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Sungsoo Hahn

Publications and source records attributed to Sungsoo Hahn.

12 recordsLinked to original sources

Entwined lattice of atoms and anionic electrons in layered electride LaCl

Controlling the lattice geometry that governs electronic structure is a central theme in condensed-matter physics, yet in crystalline solids this geometry is usually fixed by the atomic framework. Electrides offer an alternative route to electronic structure design in which their excess electrons can organize into anionic electron lattice (AEL) and provide a lattice-like degree of freedom. Recent work has highlighted the standalone limit, where the AEL in YCl yields bands well described by the dice-lattice model. Here, using angle-resolved photoemission spectroscopy (ARPES), we show that LaCl, although isostructural to YCl, realizes a qualitatively different regime where the AEL is entwined with the La cation framework, producing a fully reconstructed electronic structure. Combining the ARPES result with tight-binding model analysis, we demonstrate that this radical divergence stems from the activation of direct hopping channels between the AEL and the La atomic lattice. This coupling reshapes the effective lattice geometry, reconstructs the electronic states, and modifies the associated Chern band topology, transforming the bipartite dice-lattice network in YCl into a tripartite structure in LaCl. Our findings demonstrate that the coupling between the AEL and the atomic lattice can actively shape the effective lattice geometry that governs the electronic structure. This coupling can act as a powerful tuning knob for electronic structure design that is inaccessible in conventional materials.

cond-mat.str-el

Observation of spin-free interatomic orbital angular momentum in a chiral crystal

The inherent spin-orbit interaction of electrons inevitably couples spin to the orbital angular momentum (OAM), posing a fundamental challenge to spin-free orbital transport. Here, we propose a novel strategy to achieve spin-decoupled OAM states in crystalline solids. Using angle-resolved photoemission spectroscopy (ARPES), we resolve well-isolated s-orbital bands in a chiral Te crystal, clearly separated from the p-orbital manifold. Combined circular dichroism ARPES and first-principles calculations reveal that these bands host OAM arising exclusively from interatomic hopping, with no intra-atomic contribution. Spin-resolved ARPES further confirms the absence of spin angular momentum (SAM), providing decisive evidence of spin-free OAM states. These findings establish the existence of OAM without spin polarization in crystalline solids and highlight the essential role of inter-atomic OAM. This work provides a general framework for designing spinless OAM states, opening an opportunity toward pure orbital currents for orbitronics.

cond-mat.mtrl-sci

Magnetic-fluctuation-driven suppression of spin-orbit hybridization in the surface ferromagnet GdAg$_2$/Ag(111)

Magnetic materials hosting topological band structures have attracted intense interest due to the interplay between magnetism and spin-orbit coupling (SOC). Here, using temperature- and polarization-dependent angle-resolved photoemission spectroscopy, we investigate the surface ferromagnet GdAg$_2$/Ag(111), a two-dimensional system with Weyl-nodal-line-like band crossings. We find that spin fluctuations preserve the nodal-line-derived band crossings even above the Curie temperature, while SOC-induced hybridization develops only at low temperatures, as evidenced by spectral-weight redistribution. The suppression of the hybridization at high temperature is attributed to spin decoherence and band-dependent scattering, captured by an effective non-Hermitian framework. Our results establish magnetic fluctuations as a control knob for SOC-induced hybridization and associated Berry curvature, and highlight magnetic systems as a platform for exploring non-Hermitian band physics.

cond-mat.str-el

Low-dimensionality-induced tunable ferromagnetism in SrRuO$_3$ ultrathin films

Quantum materials near electronic or magnetic phase boundaries exhibit enhanced tunability, as their emergent properties become highly sensitive to external perturbations. Here, we demonstrate precise control of ferromagnetism in a SrRuO$_3$ ultrathin film, where a high density of states (DOS), arising from low-dimensional quantum states, places the system at the crossover between a non-magnetic and bulk ferromagnetic state. Using spin- and angle-resolved photoemission spectroscopy (SRPES/ARPES), transport measurements, and theoretical calculations, we systematically tune the Fermi level via electron doping across the high-DOS point. We directly visualize the spin-split band structure and reveal its influence on both magnetic and transport properties. Our findings provide compelling evidence that magnetism can be engineered through DOS control at a phase crossover, establishing a pathway for the rational design of tunable quantum materials.

cond-mat.str-el

Fragility of Topology under Electronic Correlations in Iron Chalcogenides

The interplay between electronic correlations and topology is a central topic in the study of quantum materials. In this work, we investigate the impact of the orbital-selective Mott phase (OSMP) on the topological properties of FeTe1-xSex (FTS), an iron chalcogenide superconductor known to host both non-trivial Z2 topology and strong electronic correlations. Using angle-resolved photoemission spectroscopy, we track the evolution of topological surface states across various doping levels and temperatures. We identify a topological phase transition between trivial and non-trivial topology as a function of selenium content, with critical behavior observed between x = 0.04 and x = 0.09. Additionally, we find that at elevated temperatures, the coherence of the topological surface state deteriorates due to the emergence of OSMP, despite the topological invariant remaining intact. Our results demonstrate that the non-trivial topology in iron chalcogenide is fragile under strong electronic correlations.

cond-mat.str-el

Tuning orbital-selective phase transitions in a two-dimensional Hund's correlated system

Hund's rule coupling ($\textit{J}$) has attracted much attention recently for its role in the description of the novel quantum phases of multi orbital materials. Depending on the orbital occupancy, $\textit{J}$ can lead to various intriguing phases. However, experimental confirmation of the orbital occupancy dependency has been difficult as controlling the orbital degrees of freedom normally accompanies chemical inhomogeneities. Here, we demonstrate a method to investigate the role of orbital occupancy in $\textit{J}$ related phenomena without inducing inhomogeneities. By growing SrRuO$_3$ monolayers on various substrates with symmetry-preserving interlayers, we gradually tune the crystal field splitting and thus the orbital degeneracy of the Ru $\textit{t$_2$$_g$}$ orbitals. It effectively varies the orbital occupancies of two-dimensional (2D) ruthenates. Via in-situ angle-resolved photoemission spectroscopy, we observe a progressive metal-insulator transition (MIT). It is found that the MIT occurs with orbital differentiation: concurrent opening of a band insulating gap in the $\textit{d$_x$$_y$}$ band and a Mott gap in the $\textit{d$_x$$_z$$_/$$_y$$_z$}$ bands. Our study provides an effective experimental method for investigation of orbital-selective phenomena in multi-orbital materials.

cond-mat.str-el

Heteroepitaxial control of Fermi liquid, Hund metal, and Mott insulator phases in the single-atomic-layer limit

Interfaces between dissimilar correlated oxides can offer devices with versatile functionalities. In that respect, manipulating and measuring novel physical properties of oxide heterointerfaces are highly desired. Yet, despite extensive studies, obtaining direct information on their momentum-resolved electronic structure remains a great challenge. This is because most correlated interfacial phenomena appear within a few atomic layers from the interface, thus limiting the application of available experimental probes. Here, we utilize atomic-scale epitaxy and photoemission spectroscopy to demonstrate the interface control of correlated electronic phases in atomic-scale ruthenate--titanate heterostructures. While bulk SrRuO$_3$ is a ferromagnetic metal, the heterointerfaces exclusively realize three distinct correlated phases in the single-atomic-layer limit. Our theory reveals that atomic-scale structural proximity effects lead to the emergence of Fermi liquid, Hund metal, and Mott insulator phases in the quantum-confined SrRuO$_3$. These results highlight the extensive interfacial tunability of electronic phases, hitherto hidden in the atomically thin correlated heterostructure.

cond-mat.str-el

Flexoelectric control of a ferromagnetic metal

Electric fields have played a key role in discovering and controlling exotic electronic states of condensed matter. However, electric fields usually do not work in metals as free carriers tend to screen electrostatic fields. While a pseudo-electric field generated by inhomogeneous lattice strain, namely a flexoelectric field, can in principle work in all classes of materials, it remains experimentally unexplored in metals. Here, using heteroepitaxy and atomic-scale imaging, we show that flexoelectric fields can polarize a metallic oxide SrRuO3 with unexpectedly large Ru off-center displacements. We also observe that the flexoelectrically induced polar state of SrRuO3 leads to sizable lattice expansion, similar to the electrostrictive expansion caused by ionic displacements in dielectrics under an external electric field. We further suggest that flexoelectrically driven Ru off-centering promotes strong coupling between lattice and electronic degrees of freedom, possibly enhancing the ferromagnetism of SrRuO3. Beyond conventional electric fields, flexoelectric fields may universally engender novel electronic states and their control via pure atomic displacements in a nondestructive and fast manner.

cond-mat.mtrl-sci

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

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

Capping and gate control of anomalous Hall effect and hump structure in ultra-thin SrRuO$_3$ films

Ferromagnetism and exotic topological structures in SrRuO$_3$ (SRO) induce sign-changing anomalous Hall effect (AHE). Recently, hump structures have been reported in the Hall resistivity of SRO thin films, especially in the ultra-thin regime. We investigate the AHE and hump structure in the Hall resistivity of SRO ultra-thin films with an SrTiO$_3$ (STO) capping layer and ionic liquid gating. STO capping results in sign changes in the AHE and modulation of the hump structure. In particular, the hump structure in the Hall resistivity is strongly modulated and even vanishes in STO-capped 4 unit cell (uc) films. In addition, the conductivity of STO-capped SRO ultra-thin films is greatly enhanced with restored ferromagnetism. We also performed ionic liquid gating to modulate the electric field at SRO/STO interface. Drastic changes in the AHE and hump structure are observed with different gate voltages. Our study shows that the hump structure as well as the AHE can be controlled by tuning inversion symmetry and the electric field at the interface.

cond-mat.mtrl-sci

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