Showing papers by "Tae Won Noh published in 2021"

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

Abstract: Magnetism and spin–orbit coupling are two quintessential ingredients underlying topological transport phenomena in itinerant ferromagnets. When spin-polarized bands support nodal points/lines with band degeneracy that can be lifted by spin–orbit coupling, the nodal structures become a source of Berry curvature, leading to a large anomalous Hall effect. However, two-dimensional systems can possess stable nodal structures only when proper crystalline symmetry exists. Here we show that two-dimensional 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 anomalous Hall effect. To demonstrate this, we performed angle-resolved photoemission studies of ultrathin films of SrRuO3, a representative metallic ferromagnet with spin–orbit coupling. We show that the sign-changing anomalous Hall effect upon variation in the film thickness, magnetization and chemical potential can be well explained by theoretical models. Our work may facilitate new switchable devices based on ferromagnetic ultrathin films. The topological nature of the electronic structure of two-dimensional ferromagnetic SrRuO3 and its relationship to the anomalous Hall effect is explored through transport measurements, angle-resolved photoemission spectroscopy and theoretical modelling.

Oxygen vacancy-induced topological nanodomains in ultrathin ferroelectric films

Abstract: Oxygen vacancy in oxide ferroelectrics can be strongly coupled to the polar order via local strain and electric fields, thus holding the capability of producing and stabilizing exotic polarization patterns. However, despite intense theoretical studies, an explicit microscopic picture to correlate the polarization pattern and the distribution of oxygen vacancies remains absent in experiments. Here we show that in a high-quality, uniaxial ferroelectric system, i.e., compressively strained BaTiO3 ultrathin films (below 10 nm), nanoscale polarization structures can be created by intentionally introducing oxygen vacancies in the film while maintaining structure integrity (namely no extended lattice defects). Using scanning transmission electron microscopy, we reveal that the nanodomain is composed of swirling electric dipoles in the vicinity of clustered oxygen vacancies. This finding opens a new path toward the creation and understanding of the long-sought topological polar objects such as vortices and skyrmions.

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

Abstract: Correlated electrons in transition metal oxides exhibit a variety of emergent phases. When transition metal oxides 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 SrRuO3 film. Combining atomic-scale epitaxy and angle-resolved photoemission measurements, we show that the monolayer SrRuO3 is a strongly correlated metal. Systematic investigation reveals that the interplay between dimensionality and electronic correlation makes the monolayer SrRuO3 an incoherent metal with orbital-selective correlation. Furthermore, the unique electronic phase of the monolayer SrRuO3 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. Transition metal oxides exhibit a variety of correlated phases in their bulk form; however, they typically become insulators in the monolayer limit. Here, the authors report a correlated metallic state in a single-atomic layer of epitaxial SrRuO3, realized in epitaxial oxide heterostructure.

Correlated Magnetic Weyl Semimetal State in Strained Pr 2 Ir 2 O 7 .

Abstract: Correlated topological phases (CTPs) with interplay between topology and electronic correlations have attracted tremendous interest in condensed matter physics. Therein, correlated Weyl semimetals (WSMs) are rare in nature and, thus, have so far been less investigated experimentally. In particular, the experimental realization of the interacting WSM state with logarithmic Fermi velocity renormalization has not been achieved yet. Here, experimental evidence of a correlated magnetic WSM state with logarithmic renormalization in strained pyrochlore iridate Pr2 Ir2 O7 (PIO) which is a paramagnetic Luttinger semimetal in bulk, is reported. Benefitting from epitaxial strain, "bulk-absent" all-in-all-out antiferromagnetic ordering can be stabilized in PIO film, which breaks time-reversal symmetry and leads to a magnetic WSM state. With further analysis of the experimental data and renormalization group calculations, an interacting Weyl liquid state with logarithmically renormalized Fermi velocity, similar to that in graphene, is found, dressed by long-range Coulomb interactions. This work highlights the interplay of strain, magnetism, and topology with electronic correlations, and paves the way for strain-engineering of CTPs in pyrochlore iridates.

Bulk Metamaterials Exhibiting Chemically Tunable Hyperbolic Responses.

Abstract: Extraordinary properties of traditional hyperbolic metamaterials, not found in nature, arise from their man-made subwavelength structures causing unique light-matter interactions. However, their preparation requiring nanofabrication processes is highly challenging and merely provides nanoscale two-dimensional structures. Stabilizing their bulk forms via scalable procedures has been a sought-goal for broad applications of this technology. Herein, we report a new strategy of designing and realizing bulk metamaterials with finely tunable hyperbolic responses. We develop a facile two-step process: (1) self-assembly to obtain heterostructured nanohybrids of building blocks and (2) consolidation to convert nanohybrid powders to dense bulk pellets. Our samples have centimeter-scale dimensions typically, readily further scalable. Importantly, the thickness of building blocks and their relative concentration in bulk materials serve as a delicate means of controlling hyperbolic responses. The resulting new bulk heterostructured material system consists of the alternating h-BN and graphite/graphene nanolayers and exhibits significant modulation in both type-I and type-II hyperbolic resonance modes. It is the first example of real bulk hyperbolic metamaterials, consequently displaying the capability of tuning their responses along both in-plane and out-of-plane directions of the materials for the first time. It also distinctly interacts with unpolarized and polarized transverse magnetic and electronic beams to give unique hyperbolic responses. Our achievement can be a new platform to create various bulk metamaterials without complicated nanofabrication techniques. Our facile synthesis method using common laboratory techniques can open doors to broad-range researchers for active interdisciplinary studies for this otherwise hardly accessible technology.

Superconducting Sr2RuO4 Thin Films without Out-of-Phase Boundaries by Higher-Order Ruddlesden-Popper Intergrowth.

Abstract: Ruddlesden-Popper (RP) phases (An+1BnO3n+1, n = 1, 2,···) have attracted intensive research with diverse functionalities for device applications. However, the realization of a high-quality RP-phase film is hindered by the formation of out-of-phase boundaries (OPBs) that occur at terrace edges, originating from lattice mismatch in the c-axis direction with the A'B'O3 (n = ∞) substrate. Here, using strontium ruthenate RP-phase Sr2RuO4 (n = 1) as a model system, an experimental approach for suppressing OPBs was developed. By tuning the growth parameters, the Sr3Ru2O7 (n = 2) phase was formed in a controlled manner near the film-substrate interface. This higher-order RP-phase then blocked the subsequent formation of OPBs, resulting in nearly defect-free Sr2RuO4 layer at the upper region of the film. Consequently, the Sr2RuO4 thin films exhibited superconductivity up to 1.15 K, which is the highest among Sr2RuO4 films grown by pulsed laser deposition. This work paves the way for synthesizing pristine RP-phase heterostructures and exploring their unique physical properties.

Growth and atomically resolved polarization mapping of ferroelectric $Bi_2WO_6$ thin film

Abstract: Aurivillius ferroelectric $Bi_2WO_6$ (BWO) encompasses a broad range of functionalities, including robust fatigue-free ferroelectricity, high photocatalytic activity, and ionic conductivity. Despite these promising characteristics, an in-depth study on the growth of BWO thin films and ferroelectric characterization, especially at the atomic scale, is still lacking. Here, we report pulsed laser deposition (PLD) of BWO thin films on (001) $SrTiO_3$ substrates and characterization of ferroelectricity using the scanning transmission electron microscopy (STEM) and piezoresponse force microscopy (PFM) techniques. We show that the background oxygen gas pressure used during PLD growth mainly determines the phase stability of BWO films, whereas the influence of growth temperature is comparatively minor. Atomically resolved STEM study of a fully strained BWO film revealed collective in-plane polar off-centering displacement of W atoms. We estimated the spontaneous polarization value based on polar displacement mapping to be about 54 $\pm$ 4 ${\mu}C cm^{-2}$, which is in good agreement with the bulk polarization value. Furthermore, we found that pristine film is composed of type-I and type-II domains, with mutually orthogonal polar axes. Complementary PFM measurements further elucidated that the coexisting type-I and type-II domains formed a multidomain state that consisted of 90$°$ domain walls (DWs) alongside multiple head-to-head and tail-to-tail 180$°$ DWs. Application of an electrical bias led to in-plane 180$°$ polarization switching and 90$°$ polarization rotation, highlighting a unique aspect of domain switching, which is immune to substrate-induced strain.

In Situ Cryogenic HAADF-STEM Observation of Spontaneous Transition of Ferroelectric Polarization Domain Structures at Low Temperatures.

Abstract: Precise determination of atomic structures in ferroelectric thin films and their evolution with temperature is crucial for fundamental study and design of functional materials. However, this has been impeded by the lack of techniques applicable to a thin-film geometry. Here we use cryogenic scanning transmission electron microscopy (STEM) to observe the atomic structure of a BaTiO3 film on a (111)-SrTiO3 substrate under varying temperatures. Our study explicitly proves a structure transition from a complex polymorphic nanodomain configuration at room temperature transitioning to a homogeneous ground-state rhombohedral structure of BaTiO3 below ∼250 K, which was predicted by phase-field simulation. More importantly, another unexpected transition is revealed, a transition to complex nanodomains below ∼105 K caused by an altered mechanical boundary condition due to the antiferrodistortive phase transition of the SrTiO3 substrate. This study demonstrates the power of cryogenic STEM in elucidating structure-property relationships in numerous functional materials at low temperatures.

Growth and Atomically Resolved Polarization Mapping of Ferroelectric Bi2WO6 Thin Films

Abstract: Aurivillius ferroelectric Bi2WO6 (BWO) encompasses a broad range of functionalities, including robust fatigue-free ferroelectricity, high photocatalytic activity, and ionic conductivity. Despite th...

Observation of spin-dependent dual ferromagnetism in perovskite ruthenates.

Abstract: 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.

Online Cell Screening Algorithm Considering Cell Inconsistencies for Maximum Available Current Estimation

Abstract: In this paper, a novel online cell screening algorithm is proposed to estimate the available maximum current considering the inconsistencies of the hundreds of cells in the battery pack for electric vehicles. The available maximum current is defined based on the allowable terminal voltage, and the inconsistency parameters which affect the maximum available current are analyzed. The proposed algorithm screens the small number of candidates of which terminal voltages first exceed the allowable range by comprehensively comparing the inconsistency parameters. The proposed algorithm uses just the comparison operation for the parameters basically measured and estimated from the battery management system, which can reduce the computational burden significantly. The proposed algorithm is validated by experiments conducted on a nickel manganese cobalt oxide-type battery pack commercially manufactured for electric vehicles.

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

Abstract: 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.