arXiv subjects

Jong Mok Ok

Publications and source records attributed to Jong Mok Ok.

At least 19 recordsLinked to original sources

arXiv2026

Plasmonic polaron in self-intercalated 1T-TiS2

Electron-boson coupling is central to a comprehensive understanding of the diverse physical phenomena emerging from many-body interactions. Yet less attention has been paid to how plasmons, collective bosonic modes of electron density oscillation, interact with conduction electrons and how external parameters can tune this interaction. Here, we present a clear display of composite quasiparticles stemming from electron-plasmon coupling, known as the plasmonic polaron, in self-intercalated 1T-TiS2, by using angle-resolved photoemission spectroscopy (ARPES), high-resolution electron energy loss spectroscopy (HR-EELS) and first-principles calculations. The single particle spectral function exhibits a distinctive plasmon-loss satellite with the same characteristic energy scale determined by HR-EELS measurements. The bosonic energy scale of plasmonic polaron is tunable by controlling charge carrier density and temperature, distinguishing itself from conventional polarons arising from electron-phonon interactions. Furthermore, we find that the dielectric screening strongly affects the formation of the plasmonic polaron states. Our findings provide direct spectroscopic evidence of plasmonic polarons and establish self-intercalated layered materials as a promising platform for studying, controlling, and harnessing plasmonic interactions in quantum materials.

cond-mat.mtrl-sci↗

arXiv2025

Observation of gapless collective charge fluctuations in an Anderson insulating state

Understanding the nature of collective charge dynamics in the Coulomb gap phase is essential for revealing the existence of many-body localization. However, the corresponding many-particle excitation spectra remain poorly understood. Here, we present a comprehensive investigation of $^{27}$Al and $^{63}$Cu nuclear magnetic/quadrupole resonance (NMR/NQR), along with specific heat ($C_p$) measurements, in the $p$-type semiconductor CuAlO$_2$. Our study unveils distinct changes in charge dynamics at two crossover temperature scales which separate three regimes associated with Anderson localization of charge carriers: thermally activated transport ($T>150$ K) $\rightarrow$ Mott variable-range hopping (VRH) $\rightarrow$ Efros-Shklovskii (ES) VRH with Coulomb gap formation ($T<50$ K). In the ES VRH regime, we observe a striking divergence in the zero-field $^{63}$Cu spin-lattice relaxation rate, $(T_1T)^{-1}$, which is strongly suppressed by an applied magnetic field, indicative of quantum critical charge fluctuations. This is further supported by a distinct magnetic field-dependence of $C_p/T$ deep within the Coulomb gap phase. Taken together, these results provide compelling evidence for the emergence of strong, gapless collective charge fluctuations within the Anderson insulating phase where single-particle excitations are gapped.

cond-mat.str-el↗

arXiv2024

Colossal optical anisotropy in wide-bandgap semiconductor CuAlO2

Colossal optical anisotropy in the entire visible spectrum is crucial for advanced photonic applications, enabling precise light manipulation without optical loss across a broad spectral range. Here, we demonstrate that CuAlO2 exhibits colossal optical anisotropy and transparency across the visible spectrum, enabled by its unique three-dimensional O-Cu-O dumbbell structure and two-dimensionally confined excitons. Using mm-sized single crystals, we independently measured ab-plane and c-axis optical properties, revealing maximum birefringence (= 3.67) and linear dichroism (= 5.21), the highest reported to date. CuAlO2 retains birefringence over 0.5 throughout the entire visible range and possesses a wide direct bandgap of 3.71 eV, surpassing the birefringence of commercial anisotropic crystals transparent in the visible spectrum. From the two-dimensional screened hydrogen model and first-principles calculations, we demonstrate that the colossal anisotropy arises from a unique excitonic Cu d-p transition confined to the atomic-thick layer. This colossal optical anisotropy and transparency across the entire visible spectrum makes CuAlO2 a promising candidate for future photonic technologies.

cond-mat.mtrl-sci↗

arXiv2023

Suppression of Antiferromagnetic Order by Strain in Honeycomb Cobaltate: Implication for Quantum Spin Liquid

Recently, layered honeycomb cobaltates have been predicted as a new promising system for realizing the Kitaev quantum spin liquid, a many-body quantum entangled ground state characterized by fractional excitations. However, these cobaltates, similar to other candidate materials, exhibit classical antiferromagnetic ordering at low temperatures, which impedes the formation of the expected quantum state. Here, we demonstrate that the control of the trigonal crystal field of Co ions is crucial to suppress classical antiferromagnetic ordering and to locate its ground state in closer vicinity to quantum spin liquid in layered honeycomb cobaltates. By utilizing heterostructure engineering on Cu3Co2SbO6 thin films, we adjust the trigonal distortion of CoO6 octahedra and the associated trigonal crystal field. The original Néel temperature of 16 K in bulk Cu3Co2SbO6 decreases (increases) to 7.8 K (22.7 K) in strained Cu3Co2SbO6 films by decreasing (increasing) the magnitude of the trigonal crystal fields. Our experimental finding substantiates the potential of layered honeycomb cobaltate heterostructures and strain engineering to accomplish the extremely elusive quantum phase of matter.

cond-mat.str-el↗

arXiv2023

Exotic magnetic anisotropy near digitized dimensional Mott boundary

The magnetic anisotropy of low-dimensional Mott systems exhibits unexpected magnetotransport behavior useful for spin-based quantum electronics. Yet, the anisotropy of natural materials is inherently determined by the crystal structure, highly limiting its engineering. We demonstrate the magnetic anisotropy modulation near a digitized dimensional Mott boundary in artificial superlattices composed of a correlated magnetic monolayer SrRuO3 and nonmagnetic SrTiO3. The magnetic anisotropy is initially engineered by modulating the interlayer coupling strength between the magnetic monolayers. Interestingly, when the interlayer coupling strength is maximized, a nearly degenerate state is realized, in which the anisotropic magnetotransport is strongly influenced by both the thermal and magnetic energy scales. Our results offer a new digitized control for magnetic anisotropy in low-dimensional Mott systems, inspiring promising integration of Mottronics and spintronics.

cond-mat.str-el↗

arXiv2023

Theoretical investigation of delafossite-Cu2ZnSnO4 as a promising photovoltaic absorber

In the quest for efficient and cost-effective photovoltaic absorber materials beyond silicon, considerable attention has been directed toward exploring alternatives. One such material, zincblende-derived Cu2ZnSnS4 (CZTS), has shown promise due to its ideal band-gap size and high absorption coefficient. However, challenges such as structural defects and secondary phase formation have hindered its development. In this study, we examine the potential of another compound Cu2ZnSnO4 (CZTO) with a similar composition to CZTS as a promising alternative. Employing ab initio density function theory (DFT) calculations in combination with an evolutionary structure prediction algorithm, we identify that the crystalline phase of the delafossite structure is the most stable among the 900 (meta)stable CZTO. Its thermodynamic stability at room temperature is also confirmed by the molecular dynamics study. Excitingly, this new phase of CZTO displays a direct band gap where the dipole-allowed transition occurs, making it a strong candidate for efficient light absorption. Furthermore, the estimation of spectroscopic limited maximum efficiency (SLME) directly demonstrates the high potential of delafossite-CZTO as a photovoltaic absorber. Our numerical results suggest that delafossite-CZTO holds another promise for future photovoltaic applications.

cond-mat.mtrl-sci↗

arXiv2023

Optical detection of bond-dependent and frustrated spin in the two-dimensional cobalt-based honeycomb antiferromagnet Cu3Co2SbO6

Two-dimensional honeycomb antiferromagnet becomes an important class of materials as it can provide a route to Kitaev quantum spin liquid, characterized by massive quantum entanglement and fractional excitations. The signatures of its proximity to Kitaev quantum spin liquid in the honeycomb antiferromagnet includes anisotropic bond-dependent magnetic responses and persistent fluctuation by frustration in paramagnetic regime. Here, we propose Cu3Co2SbO6 heterostructures as an intriguing honeycomb antiferromagnet for quantum spin liquid, wherein bond-dependent and frustrated spins interact with optical excitons. This system exhibits antiferromagnetism at 16 K with different spin-flip magnetic fields between a bond-parallel and bond-perpendicular directions, aligning more closely with the generalized Heisenberg-Kitaev than the XXZ model. Optical spectroscopy reveals a strong excitonic transition coupled to the antiferromagnetism, enabling optical detection of its spin states. Particularly, such spin-exciton coupling presents anisotropic responses between bond-parallel and bond-perpendicular magnetic field as well as a finite spin-spin correlation function around 40 K, higher than twice its Néel temperature. The characteristic temperature that remains barely changed even under strong magnetic fields highlights the robustness of the spin-fluctuation region. Our results demonstrate Cu3Co2SbO6 as a unique candidate for the quantum spin liquid phase, where the spin Hamiltonian and quasiparticle excitations can be probed and potentially controlled by light.

cond-mat.str-el↗

arXiv2023

Control of Impurity Phase Segregation in a PdCrO$_2$/CuCrO$_2$ Heterostructure

PdCrO$_2$ films are synthesized on CuCrO$_2$ buffer layers on Al$_2$O$_3$ substrates. This synthesis is accompanied by impurity phase segregation, which hampers the synthesis of high quality PdCrO$_2$ films. The potential causes of impurity phase segregation were studied by using a combination of experiments and ab initio calculations. X-ray diffraction and scanning transmission electron microscopy experiments revealed impurity phases of Cu$_x$Pd$_{1-x}$ alloy and chromium oxides, Cr$_2$O$_3$ and Cr$_3$O$_4$, in PdCrO$_2$. Calculations determined that oxygen deficiency can cause the impurity phase segregation. Therefore, preventing oxygen release from delafossites could suppress the impurity phase segregation. The amounts of Cr$_2$O$_3$ and Cr$_3$O$_4$ depend differently on temperature and oxygen partial pressure. A reasonable theory-based explanation for this experimental observation is provided.

cond-mat.mtrl-sci↗

arXiv2023

Honeycomb oxide heterostructure: a new platform for Kitaev quantum spin liquid

Kitaev quantum spin liquid, massively quantum entangled states, is so scarce in nature that searching for new candidate systems remains a great challenge. Honeycomb heterostructure could be a promising route to realize and utilize such an exotic quantum phase by providing additional controllability of Hamiltonian and device compatibility, respectively. Here, we provide epitaxial honeycomb oxide thin film Na3Co2SbO6, a candidate of Kitaev quantum spin liquid proposed recently. We found a spin glass and antiferromagnetic ground states depending on Na stoichiometry, signifying not only the importance of Na vacancy control but also strong frustration in Na3Co2SbO6. Despite its classical ground state, the field-dependent magnetic susceptibility shows remarkable scaling collapse with a single critical exponent, which can be interpreted as evidence of quantum criticality. Its electronic ground state and derived spin Hamiltonian from spectroscopies are consistent with the predicted Kitaev model. Our work provides a unique route to the realization and utilization of Kitaev quantum spin liquid.

cond-mat.str-el↗

arXiv2022

Preparation of large Cu3Sn single crystal by Czochralski method

Cu3Sn was recently predicted to host topological Dirac fermions, but related research is still in its infancy. The growth of large and high-quality Cu3Sn single crystals is, therefore, highly desired to investigate the possible topological properties. In this work, we report the single crystal growth of Cu3Sn by Czochralski (CZ) method. Crystal structure, chemical composition, and transport properties of Cu3Sn single crystals were analyzed to verify the crystal quality. Notably, compared to the mm-sized crystals from a molten Sn-flux, the cm-sized crystals obtained by the CZ method are free from contamination from flux materials, paving the way for the follow-up works.

cond-mat.mtrl-sci↗

arXiv2022

Growth of delafossite CuAlO2 single crystals in a reactive crucible

Delafossite oxide CuAlO2 has engaged great attention as a promising p-type conducting oxide. In this work, high-quality CuAlO2 single crystals with a size of several millimeters (mm) are successfully achieved with a reactive crucible melting method. The crystals are characterized by X-ray diffraction, scanning electron microscopy with energy-dispersive spectroscopy, transport measurement, and magnetic susceptibility measurement. The grown single crystals are free of contamination from a copper oxide flux. This work provides a new approach to growing high-quality delafossite oxide CuAlO2 with a few mm size.

cond-mat.mtrl-sci↗

arXiv2022

Semi-Dirac and Weyl Fermions in Transition Metal Oxides

We show that a class of compounds with $I$4/$mcm$ crystalline symmetry hosts three-dimensional semi-Dirac fermions. Unlike the known two-dimensional semi-Dirac points, the degeneracy of these three-dimensional semi-Dirac points is not lifted by spin-orbit coupling due to the protection by a nonsymmorphic symmetry -- screw rotation in the $a-b$ plane and a translation along the $c$ axis. This crystalline symmetry is found in tetragonal perovskite oxides, realizable in thin films by epitaxial strain that results in a$^0$a$^0$c$^-$-type octahedral rotation. Interestingly, with broken time-reversal symmetry, two pairs of Weyl points emerge from the semi-Dirac points within the Brillouin zone, and an additional lattice distortion leads to enhanced intrinsic anomalous Hall effect. The ability to tune the Berry phase by epitaxial strain can be useful in novel oxide-based electronic devices.

cond-mat.str-el↗

arXiv2021

Correlated Oxide Dirac Semimetal in the Extreme Quantum Limit

Quantum materials (QMs) with strong correlation and non-trivial topology are indispensable to next-generation information and computing technologies. Exploitation of topological band structure is an ideal starting point to realize correlated topological QMs. Herein, we report that strain-induced symmetry modification in correlated oxide SrNbO3 thin films creates an emerging topological band structure. Dirac electrons in strained SrNbO3 films reveal ultra-high mobility (100,000 cm2/Vs), exceptionally small effective mass (0.04me), and non-zero Berry phase. More importantly, strained SrNbO3 films reach the extreme quantum limit, exhibiting a sign of fractional occupation of Landau levels and giant mass enhancement. Our results suggest that symmetry-modified SrNbO3 is a rare example of a correlated topological QM, in which strong correlation of Dirac electrons leads to the realization of fractional occupation of Landau levels.

cond-mat.str-el↗

arXiv2021

Atomic structure of initial nucleation layer in hexagonal perovskite BaRuO$_3$ thin films

Hexagonal perovskites are an attractive group of materials due to their various polymorph phases and rich structure-property relationships. BaRuO3 (BRO) is a prototypical hexagonal perovskite, in which the electromagnetic properties are significantly modified depending on its atomic structure. Whereas thin-film epitaxy would vastly expand the application of hexagonal perovskites by epitaxially stabilizing various metastable polymorphs, the atomic structure of epitaxial hexagonal perovskites, especially at the initial growth stage, has rarely been investigated. In this study, we show that an intriguing nucleation behavior takes place during the initial stabilization of a hexagonal perovskite 9R BaRuO3 (BRO) thin film on a (111) SrTiO3 (STO) substrate. We use high-resolution high-angle annular dark field scanning transmission electron microscopy in combination with geometrical phase analysis to understand the local strain relaxation behavior. We find that nano-scale strained layers, composed of different RuO6 octahedral stacking, are initially formed at the interface, followed by a relaxed single crystal9R BRO thin film. Within the interface layer, hexagonal BROs are nucleated on the STO (111) substrate by both corner- and face-sharing. More interestingly, we find that the boundaries between the differently-stacked nucleation layers, i.e. heterostructural boundaries facilitates strain relaxation, in addition to the formation of conventional misfit dislocations evolving from homostructural boundaries. Our observations reveal an important underlying mechanism to understand the thin-film epitaxy and strain accommodation in hexagonal perovskites.

cond-mat.mtrl-sci↗

arXiv2021

Epitaxial stabilization of metastable 3C BaRuO3 thin film with ferromagnetic non-Fermi liquid phase

Thin films of perovskite Ruthenates of the general formula ARuO3 (A = Ca and Sr) are versatile electrical conductors for viable oxide electronics. They are also scientifically intriguing, as they exhibit non-trivial electromagnetic ground states depending on the A-site element. Among them, realization of the cubic perovskite (3C) BaRuO3 thin film has been a challenge so far, because the 3C phase is metastable with the largest formation energy among the various polymorph phases of BaRuO3. In this study, we successfully prepared 3C BaRuO3 thin films employing epitaxial stabilization. The 3C BaRuO3 thin films show itinerant ferromagnetism with a transition temperature of ~48 K and a non-Fermi liquid phase. The epitaxial stabilization of the 3C BaRuO3 further enabled us to make a standard comparison of perovskite Ruthenates thin films, thereby establishing the importance of the Ru-O orbital hybridization in understanding the itinerant magnetic system.

cond-mat.mtrl-sci↗

arXiv2021

Twin-domain formation in epitaxial triangular lattice delafossites

Twin domains are often found as structural defects in symmetry mismatched epitaxial thin films. The delafossite ABO2, which has a rhombohedral structure, is a good example that often forms twin domains. Although bulk metallic delafossites are known to be the most conducting oxides, the high conductivity is yet to be realized in thin film forms. Suppressed conductivity found in thin films is mainly caused by the formation of twin domains, and their boundaries can be a source of scattering centers for charge carriers. To overcome this challenge, the underlying mechanism for their formation must be understood, so that such defects can be controlled and eliminated. Here, we report the origin of structural twins formed in a CuCrO2 delafossite thin film on a substrate with hexagonal or triangular symmetries. A robust heteroepitaxial relationship is found for the delafossite film with the substrate, and the surface termination turns out to be critical to determine and control the domain structure of epitaxial delafossites. Based on such discoveries, we also demonstrate a twin-free epitaxial thin films grown on high-miscut substrates. This finding provides an important synthesis strategy for growing single domain delafossite thin films and can be applied to other delafossites for epitaxial synthesis of high-quality thin films.

cond-mat.mtrl-sci↗

arXiv2021

Strain-induced atomic-scale building blocks for ferromagnetism in epitaxial LaCoO3

The origin of strain-induced ferromagnetism, which is robust regardless of the type and degree of strain in LaCoO3 (LCO) thin films, is enigmatic despite intensive research efforts over the past decade. Here, by combining scanning transmission electron microscopy with ab initio density functional theory plus U calculations, we report that the ferromagnetism does not emerge directly from the strain itself, but rather from the creation of compressed structural units within ferroelastically formed twin-wall domains. The compressed structural units are magnetically active with the rocksalt-type high-spin/low-spin order. Our study highlights that the ferroelastic nature of ferromagnetic structural units is important for understanding the intriguing ferromagnetic properties in LCO thin films.

cond-mat.mtrl-sci↗

arXiv2020

Strong antiferromagnetic proximity coupling in a heterostructured superconductor Sr$_2$VO$_3$FeAs

We report observation of strong magnetic proximity coupling in a heterostructured superconductor Sr$_2$VO$_3$FeAs, determined by the upper critical fields $H_{c2}(T)$ measurements up to 65 T. Using the resistivity and the radio-frequency measurements for both $H \parallel ab$ and $H \parallel c$, we found a strong upward curvature of $H_{c2}^c(T)$, together with a steep increase of $H_{c2}^{ab}(T)$ near $T_c$, yielding the anisotropic factor $γ_H=H_{c2}^{ab}/H_{c2}^c$ up to $\sim$ 20, the largest value among iron-based superconductors. These are attributed to the Jaccarino-Peter effect, rather than to the multiband effect, due to strong exchange interaction between itinerant Fe spins of the FeAs layers and localized V spins of Mott-insulating SrVO$_3$ layers. These findings provide evidence for strong antiferromagnetic proximity coupling, comparable with the intralayer superexchange interaction of SrVO$_3$ layer and sufficient to induce magnetic frustration in Sr$_2$VO$_3$FeAs.

cond-mat.str-el↗