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Soonsang Huh

Publications and source records attributed to Soonsang Huh.

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BCS-BEC crossover driven by small Fermi pockets of a high-Tc cuprate superconductor

Fermi arcs observed in underdoped cuprates have sparked debate over whether they represent segments of a large Fermi surface or small Fermi pockets. This ambiguity has long hindered their classification as either the conventional Bardeen-Cooper-Schrieffer (BCS) regime or the strongly coupled Bose-Einstein condensation (BEC) crossover limit. Here, using angle-resolved photoemission spectroscopy and quantum oscillations, we demonstrate the coexistence of a small Fermi pocket and a large superconducting gap in the clean inner CuO2 layers of the four-layer cuprate Ba2Ca3Cu4O8(F,O)2. This coexistence constitutes a hallmark of the BCS-BEC crossover and has remained elusive for decades. Despite the presence of antiferromagnetic (AF) order, the superconducting gap in the small pocket is remarkably large, yielding a gap-to-Fermi-energy ratio (Delta_pocket/e_F ~ 0.6) and a critical-to-Fermi-temperature ratio (Tc/TF ~ 1.3) that reach the theoretical upper bound for two-dimensional superconductivity. Unexpectedly, this BCS-BEC crossover emerges not as the carrier density decreases but as it increases, abruptly within a narrow doping range of less than 1%. These results provide a long-sought microscopic foundation for the d-wave pairing mechanism in doped AF-Mott insulators.

cond-mat.supr-con

Superconducting coherence boosted by outer-layer metallic screening in multilayered cuprates

In multilayered high-Tc cuprates with three or more CuO2 layers per unit cell, the inner CuO2 planes (IPs) are spatially separated from the dopant layers and thus remain cleaner than the outer planes (OPs). While both interlayer coupling and the presence of clean IPs have been proposed as key factors enhancing superconductivity, their individual roles have been difficult to disentangle, as IPs and OPs typically become superconducting simultaneously. Here we investigate five-layer (Cu,C)Ba2Ca4Cu5Oy (Cu1245) with Tc = 78 K and three-layer Ba2Ca2Cu3O6(F,O)2 (F0223) with Tc = 100 K using ARPES, and uncover an unprecedented situation, in which only the IPs become superconducting while the OPs remain metallic at low temperatures. Model calculations indicate that more than 95% of the OP wavefunction remains confined to OP itself, with minimal hybridization from the superconducting IPs. In particular, we experimentally realize an ideal configuration: a single superconducting CuO2 layer sandwiched between heavily overdoped metallic outer layers, which screen disorder originating from the dopant layers. Strikingly, this clean CuO2 layer exhibits the largest superconducting gap among all known cuprates and coherent Bogoliubov peaks extending beyond the antiferromagnetic zone boundary -- long regarded as the boundary beyond which coherence vanishes in heavily underdoped cuprates. Furthermore, a widely extended coherent flat band emerges at the Brillouin zone edge, overcoming the pseudogap damping effect. Our results introduce a new physical parameter, the degree of screening, to investigate the competition between superconductivity and the pseudogap, potentially shedding new light on its origin. The nearly disorder-free superconducting CuO2 layers offer a model platform for bridging the gap between disordered real materials and idealized theoretical models, which generally neglect disorder effects.

cond-mat.supr-con

Coupling between electrons and charge density wave fluctuation and its possible role in superconductivity

In most of charge density wave (CDW) systems of different material classes, ranging from traditional correlated systems in low-dimension to recent topological systems with Kagome lattice, superconductivity emerges when the system is driven toward the quantum critical point (QCP) of CDW via external parameters of doping and pressure. Despite this rather universal trend, the essential hinge between CDW and superconductivity has not been established yet. Here, the evidence of coupling between electron and CDW fluctuation is reported, based on a temperature- and intercalation-dependent kink in the angle-resolved photoemission spectra of 2H-PdxTaSe2. Kinks are observed only when the system is in the CDW phase, regardless of whether a long- or short-range order is established. Notably, the coupling strength is enhanced upon long-range CDW suppression, albeit the coupling energy scale is reduced. Interestingly, estimation of the superconducting critical temperature by incorporating the observed coupling characteristics into McMillan's equation yields result closely resembling the known values of the superconducting dome. Our results thus highlight a compelling possibility that this new coupling mediates Cooper pairs, which provides new insights on the competing relationship not only for CDW, but also for other competing orders.

cond-mat.supr-con

Room temperature quantum emitters in van der Waals {\alpha}-MoO3

Quantum emitters in solid-state materials are highly promising building blocks for quantum information processing and communication science. Recently, single-photon emission from van der Waals materials has been reported in transition metal dichalcogenides and hexagonal boron nitride, exhibiting the potential to realize photonic quantum technologies in two-dimensional materials. Here, we report the generation of room temperature single-photon emission from exfoliated and thermally annealed single crystals of van der Waals {\alpha}-MoO3. The second-order correlation function measurement displays a clear photon antibunching, while the luminescence intensity exceeds 0.4 Mcts/s and remains stable under laser excitation. The theoretical calculation suggests that an oxygen vacancy defect is a possible candidate for the observed emitters. Together with photostability and brightness, quantum emitters in {\alpha}-MoO3 provide a new avenue to realize photon-based quantum information science in van der Waals materials.

cond-mat.mtrl-sci

Unveiling the charge density wave mechanism in vanadium-based Bi-layered kagome metals

The charge density wave (CDW), as a hallmark of vanadium-based kagome superconductor AV3Sb5 (A = K, Rb, Cs), has attracted intensive attention. However, the fundamental controversy regarding the underlying mechanism of CDW therein persists. Recently, the vanadium-based bi-layered kagome metal ScV6Sn6, reported to exhibit a long-range charge order below 94 K, has emerged as a promising candidate to further clarify this core issue. Here, employing micro-focusing angle-resolved photoemission spectroscopy ({\mu}-ARPES) and first-principles calculations, we systematically studied the unique CDW order in vanadium-based bi-layered kagome metals by comparing ScV6Sn6 with its isostructural counterpart YV6Sn6, which lacks a CDW ground state. Combining ARPES data and the corresponding joint density of states (DOS), we suggest that the VHS nesting mechanism might be invalid in these materials. Besides, in ScV6Sn6, we identified multiple hybridization energy gaps resulting from CDW-induced band folding, along with an anomalous band dispersion, implying a potential electron-phonon coupling driven mechanism underlying the formation of the CDW order. Our finding not only comprehensively maps the electronic structure of V-based bi-layer kagome metals but also provide constructive experimental evidence for the unique origin of CDW in this system.

cond-mat.mtrl-sci

Pseudogap and Fermi arc induced by Fermi surface nesting in a centrosymmetric skyrmion magnet

Skyrmions in noncentrosymmetric materials are believed to occur due to the Dzyaloshinskii-Moriya interaction. By contrast, the skyrmion formation mechanism in centrosymmetric materials remains elusive. Here, we reveal the intrinsic electronic structure of the centrosymmetric GdRu2Si2 by selectively measuring magnetic domains using angle-resolved photoemission spectroscopy (ARPES). We found robust Fermi surface (FS) nesting, consistent with the magnetic modulation q-vector detected by the previous resonant x-ray scattering measurements. The pseudogap opens at the nested FS portions, which vary for different magnetic domains. The anomalous pseudogap disconnects the FS to generate Fermi arcs with twofold symmetry. These results indicate that the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction plays a decisive role in generating the screw spin modulation responsible for the skyrmion formation in GdRu2Si2. Furthermore, we demonstrate the flexible nature of magnetism in GdRu2Si2 by manipulating magnetic domains with magnetic field and temperature cyclings, providing potential future applications for data storage and processing devices.

cond-mat.mtrl-sci

Direct observation of topological surface state in the topological superconductor 2M-WS2

The quantum spin Hall (QSH) effect has attracted extensive research interest because of the potential applications in spintronics and quantum computing, which is attributable to two conducting edge channels with opposite spin polarization and the quantized electronic conductance of 2e2/h. Recently, 2M-WS2, a new stable phase of transition metal dichalcogenides with a 2M structure showing an identical layer configuration to that of the monolayer 1T' TMDs, was suggested to be a QSH insulator as well as a superconductor with critical transition temperature around 8 K. Here, high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES are applied to investigate the electronic and spin structure of the topological surface states (TSS) in the superconducting 2M-WS2. The TSS exhibits characteristic spin-momentum-locking behavior, suggesting the existence of long-sought nontrivial Z2 topological states therein. We expect that 2M-WS2 with co-existing superconductivity and TSS might host the promising Majorana bound states.

cond-mat.supr-con

Quantum electron liquid and its possible phase transition

Purely quantum electron systems exhibit intriguing correlated electronic phases by virtue of quantum fluctuations in addition to electron-electron interactions. To realize such quantum electron systems, a key ingredient is dense electrons decoupled from other degrees of freedom. Here, we report the discovery of a pure quantum electron liquid, which spreads up to ~ 3 {\AA} in the vacuum on the surface of electride crystal. An extremely high electron density and its weak hybridisation with buried atomic orbitals evidence the quantum and pure nature of electrons, that exhibit a polarized liquid phase as demonstrated by our spin-dependent measurement. Further, upon enhancing the electron correlation strength, the dynamics of quantum electrons changes to that of non-Fermi liquid along with an anomalous band deformation, suggestive of a transition to a hexatic liquid crystal phase. Our findings cultivate the frontier of quantum electron systems, and serve as a platform for exploring correlated electronic phases in a pure fashion.

cond-mat.str-el

Kondo interaction in FeTe and its potential role in the magnetic order

Finding d-electron heavy fermion (HF) states has been an important topic as the diversity in d-electron materials can lead to many exotic Kondo effect-related phenomena or new states of matter such as correlation-driven topological Kondo insulator or cooperation between long-range magnetism and Kondo lattice behavior. Yet, obtaining direct spectroscopic evidence for a d-electron HF system has been elusive to date. Here, we report the observation of Kondo lattice behavior in an antiferromagnetic metal, FeTe, via angle-resolved photoemission spectroscopy (ARPES) and transport properties measurements. The Kondo lattice behavior is represented by the emergence of a sharp quasiparticle at low temperatures. The transport property measurements confirm the low-temperature Fermi liquid behavior and reveal successive coherent-incoherent crossover upon increasing temperature. We interpret the Kondo lattice behavior as a result of hybridization between localized Fe 3dxy and itinerant Te 5pz orbitals. Our interpretation is further evidenced by Fano-type tunneling spectra which accompany a hybridization gap. Our observations strongly suggest unusual cooperation between Kondo lattice behavior and long-range magnetic order.

cond-mat.str-el

Observation of spin-dependent dual ferromagnetism in perovskite ruthenates

We performed in-situ angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES (SARPES) experiments to investigate the relationship between electronic band structures and ferromagnetism in SrRuO$_3$ (SRO) thin films. Our high-quality ARPES and SARPES results show clear spin-lifted band structures. The spin polarization is strongly dependent on momentum around the Fermi level, whereas it becomes less dependent at high-binding energies. This experimental observation matches our dynamical mean-field theory (DMFT) results very well. As temperature increases from low to the Curie temperature, spin-splitting gap decreases and band dispersions become incoherent. Based on the ARPES study and theoretical calculation results, we found that SRO possesses spin-dependent electron correlations in which majority and minority spins are localized and itinerant, respectively. Our finding explains how ferromagnetism and electronic structure are connected, which has been under debate for decades in SRO.

cond-mat.str-el

Cu doping effects on the electronic structure of Fe1-xCuxSe

Using angle-resolved photoemission spectroscopy (ARPES), we studied the evolution of the electronic structure of Fe1-xCuxSe from x = 0 to 0.10. We found that the Cu dopant introduces extra electron carriers. The hole bands near the gamma point are observed to steadily shift downward with increasing doping and completely sink down below the Fermi level (EF) for x > 0.05. Meanwhile, the electron pocket near the M point becomes larger but loses the spectral weight near EF. We also observed that effective mass of the electron band near the M point increases with doping. Our result explains why superconductivity disappears and metal insulator transition (MIT) like behavior occurs upon Cu doping in terms of electronic structure, and provide insight into emergent magnetic fluctuation in Fe1-xCuxSe.

cond-mat.supr-con

Observation of metallic electronic structure in a single-atomic-layer oxide

Correlated electrons in transition metal oxides (TMOs) exhibit a variety of emergent phases. When TMOs are confined to a single-atomic-layer thickness, experiments so far have shown that they usually lose diverse properties and become insulators. In an attempt to extend the range of electronic phases of the single-atomic-layer oxide, we search for a metallic phase in a monolayer-thick epitaxial SrRuO$_3$ film. Combining atomic-scale epitaxy and angle-resolved photoemission measurements, we show that the monolayer SrRuO$_3$ is a strongly correlated metal. Systematic investigation reveals that the interplay between dimensionality and electronic correlation makes the monolayer SrRuO$_3$ an incoherent metal with orbital-selective correlation. Furthermore, the unique electronic phase of the monolayer SrRuO$_3$ is found to be highly tunable, as charge modulation demonstrates an incoherent-to-coherent crossover of the two-dimensional metal. Our work emphasizes the potentially rich phases of single-atomic-layer oxides and provides a guide to the manipulation of their two-dimensional correlated electron systems.

cond-mat.str-el

Deep learning-based statistical noise reduction for multidimensional spectral data

In spectroscopic experiments, data acquisition in multi-dimensional phase space may require long acquisition time, owing to the large phase space volume to be covered. In such case, the limited time available for data acquisition can be a serious constraint for experiments in which multidimensional spectral data are acquired. Here, taking angle-resolved photoemission spectroscopy (ARPES) as an example, we demonstrate a denoising method that utilizes deep learning as an intelligent way to overcome the constraint. With readily available ARPES data and random generation of training data set, we successfully trained the denoising neural network without overfitting. The denoising neural network can remove the noise in the data while preserving its intrinsic information. We show that the denoising neural network allows us to perform similar level of second-derivative and line shape analysis on data taken with two orders of magnitude less acquisition time. The importance of our method lies in its applicability to any multidimensional spectral data that are susceptible to statistical noise.

cs.LG

Effect of the sample work function on alkali metal dosing induced electronic structure change

Alkali metal dosing (AMD) has been widely used as a way to control doping without chemical substitution. This technique, in combination with angle resolved photoemission spectroscopy (ARPES), often provides an opportunity to observe unexpected phenomena. However, the amount of transferred charge and the corresponding change in the electronic structure vary significantly depending on the material. Here, we report study on the correlation between the sample work function and alkali metal induced electronic structure change for three iron-based superconductors: FeSe, Ba(Fe$_{0.94}$Co$_{0.06}$)$_{2}$As$_{2}$ and NaFeAs which share a similar Fermi surface topology. Electronic structure change upon monolayer of alkali metal dosing and the sample work function were measured by ARPES. Our results show that the degree of electronic structure change is proportional to the difference between the work function of the sample and Mulliken's absolute electronegativity of the dosed alkali metal. This finding provides a possible way to estimate the AMD induced electronic structure change.

cond-mat.str-el

Electronic band structure of (111) $SrRuO_{3}$ thin film$-$an angle-resolved photoemission spectroscopy study

We studied the electronic band structure of pulsed laser deposition (PLD) grown (111)-oriented SrRuO$_3$ (SRO) thin films using \textit{in situ} angle-resolved photoemission spectroscopy (ARPES) technique. We observed previously unreported, light bands with a renormalized quasiparticle effective mass of about 0.8$m_{e}$. The electron-phonon coupling underlying this mass renormalization yields a characteristic "kink" in the band dispersion. The self-energy analysis using the Einstein model suggests five optical phonon modes covering an energy range 44 to 90 meV contribute to the coupling. Besides, we show that the quasiparticle spectral intensity at the Fermi level is considerably suppressed, and two prominent peaks appear in the valance band spectrum at binding energies of 0.8 eV and 1.4 eV, respectively. We discuss the possible implications of these observations. Overall, our work demonstrates that high-quality thin films of oxides with large spin-orbit coupling can be grown along the polar (111) orientation by the PLD technique, enabling \textit{in situ} electronic band structure study. This could allow for characterizing the thickness-dependent evolution of band structure of (111) heterostructures$-$a prerequisite for exploring possible topological quantum states in the bilayer limit.

cond-mat.str-el

Electronic phase diagram of iron chalcogenide superconductors FeSe1-xSx and FeSe1-yTey

Here we establish a combined electronic phase diagram of isoelectronic FeSe1-xSx (0.19 > x > 0.0) and FeSe1-yTey (0.04 < y < 1.0) single crystals. The FeSe1-yTey crystals with y = 0.04 - 0.30 are grown by a hydrothermal ion-deintercalation (HID) method. Based on combined experiments of the specific heat, electrical transport, and angle-resolved photoemission spectroscopy, no signature of the tetragonal-symmetry-broken transition to orthorhombic (nematic) phase is observed in the HID FeSe1-yTey samples, as compared with the FeSe1-xSx samples showing this transition at Ts. A ubiquitous dip-like temperature dependence of the Hall coefficient is observed around a characteristic temperature T* in the tetragonal regimes, which is well above the superconducting transition. More importantly, we find that the superconducting transition temperature Tc is positively correlated with the Hall-dip temperature T* across the FeSe1-xSx and FeSe1-yTey systems, suggesting that the tetragonal background is a fundamental host for the superconductivity.

cond-mat.supr-con

Sign-tunable anomalous Hall effect induced by two-dimensional symmetry-protected nodal structures in ferromagnetic perovskite oxide thin films

Magnetism and spin-orbit coupling (SOC) are two quintessential ingredients underlying novel topological transport phenomena in itinerant ferromagnets. When spin-polarized bands support nodal points/lines with band degeneracy that can be lifted by SOC, the nodal structures become a source of Berry curvature; this leads to a large anomalous Hall effect (AHE). Contrary to three-dimensional systems that naturally host nodal points/lines, two-dimensional (2D) systems can possess stable nodal structures only when proper crystalline symmetry exists. Here we show that 2D spin-polarized band structures of perovskite oxides generally support symmetry-protected nodal lines and points that govern both the sign and the magnitude of the AHE. To demonstrate this, we performed angle-resolved photoemission studies of ultrathin films of SrRuO$_3$, a representative metallic ferromagnet with SOC. We show that the sign-changing AHE upon variation in the film thickness, magnetization, and chemical potential can be well explained by theoretical models. Our study is the first to directly characterize the topological band structure of 2D spin-polarized bands and the corresponding AHE, which could facilitate new switchable devices based on ferromagnetic ultrathin films.

cond-mat.str-el

Lifted electron pocket and reversed orbital occupancy imbalance in FeSe

The FeSe nematic phase has been the focus of recent research on iron based superconductors (IBSs) due to its unique properties. A number of electronic structure studies were performed to find the origin of the phase. However, such attempts came out with conflicting results and caused additional controversies. Here, we report results from angle resolved photoemission and X-ray absorption spectroscopy studies on FeSe with detwinning by a piezo stack. We have fully resolved band dispersions with orbital characters near the Brillouin zone corner which reveals absence of a Fermi pocket at the Y point in the 1Fe Brillouin zone. In addition, the occupation imbalance between dxz and dyz orbitals is found to be opposite to that of iron pnictides, which is consistent with the identified band characters. These results settle down controversial issues in the FeSe nematic phase and shed light on the origin of nematic phases in IBSs.

cond-mat.supr-con