arXiv subjects

Yonghun Lee

Publications and source records attributed to Yonghun Lee.

At least 19 recordsLinked to original sources

arXiv2026

High-temperature superconductivity in Nd$_{0.85}$Sr$_{0.15}$NiO$_2$ membranes under pressure

Lattice compression has emerged as a fundamental tuning parameter for nickelate superconductivity. Pressure acts as a trigger to induce superconductivity in bulk Ruddlesden-Popper nickelates. For infinite-layer nickelate thin films, compressive epitaxial strain and rare-earth ion chemical pressure have been used to substantially enhance the superconducting transition temperature ($T_c$). Efforts to go further have been constrained by the limits of epitaxial stability or the challenges of measuring thin films in high-pressure environments. Here, we overcome this limitation by developing a technique to incorporate freestanding infinite-layer $\mathrm{Nd_{0.85}Sr_{0.15}NiO_2}$ membranes into a diamond anvil cell. Using this platform, we observe a strong increase in $T_c$ up to our highest measurement pressure of $\sim$90 GPa, where a superconducting downturn can be observed near liquid nitrogen temperatures. Strikingly, we find a simple linear enhancement of $T_c$ at a rate of 0.65 K GPa$^{-1}$, with no signs of saturation. This suggests that the pairing strength in infinite-layer nickelates can be raised to a surprisingly high scale, using an approach that can be broadly applied to many two-dimensional materials.

cond-mat.supr-con↗

arXiv2026

Machine Learning Reconstruction of High-Dimensional Electronic Structure from Angle-Resolved Photoemission Spectroscopy

The emergent behavior of quantum materials is governed by their electronic structure, which can be experimentally probed by photoemission spectroscopy techniques that generate a four-dimensional dataset of energy and momentum. However, the quantitative extraction of Hamiltonian parameters from these high-dimensional spectra remains a significant challenge, currently relying on labor-intensive, expert-dependent analysis rather than standardized workflows. Here, we introduce a deep learning framework based on implicit neural representations to accelerate the retrieval of Hamiltonian parameters in two types of transition-metal oxides: perovskite nickelates and manganites. Our approach outperforms traditional analytical fitting procedures, yielding superior agreement with experimental Fermi surface topologies and energy-momentum dispersions. This work highlights the potential of deep learning tools to bridge the gap between theory and experiment, paving the way for high-throughput, autonomous discovery pipelines in quantum materials.

cond-mat.str-el↗

arXiv2026

Evolution of the Superfluid Density in Infinite-Layer Nickelates

Nickelate superconductors provide a valuable new platform for the study of unconventional superconductivity that is complementary to the cuprates. One of the central puzzles about high-temperature superconductors is what factors determine the scale of their superconducting transition temperature ($T_\mathrm{c}$). To address this question for infinite-layer nickelates, we present a systematic mutual inductance study of the superfluid density across the doping-dependent superconducting dome of $\mathrm{Nd}_{1-x}\mathrm{Sr}_x\mathrm{NiO}_2$. We observe a weak superfluid stiffness that exhibits an approximately square-root correlation with $T_\mathrm{c}$. We also find a strong interplay between Nd magnetism and the superconducting phase, manifested as a substantial low-temperature suppression of superfluid density. These observations highlight the importance of superconducting phase fluctuations in limiting $T_\mathrm{c}$ and unexpectedly strong coupling between the Nd 4$f$ moments and the superfluid.

cond-mat.supr-con↗

arXiv2026

Optical conductivity signatures of strong correlations and multiband superconductivity in infinite-layer nickelates

Since the discovery of superconductivity in infinite-layer nickelates, there have been extensive efforts to unravel their electronic structure and pairing mechanism. In particular, understanding how the electronic structure evolves with doping is essential for clarifying theoretical models of superconductivity in nickelates. Here we present studies of the optical conductivity of Nd1-xSrxNiO2 thin films spanning the full phase diagram 0.025 < x < 0.30 using spectroscopic ellipsometry. The data are consistent with a two-band Drude model, which allows the decomposition of the intraband response into distinct contributions. One is from a "narrow" Drude term which we associate with electron bands, and the other a "broad" Drude term linked to the hole band with strong correlations. Increasing Sr doping leads to an expansion of the hole band spectral weight, and a corresponding reduction in the electron band, indicative of the multiband electronic structure and a doping-dependent reconstruction of the Fermi surface. Both doping and temperature-dependent optical spectra display significant spectral weight transfer from high to low energy, a hallmark of strong electronic correlations. In the superconducting state at optimal doping (x = 0.15), both electron and hole bands contribute to the superconducting condensate, signifying multiband superconductivity.

cond-mat.supr-con↗

arXiv2025

Mind the Gap -- Imaging Buried Interfaces in Twisted Oxide Moir\'es

The ability to tune electronic structure in twisted stacks of two-dimensional (2D) materials has motivated the exploration of similar moir\'e physics with twisted oxide membranes. Due to the intrinsic three-dimensional nature of bonding in many oxides, achieving atomic-level coupling is significantly more challenging than with van der Waals materials. Although clean interfaces with atomic-level proximity have been demonstrated in ceramic bicrystals using high-temperature and high-pressure processing to facilitate atomic diffusion that flattens rough interfaces, such conditions are not readily accessible when bonding oxide membranes. This study shows how topographic mismatch due to surface roughness of the membranes can restrict atomic-scale proximity at the interface to isolated patches even after contaminants and amorphous interlayers are eliminated. In interfaces between 2D materials and oxide membranes the reduced ability of the 2D material to conform to the membrane's step-terrace topography also limits atomic-scale contact. When imaging stacked membranes in projection, we find conventional through-focal imaging to be relatively insensitive to the buried interface, whereas electron ptychography detects structural variations on the order of a nanometer. These findings highlight interface roughness as a key challenge for the field of oxide twistronics and emphasize the need for reliable characterization methods, both in cross-section and projection.

cond-mat.mtrl-sci↗

arXiv2025

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↗

arXiv2025

The Classical-to-Quantum Crossover in strain-induced ferroelectric transition in SrTiO$_3$ membranes

Mechanical strain presents an effective control over symmetry-breaking phase transitions. In quantum paralelectric SrTiO3, strain can induce the ferroelectric transition via modification of local Ti potential landscape. However, brittle bulk materials can only withstand limited strain range (~0.1%). Taking advantage of nanoscopically-thin freestanding membranes, we demonstrated in-situ strain-induced reversible ferroelectric transition in a single freestanding SrTiO3 membranes. We measure the ferroelectric order by detecting the local anisotropy of the Ti 3d orbital using X-ray linear dichroism at the Ti-K pre-edge, while the strain is determined by X-ray diffraction. With reduced thickness, the SrTiO3 membranes remain elastic with >1% tensile strain cycles. A robust displacive ferroelectricity appears beyond a temperature-dependent critical strain. Interestingly, we discover a crossover from a classical ferroelectric transition to a quantum regime at low temperatures, which enhances strain-induced ferroelectricity. Our results offer a new opportunities to strain engineer functional properties in low dimensional quantum materials and provide new insights into the role of the ferroelectric fluctuations in quantum paraelectric SrTiO3.

cond-mat.mtrl-sci↗

arXiv2024

Electronically Amplified Electron-Phonon Interaction and Metal-Insulator Transition in Perovskite Nickelates

The relative role of electron-electron and electron-lattice interactions in driving the metal-insulator transition in perovskite nickelates opens a rare window into the non-trivial interplay of the two important degrees of freedom in solids. The most promising solution is to extract the electronic and lattice contributions during the phase transition by performing high-resolution spectroscopy measurements. Here, we present a three-dimensional electronic structure study of Nd1-xSrxNiO3 (x = 0 and 0.175) thin films with unprecedented accuracy, in which the low energy fermiology has a quantitative agreement with model simulations and first-principles calculations. Two characteristic phonons, the octahedral rotational and breathing modes, are illustrated to be coupled with the electron dynamics in the metallic phase, showing a kink structure along the band dispersion, as well as a hump feature in the energy spectrum. Entering the insulating state, the electron-phonon interaction is amplified by strong electron correlations, transforming the mobile large polarons at high temperatures to localized small polarons in the ground state. Moreover, the analysis of quasiparticle residue enables us to establish a transport-spectroscopy correspondence in Nd1-xSrxNiO3 thin films. Our findings demonstrate the essential role of electron-lattice interaction enhanced by the electronic correlation to stabilize the insulating phase in the perovskite nickelates.

cond-mat.str-el↗

arXiv2024

Highly confined epsilon-near-zero- and surface-phonon polaritons in SrTiO3 membranes

Recent theoretical studies have suggested that transition metal perovskite oxide membranes can enable surface phonon polaritons in the infrared range with low loss and much stronger subwavelength confinement than bulk crystals. Such modes, however, have not been experimentally observed so far. Here, using a combination of far-field Fourier-transform infrared (FTIR) spectroscopy and near-field synchrotron infrared nanospectroscopy (SINS) imaging, we study the phonon-polaritons in a 100 nm thick freestanding crystalline membrane of SrTiO3 transferred on metallic and dielectric substrates. We observe a symmetric-antisymmetric mode splitting giving rise to epsilon-near-zero and Berreman modes as well as highly confined (by a factor of 10) propagating phonon polaritons, both of which result from the deep-subwavelength thickness of the membranes. Theoretical modeling based on the analytical finite-dipole model and numerical finite-difference methods fully corroborate the experimental results. Our work reveals the potential of oxide membranes as a promising platform for infrared photonics and polaritonics.

cond-mat.mtrl-sci↗

arXiv2024

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↗

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$\Delta/k_\mathrm{B}T_\mathrm{c}$ 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

Low temperature dynamic polaron liquid in a manganite exhibiting colossal magnetoresistance

Polarons - fermionic charge carriers bearing a strong companion lattice deformation - exhibit a natural tendency for self-localization due to the recursive interaction between electrons and the lattice. While polarons are ubiquitous in insulators, how they evolve in transitions to metallic and superconducting states in quantum materials remains an open question. Here, we use resonant inelastic x-ray scattering (RIXS) to track the electron-lattice coupling in the colossal magneto-resistive bi-layer manganite La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ across its metal-to-insulator transition. The response in the insulating high-temperature state features harmonic emissions of a dispersionless oxygen phonon at small energy transfer. Upon cooling into the metallic state, we observe a drastic redistribution of spectral weight from the region of these harmonic emissions to a broad high energy continuum. In concert with theoretical calculations, we show that this evolution implies a shift in electron-lattice coupling from static to dynamic lattice distortions that leads to a distinct polaronic ground state in the low temperature metallic phase - a dynamic polaron liquid.

cond-mat.str-el↗

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

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↗

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

A flat band-induced correlated kagome metal

The notion of an electronic flat band refers to a collectively degenerate set of quantum mechanical eigenstates in periodic solids. The vanishing kinetic energy of flat bands relative to the electron-electron interaction is expected to result in a variety of many-body quantum phases of matter. Despite intense theoretical interest, systematic design and experimental realization of such flat band-driven correlated states in natural crystals have remained a challenge. Here we report the realization of a partially filled flat band in a new single crystalline kagome metal Ni$_3$In. This flat band is found to arise from the Ni $3d$-orbital wave functions localized at triangular motifs within the kagome lattice plane, where an underlying destructive interference among hopping paths flattens the dispersion. We observe unusual metallic and thermodynamic responses suggestive of the presence of local fluctuating magnetic moments originating from the flat band states, which together with non-Fermi liquid behavior indicate proximity to quantum criticality. These results demonstrate a lattice and orbital engineering approach to designing flat band-based many-body phenomena that may be applied to integrate correlation with topology and as a novel means to construct quantum criticality.

cond-mat.mtrl-sci↗