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Jaewhan Oh

Publications and source records attributed to Jaewhan Oh.

4 recordsLinked to original sources

Correlative 3D Mapping of Structure, Composition, and Valence State Dynamics in Battery Cathodes via Simultaneous ADF-EDS-EELS Tomography

Understanding degradation in battery cathodes and other functional materials requires simultaneous knowledge of structural, chemical, and electronic changes in three dimensions (3D). Here, we present a simultaneous ADF-EDS-EELS tomography method that enables 3D mapping of atomic structure, composition, valence states, and transition metal inhomogeneity within a single, low-dose STEM tilt series acquisition. Applied to LiNi1/3Co1/3Mn1/3O2 (NCM111) particles at different electrochemical cycling stages, this method reveals nanoscale degradation processes with full spatial correlation. We observe that while chemical composition evolves uniformly throughout the entire primary particle, valence state changes and transition metal segregation are strongly depth-dependent and concentrated near the surface. This coexistence of bulk and surface-driven degradation dynamics reveals distinct mechanisms acting at different spatial scales. The evolution of inhomogeneity and valence states deviates from simple phase transition models, highlighting the roles of ion migration and dissolution-driven segregation. Our findings establish valence state gradients and nanoscale inhomogeneity as active contributors to cathode failure. More broadly, this correlative 3D platform opens new opportunities for studying redox-driven transformations in fields such as neuromorphic computing and heterogeneous catalysis, where composition-structure-function coupling is inherently three-dimensional.

cond-mat.mtrl-sci

Spatial correlations of charge density wave order across the transition in 2H-NbSe2

Charge density waves (CDWs) involve coupled amplitude and phase degrees of freedom, but direct access to local amplitude correlations remains experimentally challenging. Here, we report cryogenic four-dimensional scanning transmission electron microscopy (4D-STEM) measurements of CDW ordering in a 2H-NbSe2 flake of 24 nm thickness, enabled by liquid helium-based cooling. By mapping the spatial distribution of CDW superlattice intensities at nanometer-scale resolution and analyzing their autocorrelations, we extract the temperature-dependent correlation length associated with the local amplitude of the CDW order parameter, independent of global phase coherence. Our results reveal that a finite local CDW amplitude is already established well above the transition temperature. When the system is cooled below the transition temperature down to 20 K, the correlation length extends to nearly 110 nm, and the local CDW amplitude is found to strongly anticorrelate with the local strain field.

cond-mat.str-el

Singular Hall response from a correlated ferromagnetic flat nodal-line semimetal

Topological quantum phases have been largely understood in weakly correlated systems, which have identified various quantum phenomena such as spin Hall effect, protected transport of helical fermions, and topological superconductivity. Robust ferromagnetic order in correlated topological materials particularly attracts attention, as it can provide a versatile platform for novel quantum devices. Here, we report singular Hall response arising from a unique band structure of flat topological nodal lines in combination with electron correlation in an itinerant, van der Waals ferromagnetic semimetal, Fe3GaTe2, with a high Curie temperature of Tc=360 K. High anomalous Hall conductivity violating the conventional scaling, resistivity upturn at low temperature, and a large Sommerfeld coefficient are observed in Fe3GaTe2, which implies heavy fermion features in this ferromagnetic topological material. Our circular dichroism in angle-resolved photoemission spectroscopy and theoretical calculations support the original electronic features in the material. Thus, low-dimensional Fe3GaTe2 with electronic correlation, topology, and room-temperature ferromagnetic order appears to be a promising candidate for robust quantum devices.

cond-mat.str-el

Revealing the Three-Dimensional Arrangement of Polar Topology in Nanoparticles

In the early 2000s, low dimensional systems were predicted to have topologically nontrivial polar structures, such as vortices or skyrmions, depending on mechanical or electrical boundary conditions. A few variants of these structures have been experimentally observed in thin film model systems, where they are engineered by balancing electrostatic charge and elastic distortion energies. However, the measurement and classification of topological textures for general ferroelectric nanostructures have remained elusive, as it requires mapping the local polarization at the atomic scale in three dimensions. Here we unveil topological polar structures in ferroelectric BaTiO3 nanoparticles via atomic electron tomography, which enables us to reconstruct the full three-dimensional arrangement of cation atoms at an individual atom level. Our three-dimensional polarization maps reveal clear topological orderings, along with evidence of size-dependent topological transitions from a single vortex structure to multiple vortices, consistent with theoretical predictions. The discovery of the predicted topological polar ordering in nanoscale ferroelectrics, independent of epitaxial strain, widens the research perspective and offers potential for practical applications utilizing contact-free switchable toroidal moments.

cond-mat.mtrl-sci