions to quantum phenomena, independent tuning of these two parameters is required. Here, by utilizing a hybrid liquid/solid electric dual-gate geometry acting on the conducting LaAlO3/SrTiO3 heterointerface, we obtain an additional degree of freedom to strongly modify the electron confinement profile and thus the strength of interfacial scattering, independent from the carrier density. A dual-gate controlled nonlinear Hall effect is a direct manifestation of this profile, which can be quantitatively understood by a Poisson-Schrodinger subband model. In particular, the large nonlinear dielectric response of SrTiO3 enables a very wide range of tunable density and disorder, far beyond that for conventional semiconductors. Our study provides a broad framework for understanding various reported phenomena at the LaAlO3/SrTiO3 interface.

cond-mat.str-el↗