arXiv subjects

Harold Y. Hwang

Publications and source records attributed to Harold Y. Hwang.

At least 55 records · Page 3Linked to original sources

arXiv2023

Evidence for highly damped Higgs mode in infinite-layer nickelates

The dynamics of Higgs mode in superconductors, manifested as coherent oscillations of the superconducting order parameter amplitude, provides vital insights into the nature of the superconducting gap structure and symmetry. Here we utilize two-dimensional terahertz coherent spectroscopy to investigate Higgs dynamics of a newly discovered infinite-layer nickelate superconductor. While we observe distinct nonlinear terahertz responses from the superconducting state, well-defined long-lived Higgs modes, as commonly observed in $s$-wave superconductors, are entirely absent in the nickelate film. Instead, we find the coherent nonlinear terahertz response is dominated by the quasiparticle excitations. These observations strongly indicate that the Higgs mode in infinite-layer nickelates is heavily damped by the quasiparticle excitations at arbitrarily low energies, which is a characteristic of $d$-wave pairing symmetry. Additionally, by examining the temperature dependence of the nonlinear terahertz response, we discover short-range superconducting fluctuations in the vicinity of $T_\mathrm{c}$. Our findings provide proof of a new $d$-wave system and establish a foundation for investigating the unconventional superconductivity in nickelates.

cond-mat.supr-con↗

arXiv2023

Low-energy electrodynamics of infinite-layer nickelates: evidence for d-wave superconductivity in the dirty limit

The discovery of superconductivity in infinite-layer nickelates establishes a new category of unconventional superconductors that share structural and electronic similarities with cuprates. Despite exciting advances, such as the establishment of a cuprate-like phase diagram and the observation of charge order and short-range antiferromagnetic fluctuation, the key issues of superconducting pairing symmetry, gap amplitude, and superconducting fluctuation remain elusive. In this work, we utilize static and ultrafast terahertz spectroscopy to address these outstanding problems. We demonstrate that the equilibrium terahertz conductivity and nonequilibrium terahertz responses of an optimally Sr-doped nickelate film ($T_c$ = 17 K) are in line with the electrodynamics of $d$-wave superconductivity in the dirty limit. The gap-to-$T_c$ ratio 2$Δ/k_\mathrm{B}T_\mathrm{c}$ is extracted to be 3.4, indicating the superconductivity falls in the weak-coupling regime. In addition, we observed significant superconducting fluctuation near $T_\mathrm{c}$, while it does not extend into the deep normal state as optimally hole-doped cuprates. Our result highlights a new $d$-wave system which closely resembles the electron-doped cuprates, expanding the family of unconventional superconductivity in oxides.

cond-mat.supr-con↗

arXiv2023

The vortex-Nernst effect in a superconducting infinite-layer nickelate

We report measurements of the Nernst and Seebeck effects in Nd$_{1-x}$Sr$_x$NiO$_2$ thin films near the superconducting transition temperature, $T$ = 6.5 - 15 K. Our main result is the observation of a vortex-Nernst signal $S_{yx}(T,H)$ with a maximum at $μ_0H$ = 5 T and a tail that extends to $μ_0H$ $\approx$ 15 T, which we identify as the upper-critical field $H_{c2}$. At $T > T_{\rm c} =$ 6.1 K, $H_{c2}$ remains large (15 T), up to the highest temperature we can resolve from $S_{yx}$ (11 K). These results indicate the existence of a vortex-liquid state over a wide range of finite-resistance temperatures, as in the high-$T_{\rm c}$ cuprates.

cond-mat.supr-con↗

arXiv2023

An electronic band sculpted by oxygen vacancies and indispensable for dilute superconductivity

Dilute superconductivity survives in bulk strontium titanate when the Fermi temperature falls well below the Debye temperature. Here, we show that the onset of the superconducting dome is dopant-dependent. When mobile electrons are introduced by removing oxygen atoms, the superconducting transition survives down to $2 \times 10^{17}$ cm$^{-3}$, but when they are brought by substituting Nb with Ti, the threshold density for superconductivity is an order of magnitude higher. Our study of quantum oscillations reveals a significant difference in the band dispersion between the dilute metals made by these doping routes and our band calculations demonstrate that the rigid band approximation does not hold when mobile electrons are introduced by oxygen vacancies. We identify the band sculpted by theses vacancies as the exclusive locus of superconducting instability in the ultra-dilute limit.

cond-mat.supr-con↗

arXiv2023

Observation of Coulomb blockade and Coulomb staircases in superconducting Pr0.8Sr0.2NiO2 films

Motivated by the discovery of superconductivity in the infinite-layer nickelate family, we report an experimental endeavor to clean the surface of nickelate superconductor Pr0.8Sr0.2NiO2 films by Ar+ ion sputtering and subsequent annealing, and we study their electronic structures by cryogenic scanning tunneling microscopy and spectroscopy. The annealed surfaces are characterized by nano-sized clusters and Coulomb staircases with periodicity inversely proportional to the projected area of the nanoclusters, consistent with a double-barrier tunneling junction model. Moreover, the dynamical Coulomb blockade effects are observed and result in well-defined energy gaps around the Fermi level, which correlate closely with the specific configuration of the junctions. These Coulomb blockade-related phenomena provide an alternative plausible cause of the observed gap structure that should be considered in the spectroscopic understanding of nickelate superconductors with the nano-clustered surface.

cond-mat.supr-con↗

arXiv2023

Emergent chirality in a polar meron to skyrmion phase transition

Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. With the discovery of topologically-stable polar skyrmions, it is of both fundamental and practical interest to understand the microscopic nature and the possibility of temperature- and strain-driven phase transitions in ensembles of such polar skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of -1) to a two-dimensional, tetratic lattice of merons (with topological charge of -1/2) upon varying the temperature and elastic boundary conditions in [(PbTiO3)16/(SrTiO3)16]8 lifted-off membranes. This topological phase transition is accompanied by a change in chirality, from zero-net chirality (in meronic phase) to net-handedness (in skyrmionic phase). To map these changes microscopically required developing new imaging methods. We show how scanning convergent beam electron diffraction provides a robust measure of the local polarization simultaneously with the strain state at sub-nm resolution, while also directly mapping the chirality of each skyrmion. Using this, we demonstrate strain as a crucial order parameter to drive isotropic-to-anisotropic structural transitions of chiral polar skyrmions to non-chiral merons, validated with X-ray reciprocal space mapping and theoretical phase-field simulations. These results revealed by our new measurement methods provide the first illustration of systematic control of rich variety of topological dipole textures by altering the mechanical boundary conditions, which may offer a promising way to control their functionalities in ferroelectric nanodevices using the local and spatial distribution of chirality and order.

cond-mat.mes-hall↗

arXiv2022

Delamination-assisted ultrafast wrinkle formation in a freestanding film

The ability to synthesize and control two-dimensional (2D) crystals creates numerous opportunities for studying emergent states of matter and their novel functionalities. Freestanding films provide a particularly versatile platform for materials engineering in 2D thanks to additional structural motifs not found in films adhered to a flat substrate. A ubiquitous example is wrinkles, yet little is known about how they can develop over as fast as a few picoseconds due to a lack of experimental probes to visualize their dynamics in real time at the nanoscopic scale. Here, we use ultrafast electron diffraction to directly observe light-activated wrinkling formation in a freestanding La$_{2/3}$Ca$_{1/3}$MnO$_3$ film. Via a ``lock-in'' analysis of a single mode of oscillation in the diffraction peak position, intensity, and width, we are able to quantitatively reconstruct how wrinkles develop at the picosecond timescale. Contrary to the common assumption of a fixed boundary condition for freestanding films, we found that wrinkle development is associated with ultrafast delamination at the contact point between the film boundary and the underlying substrate, avoiding a strain build-up in the film. Not only does our work provide a generic protocol to quantify wrinkling dynamics in freestanding films, it also highlights the importance of film-substrate interaction for determining the properties of freestanding structures.

cond-mat.mtrl-sci↗

arXiv2022

Theory of superconductivity in doped quantum paraelectrics

Recent experiments on Nb-doped SrTiO$_3$ have shown that the superconducting energy gap to the transition temperature ratio maintains the Bardeen-Cooper-Schrieffer (BCS) value throughout its superconducting dome. Motivated by these and related studies, we show that the Cooper pairing mediated by a single soft transverse-optical phonon is the most natural mechanism for such a superconducting dome given experimental constraints, and present the microscopic theory for this pairing mechanism. Furthermore, we show that this mechanism is consistent with the $T^2$ resistivity in the normal state. Lastly, we discuss what physical insights SrTiO$_3$ provides for superconductivity in other quantum paraelectrics such as KTaO$_3$.

cond-mat.supr-con↗

arXiv2022

Rare-Earth Control of the Superconducting Upper Critical Field in Infinite-Layer Nickelates

The consequences of varying the rare-earth element in the superconducting infinite-layer nickelates have been much debated. Here we show striking differences in the magnitude and anisotropy of the superconducting upper critical field across the La-, Pr-, and Nd-nickelates. These 5 distinctions originate from the 4f electron characteristics of the rare-earth ions in the lattice: they are absent for La3+, nonmagnetic for the Pr3+ singlet ground state, and magnetic for the Nd3+ Kramer's doublet. The unique polar and azimuthal angle-dependent magnetoresistance found in the Nd-nickelates can be understood to arise from the magnetic contribution of the Nd3+ 4f moments. In the absence of rare-earth effects, we find that the nickelates broadly violate the Pauli limit. Such robust and tunable superconductivity suggests potential in future high-field applications.

cond-mat.supr-con↗

arXiv2022

Character of the "normal state" of the nickelate superconductors

The occurrence of superconductivity in proximity to various strongly correlated phases of matter has drawn extensive focus on their normal state properties, to develop an understanding of the state from which superconductivity emerges. The recent finding of superconductivity in layered nickelates raises similar interests. However, transport measurements of doped infinite-layer nickelate thin films have been hampered by materials limitations of these metastable compounds - in particular, a relatively high density of extended defects. Here, by moving to a substrate (LaAlO$_{3}$)$_{0.3}$(Sr$_{2}$TaAlO$_{6}$)$_{0.7}$ which better stabilizes the growth and reduction conditions, we can synthesize the doping series of Nd$_{1-x}$Sr$_{x}$NiO$_{2}$ essentially free from extended defects. This enables the first examination of the 'intrinsic' temperature and doping dependent evolution of the transport properties. The normal state resistivity exhibits a low-temperature upturn in the underdoped regime, linear behavior near optimal doping, and quadratic temperature dependence for overdoping. This is strikingly similar to the copper oxides, despite key distinctions - namely the absence of an insulating parent compound, multiband electronic structure, and a Mott-Hubbard orbital alignment rather than the charge-transfer insulator of the copper oxides. These results suggest an underlying universality in the emergent electronic properties of both superconducting families.

cond-mat.supr-con↗

arXiv2022

Electronic structure of superconducting nickelates probed by resonant photoemission spectroscopy

The discovery of infinite-layer nickelate superconductors has spurred enormous interest. While the Ni$^{1+}$ cations possess nominally the same 3$d^9$ configuration as Cu$^{2+}$ in cuprates, the electronic structure variances remain elusive. Here, we present a soft x-ray photoemission spectroscopy study on parent and doped infinite-layer Pr-nickelate thin films with a doped perovskite reference. By identifying the Ni character with resonant photoemission and comparison to density functional theory + U (on-site Coulomb repulsion energy) calculations, we estimate U ~5 eV, smaller than the charge transfer energy $Δ$ ~8 eV, confirming the Mott-Hubbard electronic structure in contrast to charge-transfer cuprates. Near the Fermi level ($E_F$), we observe a signature of occupied rare-earth states in the parent compound, which is consistent with a self-doping picture. Our results demonstrate a correlation between the superconducting transition temperature and the oxygen 2$p$ hybridization near $E_F$ when comparing hole-doped nickelates and cuprates.

cond-mat.supr-con↗

arXiv2022

Evidence for nodal superconductivity in infinite-layer nickelates

Infinite-layer nickelates present a new family of potential unconventional superconductors. A key open question is the superconducting pairing symmetry. We present low-temperature measurements of the London penetration depth in optimally doped La_{0.8}Sr_{0.2}NiO_{2}, Pr_{0.8}Sr_{0.2}NiO_{2}, and Nd_{0.8}Sr_{0.2}NiO_{2}. For La and Pr-nickelates, the superfluid density shows a quadratic temperature dependence, indicating nodal superconductivity in the presence of disorder. Nd-nickelate exhibits complex low-temperature behavior, which we attribute to magnetic impurities. These results are consistent with d-wave pairing.

cond-mat.supr-con↗

arXiv2022

Intrinsic magnetism in superconducting infinite-layer nickelates

The discovery of superconductivity in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ [1] introduced a new family of layered nickelate superconductors that has now been extended to include a range of Sr-doping [2, 3], Pr or La in place of Nd [4-6], and the 5-layer Nd$_6$Ni$_5$O$_{12}$ [7]. A number of studies indicate that electron correlations are strong in these materials [8-14], and hence a central question is whether or not magnetism is present as a consequence of these interactions. Here we report muon spin rotation/relaxation studies of a series of superconducting infinite-layer nickelates. In all cases we observe an intrinsic magnetic ground state, regardless of the rare earth ion or doping, arising from local moments on the nickel sublattice. The coexistence of magnetism - which is likely to be antiferromagnetic and short-range ordered - with superconductivity is reminiscent of some iron pnictides [15] and heavy fermion compounds [16], and qualitatively distinct from the doped cuprates [17].

cond-mat.supr-con↗

arXiv2022

Reconstructing the polar interface of infinite-layer nickelate thin films

Nickel-based superconductors provide a long-awaited experimental platform to explore possible cuprate-like superconductivity. Despite similar crystal structure and $d$ electron filling, these systems exhibit several differences. Nickelates are the most polar layered oxide superconductor, raising questions about the interface between substrate and thin film -- thus far the only sample geometry to successfully stabilize superconductivity. We conduct a detailed experimental and theoretical study of the prototypical interface between Nd$_{1-x}$Sr$_x$NiO$_2$ and SrTiO$_3$. Atomic-resolution electron energy loss spectroscopy in the scanning transmission electron microscope reveals the formation of a single intermediate Nd(Ti,Ni)O$_3$ layer. Density functional theory calculations with a Hubbard $U$ term show how the observed structure alleviates the strong polar discontinuity. We explore effects of oxygen occupancy, hole doping, and cation structure to disentangle the contributions of each for reducing interface charge density. Resolving the nontrivial interface structure will be instructive for future synthesis of nickelate films on other substrates and in vertical heterostructures.

cond-mat.supr-con↗

arXiv2021

A Broken Translational Symmetry State in an Infinite-Layer Nickelate

A defining signature of strongly correlated electronic systems is the existence of competing phases with similar ground state energies, resulting in a rich phase diagram. While in the recently discovered nickelate superconductors, a high antiferromagnetic exchange energy has been reported, which implies the existence of strong electronic correlations, signatures of competing phases have not yet been observed. Here, we uncover a charge order (CO) in infinite-layer nickelates La1-xSrxNiO2 using resonant x-ray scattering across the Ni L-edge. In the parent compound, the CO arranges along the Ni-O bond direction with an incommensurate wave vector (0.344+/-0.002, 0) r.l.u., distinct from the stripe order in other nickelates which propagates along a direction 45 degree to the Ni-O bond. The CO resonance profile indicates that CO originates from the Ni 3d states and induces a parasitic charge modulation of La electrons. Upon doping, the CO diminishes and the ordering wave vector shifts toward a commensurate value of 1/3 r.l.u., indicating that the CO likely arises from strong correlation effects and not from Fermi surface nesting.

cond-mat.supr-con↗

arXiv2021

Insulator-to-Metal Crossover near the Edge of the Superconducting Dome in Nd$_{1-x}$Sr$_x$NiO$_2$

We report a systematic magnetotransport study of superconducting infinite-layer nickelate thin films Nd$_{1-x}$Sr$_x$NiO$_2$ with $0.15 \leq x \leq 0.225$. By suppressing superconductivity with out-of-plane magnetic fields up to 37.5 T, we find that the normal state resistivity of Nd$_{1-x}$Sr$_x$NiO$_2$ is characterized by a crossover from a metallic $T^2$-behavior to an insulating log(1/$T$)-behavior for all $x$ except $x = 0.225$, at which the resistivity is predominantly metallic. The log(1/$T$)-behavior is found to be robust against magnetic fields, inconsistent with scenarios involving localization or Kondo scattering, and points to an anomalous insulating state possibly driven by strong correlations. In the metallic state, we find no evidence for non-Fermi-liquid behavior arising from proximity to a putative quantum critical point located inside the superconducting dome.

cond-mat.supr-con↗

arXiv2021

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↗

arXiv2021

Low-density superconductivity in SrTiO$_3$ bounded by the adiabatic criterion

SrTiO$_3$ exhibits superconductivity for carrier densities $10^{19}-10^{21}$ cm$^{-3}$. Across this range, the Fermi level traverses a number of vibrational modes in the system, making it ideal for studying dilute superconductivity. We use high-resolution planar-tunneling spectroscopy to probe chemically-doped SrTiO$_3$ across the superconducting dome. The over-doped superconducting boundary aligns, with surprising precision, to the Fermi energy crossing the Debye energy. Superconductivity emerges with decreasing density, maintaining throughout the Bardeen-Cooper-Schrieffer (BCS) gap to transition-temperature ratio, despite being in the anti-adiabatic regime. At lowest superconducting densities, the lone remaining adiabatic phonon van Hove singularity is the soft transverse-optic mode, associated with the ferroelectric instability. We suggest a scenario for pairing mediated by this mode in the presence of spin-orbit coupling, which naturally accounts for the superconducting dome and BCS ratio.

cond-mat.supr-con↗