SearcharxivSearch

arXiv subjects

Cheng-Tai Kuo

Publications and source records attributed to Cheng-Tai Kuo.

17 recordsLinked to original sources

Low-Temperature Suppression of Intertwined Orders in La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ Thin Films

The strong coupling between spin, charge, and lattice degrees of freedom in perovskite oxides leads to an array of exotic phenomena, giving these materials rich phase diagrams that can include coupled orders. This is exemplified by the A-site doped ferrite La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ (LSFO), which exhibits a coupled paramagnetic-antiferromagnetic and charge ordering phase transition at $\sim$190 K that has been well studied in thin films, bulk, and polycrystalline samples. However, the low temperature behavior of LSFO thin films below $\sim$100 K has not been thoroughly explored. This work uses several X-ray scattering and spectroscopy techniques to directly probe LSFO's magnetic and charge order down to low temperature. Using resonant X-ray scattering, we observe a complete suppression of LSFO's known antiferromagnetic and charge order below $\sim$25 K. Further spectroscopy and coherent scattering measurements provide insight into LSFO's electronic structure and domain dynamics in this new low temperature phase, and we propose possible explanations for the observed order suppression based on reduced dimensionality of domains in our thin films. Our findings provide insight into the effects of competing interactions in strongly correlated materials, particularly those with coupled orders.

cond-mat.str-el

Interlayer Five-Spin Polaron in Superconducting Bilayer Nickelates

The discovery of high-$T_c$ superconductivity in Ruddlesden-Popper nickelates has sparked substantial effort towards understanding unconventional electronic states beyond a traditional cuprate-like $d^9$ configurational ground state. An understanding of the interplay between magnetic ground states and multi-orbital physics is key for establishing a microscopic mechanism for superconductivity. In the bilayer nickelates, spin density wave (SDW) order is a prominent feature in the non-superconducting regime, yet its relation to superconducting pairing remains an open question. Here, we use resonant x-ray scattering to examine the existence of SDW order in superconducting bilayer nickelate thin films La$_2$PrNi$_2$O$_7$ (LPNO). Comparing superconducting and oxygen-deficient LPNO thin films, we find that superconductivity occurs in SDW-free, oxygen-stoichiometric regions, whereas oxygen-deficiency promotes SDW order, indicating phase segregation of SDW and superconductivity. Furthermore, Ni-$L_3$ and O-$K$ edge spectroscopy reveals distinct electronic structures - particularly along the $c$-axis - between the two regions. Our results identify oxygen stoichiometry as a key parameter controlling interlayer coupling and thus the electronic structure of bilayer nickelates. In concert with theory, we propose that a ligand hole primarily resides at the inter-bilayer apical oxygen, forming a robust interlayer five-spin polaron state, which serves as the ground state for superconducting bilayer nickelates.

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

Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet

Disorder in magnetic systems typically suppresses long-range order, promoting short-range states such as spin glasses and magnetic clusters. This is particularly prominent in high-entropy materials, characterized by the random distributions of local magnetic entities and exchange interactions. However, in rare exceptions, long-range magnetic order can persist in high-entropy systems, while the microscopic characters and underlying mechanisms remain elusive, especially the magnetic behaviors of individual elements. Here, combining neutron diffraction and resonant soft x-ray scattering, we have conducted an element-specific investigation into the magnetic order of a high-entropy honeycomb-lattice van der Waals material (Mn1/4Fe1/4Co1/4Ni1/4)PS3. Despite significant atomic disorder, long-range zigzag antiferromagnetic order is observed below 72 K, with all four transition-metal elements participating in a unified phase transition. However, the spin orientations of various elements are distinct, attributed to the competition between single-ion anisotropies and exchange interactions. Our findings showcase a novel form of long-range magnetic order with disordered spin orientations, which is synergically stabilized by distinct magnetic elements in a high entropy magnet, offering a new paradigm for understanding complex magnetic systems.

cond-mat.str-el

Probing Coordination Environments in Buried Oxides of Aluminum Josephson Junctions by Resonant X-ray Reflectivity

Decoherence remains a critical obstacle to achieving high-fidelity, scalable superconducting qubits, with the tunnel barrier of Josephson junctions a key source of loss. Here we apply resonant X-ray reflectivity to non-destructively probe the electronic structure of buried layers in Al/AlO$_x$/Al Josephson junctions. At the Al $K$-edge, energy-dependent modulations in the reflectivity maps enable Kramers-Kronig-constrained extraction of the layer-resolved atomic scattering factors. The analysis reveals that the barrier coordination evolves from more tetrahedral toward predominantly octahedral character with increasing oxidation pressure. At the interfaces, the lower metal-oxide boundary is comparatively under-coordinated and disordered relative to the upper interface. Comparison with simulated X-ray absorption spectra identifies the dominant coordination motifs within the oxide and its interfaces, providing depth-resolved structural insight that constrains microscopic models of two-level system formation. These results link growth conditions, local coordination environments, and junction electronic properties, demonstrating resonant X-ray reflectivity as a powerful tool for probing the microscopic materials properties of Josephson junctions and providing a materials-level framework for mitigating decoherence in superconducting qubits.

cond-mat.mtrl-sci

Introducing new resonant soft x-ray scattering capability in SSRL

Resonant soft X-ray scattering (RSXS) is a powerful technique for probing both spatial and electronic structures within solid-state systems. We present a newly developed RSXS capability at beamline 13-3 of the Stanford Synchrotron Radiation Lightsource (SSRL), designed to enhance materials science research. This advanced setup achieves a base sample temperature as low as 9.8 K combined with extensive angular motions (azimuthal \phi and flipping \chi), enabling comprehensive exploration of reciprocal space. Two types of detectors, an Au/GaAsP Schottky photodiode and a CCD detector with over 95% quantum efficiency, are integrated to effectively capture scattered photons. Extensive testing has confirmed the enhanced functionality of this RSXS setup, including its temperature and angular performance. The versatility and effectiveness of the system have been demonstrated through studies of various materials, including superlattice heterostructures and high-temperature superconductors.

physics.ins-det

Observation of Subharmonic Charge-Density-Wave Correlations in La-Based Cuprates

Pair-density-wave (PDW) correlations have been proposed as an important ingredient in the complex phase diagram of high-$T_{\rm c}$ cuprates, yet bulk-sensitive experimental signatures remain scarce. Here we report resonant x-ray scattering measurements revealing a subharmonic charge-density-wave (CDW) scattering response in Sr-doped $1/8$-LBCO. The subharmonic response appears at approximately half the primary CDW ordering wave vector and emerges within a physically relevant temperature regime associated with the development of in-plane superconducting correlations. Comparable subharmonic behavior is also observed in a chemically distinct La-based cuprate, LSCO, within the same stripe-ordered, layer-decoupled regime. Together, these observations identify a bulk-sensitive scattering signature that is consistent with PDW correlations in La-based superconducting cuprates.

cond-mat.supr-con

Orientation Controlled Anisotropy in Single Crystals of Quasi-1D BaTiS3

Low-dimensional materials with chain-like (one-dimensional) or layered (twodimensional) structures are of significant interest due to their anisotropic electrical, optical, thermal properties. One material with chain-like structure, BaTiS3 (BTS), was recently shown to possess giant in-plane optical anisotropy and glass-like thermal conductivity. To understand the origin of these effects, it is necessary to fully characterize the optical, thermal, and electronic anisotropy of BTS. To this end, BTS crystals with different orientations (aand c-axis orientations) were grown by chemical vapor transport. X-ray absorption spectroscopy (XAS) was used to characterize the local structure and electronic anisotropy of BTS. Fourier transform infrared (FTIR) reflection/transmission spectra show a large inplane optical anisotropy in the a-oriented crystals, while the c-axis oriented crystals were nearly isotropic in-plane. BTS platelet crystals are promising uniaxial materials for IR optics with their optic axis parallel to the c-axis. The thermal conductivity measurements revealed a thermal anisotropy of ~4.5 between the c- and a-axis. Time-domain Brillouin scattering showed that the longitudinal sound speed along the two axes is nearly the same suggesting that the thermal anisotropy is a result of different phonon scattering rates.

cond-mat.mtrl-sci

Orbital contributions in the element-resolved valence electronic structure of Bi2Se3

In this work, we studied the bulk band structure of a topological insulator (TI) Bi2Se3 and determined the contributions of the Bi and Se orbital states to the valence bands using standing wave-excited hard x-ray photoemission spectroscopy (SW-HAXPES). This SW technique can provide the element-resolved information and extract individual Bi and Se contributions to the Bi2Se3 valence band. Comparisons with density functional theory (DFT) calculations (LDA and GW) reveal that the Bi 6s, Bi 6p, and Se 4p states are dominant in the Bi2Se3 HAXPES valence band. These findings pave a way for studying the element-resolved band structure and orbital contributions of this class of TIs.

cond-mat.mtrl-sci

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

Probing the polar-nonpolar oxide interfaces using resonant x-ray standing wave techniques

Transition metal (TM) oxide heterostructure superlattices have attracted great attention in research communities because of their emergent interfacial phenomena that do not exist in the bulk form. In order to understand the mechanisms that cause these phenomena, it is important to use depth-resolved spectroscopies to study the electronic structure across the buried oxide interfaces. In this review, we focus on the recent applications of standing wave (SW) photoemission (SW-XPS) and resonant inelastic x-ray scattering (SW-RIXS) spectroscopy to study the depth profiles of electronic structure or carriers around the polar-nonpolar oxide interfaces. Using the incident photon energies near the TM x-ray absorption resonance, the created SW excitation can enhance the spectral response and certain electronic transitions, providing important insight into the interfacial electronic structure in the energy and real space regimes. Following the background introductions, we describe two SW experiments and demonstrate that the combination of SW-XPS and SW-RIXS has the potential to obtain the depth distribution of electronic/orbital states around the buried interfaces with Angstrom precision.

cond-mat.mtrl-sci

High resolution depth profiling using near-total-reflection hard X-ray photoelectron spectroscopy

By adjusting the incidence angle of incoming X-ray near the critical angle of X-ray total reflection, the photoelectron intensity is strongly modulated due to the variation of X-ray penetration depth. Photoelectron spectroscopy (PES) combining with near total reflection (NTR) exhibit tunable surface sensitivity, providing depth-resolved information. In this review article, we first describe the experimental setup and specific data analysis process. We then review three different examples which show the broad application of this method. The emphasis is on its applications to correlated oxide heterostructures, especially quantitative depth analyses of compositions and electronic states. In a last part, we discussed the limitations of this technique, mostly in terms of range of samples which can be studied.

cond-mat.mtrl-sci

Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects

The discovery of a two-dimensional electron system (2DES) at the interfaces of perovskite oxides such as LaAlO3 and SrTiO3 has motivated enormous efforts in engineering interfacial functionalities with this type of oxide heterostructures. However, its fundamental origins are still not understood, e.g. the microscopic mechanisms of coexisting interface conductivity and magnetism. Here we report a comprehensive spectroscopic investigation of the depth profile of 2DES-relevant Ti 3d interface carriers using depth- and element-specific techniques, standing-wave excited photoemission and resonant inelastic scattering. We found that one type of Ti 3d interface carriers, which give rise to the 2DES are located within 3 unit cells from the n-type interface in the SrTiO3 layer. Unexpectedly, another type of interface carriers, which are polarity-induced Ti-on-Al antisite defects, reside in the first 3 unit cells of the opposing LaAlO3 layer (~10 Å). Our findings provide a microscopic picture of how the localized and mobile Ti 3d interface carriers distribute across the interface and suggest that the 2DES and 2D magnetism at the LaAlO3/SrTiO3 interface have disparate explanations as originating from different types of interface carriers.

cond-mat.mtrl-sci

Depth-resolved resonant inelastic x-ray scattering at a superconductor/half-metallic ferromagnet interface through standing-wave excitation

We demonstrate that combining standing-wave (SW) excitation with resonant inelastic x-ray scattering (RIXS) can lead to depth resolution and interface sensitivity for studying orbital and magnetic excitations in correlated oxide heterostructures. SW-RIXS has been applied to multilayer heterostructures consisting of a superconductor La$_{1.85}$Sr$_{0.15}$CuO$_{4}$(LSCO) and a half-metallic ferromagnet La$_{0.67}$Sr$_{0.33}$MnO$_{3}$ (LSMO). Easily observable SW effects on the RIXS excitations were found in these LSCO/LSMO multilayers. In addition, we observe different depth distribution of the RIXS excitations. The magnetic excitations are found to arise from the LSCO/LSMO interfaces, and there is also a suggestion that one of the dd excitations comes from the interfaces. SW-RIXS measurements of correlated-oxide and other multilayer heterostructures should provide unique layer-resolved insights concerning their orbital and magnetic excitations, as well as a challenge for RIXS theory to specifically deal with interface effects.

cond-mat.mtrl-sci

Atomic-layer-resolved composition and electronic structure of the cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ from soft x-ray standing-wave photoemission

A major remaining challenge in the superconducting cuprates is the unambiguous differentiation of the composition and electronic structure of the CuO$_2$ layers and those of the intermediate layers. The large c axis for these materials permits employing soft x-ray (930.3 eV) standing wave (SW) excitation in photoemission that yields atomic layer-by-atomic layer depth resolution of these properties. Applying SW photoemission to Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ yields the depth distribution of atomic composition and the layer-resolved densities of states. We detect significant Ca presence in the SrO layers and oxygen bonding to three different cations. The layer-resolved valence electronic structure is found to be strongly influenced by the supermodulation structure--as determined by comparison to DFT calculations, by Ca-Sr intermixing, and by the Cu 3d-3d Coulomb interaction, further clarifying the complex interactions in this prototypical cuprate. Measurements of this type for other quasi-two-dimensional materials with large-c represent a promising future direction.

cond-mat.supr-con

Element- and momentum-resolved electronic structure of the dilute magnetic semiconductor manganese doped gallium arsenide

The dilute magnetic semiconductors have promise in spin-based electronics applications due to their potential for ferromagnetic order at room temperature, and various unique switching and spin-dependent conductivity properties. However, the precise mechanism by which the transition-metal doping produces ferromagnetism has been controversial. Here we have studied a dilute magnetic semiconductor (5% manganese-doped gallium arsenide) with Bragg-reflection standing-wave hard X-ray angle-resolved photoemission spectroscopy, and resolved its electronic structure into element- and momentum- resolved components. The measured valence band intensities have been projected into element-resolved components using analogous energy scans of Ga 3d, Mn 2p, and As 3d core levels, with results in excellent agreement with element-projected Bloch spectral functions and clarification of the electronic structure of this prototypical material. This technique should be broadly applicable to other multi-element materials.

cond-mat.mtrl-sci

Interface properties and built-in potential profile of a LaCrO$_3$/SrTiO$_3$ superlattice determined by standing-wave excited photoemission spectroscopy

LaCrO$_3$ (LCO) / SrTiO$_3$ (STO) heterojunctions are intriguing due to a polar discontinuity along (001), two distinct and controllable interface structures [(LaO)$^+$/(TiO$_2$)$^0$ and (SrO)$^0$/(CrO$_2$)$^-$], and interface-induced polarization. In this study, we have used soft- and hard x-ray standing-wave excited photoemission spectroscopy (SW-XPS) to generate a quantitative determination of the elemental depth profiles and interface properties, band alignments, and the depth distribution of the interface-induced built-in potentials in the two constituent oxides. We observe an alternating charged interface configuration: a positively charged (LaO)$^+$/(TiO$_2$)$^0$ intermediate layer at the LCO$_\textbf{top}$/STO$_\textbf{bottom}$ interface and a negatively charged (SrO)$^0$/(CrO$_2$)$^-$ intermediate layer at the STO$_\textbf{top}$/LCO$_\textbf{bottom}$ interface. Using core-level SW data, we have determined the depth distribution of species, including through the interfaces, and these results are in excellent agreement with scanning transmission electron microscopy and electron energy loss spectroscopy (STEM-EELS) mapping of local structure and composition. SW-XPS also enabled deconvolution of the LCO-contributed and STO- contributed matrix-element-weighted density of states (MEWDOSs) from the valence band (VB) spectra for the LCO/STO superlattice (SL). Monitoring the VB edges of the deconvoluted MEWDOS shifts with a change in probing profile, the alternating charge- induced built-in potentials are observed in both constituent oxides. Finally, using a two-step simulation approach involving first core-level binding energy shifts and then valence-band modeling, the built-in potential gradients across the SL are resolved in detail and represented by the depth distribution of VB edges.

cond-mat.mtrl-sci