Showing 1–50 of 91 results for author: Ryu, H

Tuning the low-energy band structure in twisted bilayer WSe2

Authors: T. -H. -Y. Vu, O. J. Clark, N. H. Jo, J. Blyth, Q. Li, C. Jozwiak, A. Bostwick, J. B. Muir, L. Jia, J. A. Davis, I. Di Bernardo, A. Grubisic Cabo, K. Xing, W. Zhao, S. H. Ryu, S. H. Lee, Z. Mao, K. Watanabe, T. Taniguchi, B. A. Chambers, S. L. Harmer, E. Rotenberg, M. S. Fuhrer, M. T. Edmonds

Abstract: Tuning the electronic structures of two-dimensional (2D) material-based heterostructures is of crucial importance for their use in functional next-generation electronics. Here, through angle-resolved photoemission spectroscopy with nanoscale spatial resolution (nano-ARPES), we systematically track the evolution of the near-Fermi-level electronic structure of bilayer WSe2 over a large range of twis… ▽ More Tuning the electronic structures of two-dimensional (2D) material-based heterostructures is of crucial importance for their use in functional next-generation electronics. Here, through angle-resolved photoemission spectroscopy with nanoscale spatial resolution (nano-ARPES), we systematically track the evolution of the near-Fermi-level electronic structure of bilayer WSe2 over a large range of twist angle. While the momentum positioning of the valence band maxima is independent of twist angle, we find that the energetic separation between the hole bands at the K point of the Brillouin zone and the higher binding-energy hole band at Γ can be varied in excess of 100 meV. We explore the mechanisms underpinning this evolution and discuss the implications for tuning both the size of the band gaps, and the efficiency of the spin-dependent electron-phonon coupling channels in homobilayer transition metal dichalcogenide devices. △ Less

Submitted 19 May, 2026; originally announced May 2026.

Plasmonic polaron in self-intercalated 1T-TiS2

Authors: Byoung Ki Choi, Woojin Choi, Zhiyu Tao, Ji-Eun Lee, Sae Hee Ryu, Seungrok Mun, Hyobeom Lee, Kyoungree Park, Seha Lee, Hayoon Im, Yong Zhong, Hyejin Ryu, Min Jae Kim, Sue Hyeon Hwang, Xuetao Zhu, Jiandong Guo, Jong Mok Ok, Jaekwang Lee, Haeyong Kang, Sungkyun Park, Jonathan D. Denlinger, Heung-Sik Kim, Aaron Bostwick, Zhi-Xun Shen, Choongyu Hwang , et al. (2 additional authors not shown)

Abstract: 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 s… ▽ More 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. △ Less

Submitted 3 March, 2026; originally announced March 2026.

Operational Quasiprobability in Quantum Thermodynamics: Work Extraction by Coherence and Non-joint Measurability

Authors: Jeongwoo Jae, Junghee Ryu, Hoon Ryu

Abstract: We employ the operational quasiprobability (OQ) as a work distribution, which reproduces the Jarzynski equality and yields the average work consistent with the classical definition. The OQ distribution can be experimentally implemented through the end-point measurement and the two-point measurement scheme. Using this framework, we demonstrate the explicit contribution of coherence to the fluctuati… ▽ More We employ the operational quasiprobability (OQ) as a work distribution, which reproduces the Jarzynski equality and yields the average work consistent with the classical definition. The OQ distribution can be experimentally implemented through the end-point measurement and the two-point measurement scheme. Using this framework, we demonstrate the explicit contribution of coherence to the fluctuation, the average, and the second moment of work. In a two-level system, we show that non-joint measurability, a generalized notion of measurement incompatibility, can increase the amount of extractable work beyond the classical bound imposed by jointly measurable measurements. We further prove that the real part of Kirkwood-Dirac quasiprobability (KDQ) and the OQ are equivalent in two-level systems, and they are nonnegative for binary unbiased measurements if and only if the measurements are jointly measurable. In a three-level Nitrogen-vacancy center system, the OQ and the KDQ exhibit different amounts of negativities while enabling the same work extraction, implying that the magnitude of negativity is not a faithful indicator of nonclassical work. These results highlight that coherence and non-joint measurability play fundamental roles in the enhancement of work. △ Less

Submitted 5 October, 2025; originally announced October 2025.

Comments: 12 pages, 3 figures

Quantum simulation approach to ultra-weak magnetic anisotropy in a frustrated spin-1/2 antiferromagnet

Authors: Ki Won Jeong, Jae Yeon Seo, Sunghyun Lim, Jae Min Hong, Hyeon Jun Ryu, Jongseok Byeon, Kyungsun Moon, Nara Lee, Young Jai Choi

Abstract: The intrinsic equivalence between electron spin and qubit offers a natural foundation for quantum simulations of magnetic materials. However, incorporating magnetocrystalline anisotropy (MCA), a key feature of real magnets, remains a major challenge. Here, we develop a quantum simulation framework for MCA in CuSb2O6, a spin-1/2 antiferromagnet with alternating ferromagnetic chains arising from fru… ▽ More The intrinsic equivalence between electron spin and qubit offers a natural foundation for quantum simulations of magnetic materials. However, incorporating magnetocrystalline anisotropy (MCA), a key feature of real magnets, remains a major challenge. Here, we develop a quantum simulation framework for MCA in CuSb2O6, a spin-1/2 antiferromagnet with alternating ferromagnetic chains arising from frustrated, anisotropic exchange interactions in a nearly square lattice. The $\mathrm{Cu}^{2+}$ spin network is modeled as a four-qubit square lattice, with four paired ancilla qubits introduced to encode angle-dependent MCA. This two-qubit representation per spin site resolves the limitation that squared Pauli operators yield only the identity, enabling MCA terms to be faithfully embedded into quantum circuits. Using the variational quantum eigensolver, we determine an exceptionally small easy-axis MCA constant, just 0.00022% of the nearest-neighbor exchange interaction, yet sufficient to drive a spin-flop transition with $90^{\circ}$ spin reorientation and strong angular variation in magnetic torque. Beyond this regime, the simulations uncover a half-saturated magnetic phase at ultra-high fields, stabilized by anisotropic next-nearest-neighbor interactions. Our findings demonstrate the feasibility of resource-efficient quantum simulations of complex magnetic phenomena in real materials. △ Less

Submitted 1 October, 2025; v1 submitted 26 September, 2025; originally announced September 2025.

Unusual ferromagnetic band evolution and high Curie temperature in monolayer 1T-CrTe2 on bilayer graphene

Authors: Kyoungree Park, Ji-Eun Lee, Dongwook Kim, Yong Zhong, Camron Farhang, Hyobeom Lee, Hayoon Im, Woojin Choi, Seha Lee, Seungrok Mun, Kyoo Kim, Jun Woo Choi, Hyejin Ryu, Jing Xia, Heung-Sik Kim, Choongyu Hwang, Ji Hoon Shim, Zhi-Xun Shen, Sung-Kwan Mo, Jinwoong Hwang

Abstract: 2D van der Waals ferromagnets hold immense promise for spintronic applications due to their controllability and versatility. Despite their significance, the realization and in-depth characterization of ferromagnetic materials in atomically thin single layers, close to the true 2D limit, has been scarce. Here, a successful synthesis of monolayer (ML) 1T-CrTe2 is reported on a bilayer graphene (BLG)… ▽ More 2D van der Waals ferromagnets hold immense promise for spintronic applications due to their controllability and versatility. Despite their significance, the realization and in-depth characterization of ferromagnetic materials in atomically thin single layers, close to the true 2D limit, has been scarce. Here, a successful synthesis of monolayer (ML) 1T-CrTe2 is reported on a bilayer graphene (BLG) substrate via molecular beam epitaxy. Using angle-resolved photoemission spectroscopy and magneto-optical Kerr effect measurements, that the ferromagnetic transition is observed at the Curie temperature (TC) of 150 K in ML 1T-CrTe2 on BLG, accompanied by unconventional temperature-dependent band evolutions. The spectroscopic analysis and first-principle calculations reveal that the ferromagnetism may arise from Goodenough-Kanamori super-exchange and double-exchange interactions, enhanced by the lattice distortion and the electron doping from the BLG substrate. These findings provide pivotal insight into the fundamental understanding of mechanisms governing 2D ferromagnetism and offer a pathway for engineering higher TC in 2D materials for future spintronic devices. △ Less

Submitted 11 September, 2025; originally announced September 2025.

Comments: 26 pages, 4 figures

Journal ref: Small 2025

Local interface effects modulate global charge order and optical properties of 1T-TaS$_2$/1H-WSe$_2$ heterostructures

Authors: Samra Husremović, Valerie S. McGraw, Medha Dandu, Lilia S. Xie, Sae Hee Ryu, Oscar Gonzalez, Shannon S. Fender, Madeline Van Winkle, Karen C. Bustillo, Takashi Taniguchi, Kenji Watanabe, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Archana Raja, Katherine Inzani, D. Kwabena Bediako

Abstract: 1T-TaS$_2$ is a layered charge density wave (CDW) crystal exhibiting sharp phase transitions and associated resistance changes. These resistance steps could be exploited for information storage, underscoring the importance of controlling and tuning CDW states. Given the importance of out-of-plane interactions in 1T-TaS$_2$, modulating interlayer interactions by heterostructuring is a promising met… ▽ More 1T-TaS$_2$ is a layered charge density wave (CDW) crystal exhibiting sharp phase transitions and associated resistance changes. These resistance steps could be exploited for information storage, underscoring the importance of controlling and tuning CDW states. Given the importance of out-of-plane interactions in 1T-TaS$_2$, modulating interlayer interactions by heterostructuring is a promising method for tailoring CDW phase transitions. In this work, we investigate the optical and electronic properties of heterostructures comprising 1T-TaS$_2$ and monolayer 1H-WSe$_2$. By systematically varying the thickness of 1T-TaS$_2$ and its azimuthal alignment with 1H-WSe$_2$, we find that intrinsic moiré strain and interfacial charge transfer introduce CDW disorder in 1T-TaS$_2$ and modify the CDW ordering temperature. Furthermore, our studies reveal that the interlayer alignment impacts the exciton dynamics in 1H-WSe$_2$, indicating that heterostructuring can concurrently tailor the electronic phases in 1T-TaS$_2$ and the optical properties of 1H-WSe$_2$. This work presents a promising approach for engineering optoelectronic behavior of heterostructures that integrate CDW materials and semiconductors. △ Less

Submitted 2 August, 2025; originally announced August 2025.

Dark states of electrons in a quantum system with two pairs of sublattices

Authors: Yoonah Chung, Minsu Kim, Yeryn Kim, Seyeong Cha, Joon Woo Park, Jeehong Park, Yeonjin Yi, Dongjoon Song, Jung Hyun Ryu, Kimoon Lee, Timur K. Kim, Cephise Cacho, Jonathan Denlinger, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Keun Su Kim

Abstract: A quantum state of matter that is forbidden to interact with photons and is therefore undetectable by spectroscopic means is called a dark state. This basic concept can be applied to condensed matter where it suggests that a whole band of quantum states could be undetectable across a full Brillouin zone. Here we report the discovery of such condensed matter dark states in palladium diselenide as a… ▽ More A quantum state of matter that is forbidden to interact with photons and is therefore undetectable by spectroscopic means is called a dark state. This basic concept can be applied to condensed matter where it suggests that a whole band of quantum states could be undetectable across a full Brillouin zone. Here we report the discovery of such condensed matter dark states in palladium diselenide as a model system that has two pairs of sublattices in the primitive cell. By using angle-resolved photoemission spectroscopy, we find valence bands that are practically unobservable over the whole Brillouin zone at any photon energy, polarisation, and scattering plane. Our model shows that two pairs of sublattices located at half-translation positions and related by multiple glide-mirror symmetries make their relative quantum phases polarised into only four kinds, three of which become dark due to double destructive interference. This mechanism is generic to other systems with two pairs of sublattices, and we show how the phenomena observed in cuprates, lead-halide perovskites, and density wave systems can be resolved by the mechanism of dark states. Our results suggest that the sublattice degree of freedom, which has been overlooked so far, should be considered in the study of correlated phenomena and optoelectronic characteristics. △ Less

Submitted 10 July, 2025; originally announced July 2025.

Journal ref: Nature Physics 20, 1582-1588 (2024)

Pseudogap in a crystalline insulator doped by disordered metals

Authors: Sae Hee Ryu, Minjae Huh, Do Yun Park, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Keun Su Kim

Abstract: A key to understand how electrons behave in crystalline solids is the band structure that connects the energy of electron waves to their wavenumber (k). Even in the phase of matter with only short-range order (liquid or amorphous solid), the coherent part of electron waves still possesses a band structure. Theoretical models for the band structure of liquid metals were formulated more than 5 decad… ▽ More A key to understand how electrons behave in crystalline solids is the band structure that connects the energy of electron waves to their wavenumber (k). Even in the phase of matter with only short-range order (liquid or amorphous solid), the coherent part of electron waves still possesses a band structure. Theoretical models for the band structure of liquid metals were formulated more than 5 decades ago, but thus far, bandstructure renormalization and pseudogap induced by resonance scattering have remained unobserved. Here, we report the observation of this unusual band structure at the interface of a crystalline insulator (black phosphorus) and disordered dopants (alkali metals). We find that a conventional parabolic band structure of free electrons bends back towards zero k with the pseudogap of 30-240 meV from the Fermi level. This is k renormalization caused by resonance scattering that leads to the formation of quasi-bound states in the scattering potential of alkali-metal ions. The depth of this potential tuned by different kinds of alkali metal (Na, K, Rb, and Cs) allows to classify the pseudogap of p-wave and d-wave resonance. Our results may provide a clue to the puzzling spectrum of various crystalline insulators doped by disordered dopants, such as the waterfall dispersion in cuprates. △ Less

Submitted 10 July, 2025; originally announced July 2025.

Journal ref: Nature 596, 68-73 (2021)

A variational quantum eigensolver tailored to multi-band tight-binding simulations of electronic structures

Authors: Dongkeun Lee, Hoon Ryu

Abstract: We propose a cost-efficient measurement scheme of the variational quantum eigensolver (VQE) for atomistic simulations of electronic structures based on a tight-binding (TB) theory. Leveraging the lattice geometry of a material domain, the sparse TB Hamiltonian is constructed in a bottom-up manner and is represented as a linear combination of the standard-basis (SB) operators. The cost function is… ▽ More We propose a cost-efficient measurement scheme of the variational quantum eigensolver (VQE) for atomistic simulations of electronic structures based on a tight-binding (TB) theory. Leveraging the lattice geometry of a material domain, the sparse TB Hamiltonian is constructed in a bottom-up manner and is represented as a linear combination of the standard-basis (SB) operators. The cost function is evaluated with an extended version of the Bell measurement circuit that can simultaneously measure multiple SB operators and therefore reduces the number of circuits required bythe evaluation process. The proposed VQE scheme is applied to find band-gap energies of metal-halide-perovskite supercells that have finite dimensions with closed boundaries and are described with a sp3 TB model. Experimental results confirm that the proposed scheme gives solutions that follow well the accurate ones, but, more importantly, has the computing efficiency that is obviously superior to the commutativity-based Pauli grouping methods. Extending the application scope of VQE to three-dimensional confined atomic structures, this work can serve as a practical guideline for handling TB simulations in the noise-intermediate-scale quantum devices. △ Less

Submitted 23 May, 2025; originally announced May 2025.

Comments: 12 pages, 7 figures, 48 references

Journal ref: Journal of Chemical Theory and Computation, 2025

Spin-orbit-splitting-driven nonlinear Hall effect in NbIrTe4

Authors: Ji-Eun Lee, Aifeng Wang, Shuzhang Chen, Minseong Kwon, Jinwoong Hwang, Minhyun Cho, Ki-Hoon Son, Dong-Soo Han, Jun Woo Choi, Young Duck Kim, Sung-Kwan Mo, Cedomir Petrovic, Choongyu Hwang, Se Young Park, Chaun Jang, Hyejin Ryu

Abstract: The Berry curvature dipole (BCD) serves as a one of the fundamental contributors to emergence of the nonlinear Hall effect (NLHE). Despite intense interest due to its potential for new technologies reaching beyond the quantum efficiency limit, the interplay between BCD and NLHE has been barely understood yet in the absence of a systematic study on the electronic band structure. Here, we report NLH… ▽ More The Berry curvature dipole (BCD) serves as a one of the fundamental contributors to emergence of the nonlinear Hall effect (NLHE). Despite intense interest due to its potential for new technologies reaching beyond the quantum efficiency limit, the interplay between BCD and NLHE has been barely understood yet in the absence of a systematic study on the electronic band structure. Here, we report NLHE realized in NbIrTe4 that persists above room temperature coupled with a sign change in the Hall conductivity at 150 K. First-principles calculations combined with angle-resolved photoemission spectroscopy (ARPES) measurements show that BCD tuned by the partial occupancy of spin-orbit split bands via temperature is responsible for the temperature-dependent NLHE. Our findings highlight the correlation between BCD and the electronic band structure, providing a viable route to create and engineer the non-trivial Hall effect by tuning the geometric properties of quasiparticles in transition-metal chalcogen compounds. △ Less

Submitted 21 August, 2024; originally announced August 2024.

Journal ref: Nature Communications 15, 3971 (2024)

Controlling structure and interfacial interaction of monolayer TaSe2 on bilayer graphene

Authors: Hyobeom Lee, Hayoon Im, Byoung Ki Choi, Kyoungree Park, Yi Chen, Wei Ruan, Yong Zhong, Ji-Eun Lee, Hyejin Ryu, Michael F. Crommie, Zhi-Xun Shen, Choongyu Hwang, Sung-Kwan Mo, Jinwoong Hwang

Abstract: Tunability of interfacial effects between two-dimensional (2D) crystals is crucial not only for understanding the intrinsic properties of each system, but also for designing electronic devices based on ultra-thin heterostructures. A prerequisite of such heterostructure engineering is the availability of 2D crystals with different degrees of interfacial interactions. In this work, we report a contr… ▽ More Tunability of interfacial effects between two-dimensional (2D) crystals is crucial not only for understanding the intrinsic properties of each system, but also for designing electronic devices based on ultra-thin heterostructures. A prerequisite of such heterostructure engineering is the availability of 2D crystals with different degrees of interfacial interactions. In this work, we report a controlled epitaxial growth of monolayer TaSe2 with different structural phases, 1H and 1T, on a bilayer graphene (BLG) substrate using molecular beam epitaxy, and its impact on the electronic properties of the heterostructures using angle-resolved photoemission spectroscopy. 1H-TaSe2 exhibits significant charge transfer and band hybridization at the interface, whereas 1T-TaSe2 shows weak interactions with the substrate. The distinct interfacial interactions are attributed to the dual effects from the differences of the work functions as well as the relative interlayer distance between TaSe2 films and BLG substrate. The method demonstrated here provides a viable route towards interface engineering in a variety of transition-metal dichalcogenides that can be applied to future nano-devices with designed electronic properties. △ Less

Submitted 27 July, 2024; originally announced July 2024.

Comments: 23 pages, 4 figures

Journal ref: Nano Convergence 11, 14 (2024)

Tailored topotactic chemistry unlocks heterostructures of magnetic intercalation compounds

Authors: Samra Husremović, Oscar Gonzalez, Berit H. Goodge, Lilia S. Xie, Zhizhi Kong, Wanlin Zhang, Sae Hee Ryu, Stephanie M. Ribet, Karen C. Bustillo, Chengyu Song, Jim Ciston, Takashi Taniguchi, Kenji Watanabe, Colin Ophus, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, D. Kwabena Bediako

Abstract: The construction of thin film heterostructures has been a widely successful archetype for fabricating materials with emergent physical properties. This strategy is of particular importance for the design of multilayer magnetic architectures in which direct interfacial spin--spin interactions between magnetic phases in dissimilar layers lead to emergent and controllable magnetic behavior. However,… ▽ More The construction of thin film heterostructures has been a widely successful archetype for fabricating materials with emergent physical properties. This strategy is of particular importance for the design of multilayer magnetic architectures in which direct interfacial spin--spin interactions between magnetic phases in dissimilar layers lead to emergent and controllable magnetic behavior. However, crystallographic incommensurability and atomic-scale interfacial disorder can severely limit the types of materials amenable to this strategy, as well as the performance of these systems. Here, we demonstrate a method for synthesizing heterostructures comprising magnetic intercalation compounds of transition metal dichalcogenides (TMDs), through directed topotactic reaction of the TMD with a metal oxide. The mechanism of the intercalation reaction enables thermally initiated intercalation of the TMD from lithographically patterned oxide films, giving access to a new family of multi-component magnetic architectures through the combination of deterministic van der Waals assembly and directed intercalation chemistry. △ Less

Submitted 21 June, 2024; originally announced June 2024.

Good plasmons in a bad metal

Authors: Francesco L. Ruta, Yinming Shao, Swagata Acharya, Anqi Mu, Na Hyun Jo, Sae Hee Ryu, Daria Balatsky, Dimitar Pashov, Brian S. Y. Kim, Mikhail I. Katsnelson, James G. Analytis, Eli Rotenberg, Andrew J. Millis, Mark van Schilfgaarde, D. N. Basov

Abstract: Correlated materials may exhibit unusually high resistivity increasing linearly in temperature, breaking through the Mott-Ioffe-Regel bound, above which coherent quasiparticles are destroyed. The fate of collective charge excitations, or plasmons, in these systems is a subject of debate. Several studies suggest plasmons are overdamped while others detect unrenormalized plasmons. Here, we present d… ▽ More Correlated materials may exhibit unusually high resistivity increasing linearly in temperature, breaking through the Mott-Ioffe-Regel bound, above which coherent quasiparticles are destroyed. The fate of collective charge excitations, or plasmons, in these systems is a subject of debate. Several studies suggest plasmons are overdamped while others detect unrenormalized plasmons. Here, we present direct optical images of low-loss hyperbolic plasmon polaritons (HPPs) in the correlated van der Waals metal MoOCl2. HPPs are plasmon-photon modes that waveguide through extremely anisotropic media and are remarkably long-lived in MoOCl2. Many-body theory supported by photoemission results reveals that MoOCl2 is in an orbital-selective and highly incoherent Peierls phase. Different orbitals acquire markedly different bonding-antibonding character, producing a highly-anisotropic, isolated Fermi surface. The Fermi surface is further reconstructed and made partly incoherent by electronic interactions, renormalizing the plasma frequency. HPPs remain long-lived in spite of this, allowing us to uncover previously unseen imprints of electronic correlations on plasmonic collective modes. △ Less

Submitted 9 June, 2024; originally announced June 2024.

Comments: 32 pages, 16 figures

On the feasibility of quantum teleportation protocols implemented with Silicon devices

Authors: Junghee Ryu, Hoon Ryu

Abstract: With recent experimental advancements demonstrating high-fidelity universal logic gates and basic programmability, Silicon-based spin quantum bit (qubit) have emerged as promising candidates for scalable quantum computing. However, implementation of more complex quantum information protocols with many qubits still remains a critical challenge for realization of practical programmability in Silicon… ▽ More With recent experimental advancements demonstrating high-fidelity universal logic gates and basic programmability, Silicon-based spin quantum bit (qubit) have emerged as promising candidates for scalable quantum computing. However, implementation of more complex quantum information protocols with many qubits still remains a critical challenge for realization of practical programmability in Silicon devices. In this study, we present a computational investigation of entanglement-based quantum information applications implemented on an electrically defined quantum dot structure in Silicon. Using in-house multi-scale simulations based on tight-binding calculations augmented with bulk physics, we model a five quantum dot system that can create up to five electron spin qubits, and discuss details of control engineering needed to implement single-qubit rotations and two-qubit logic operations in a programmable manner. Using these elementary operations, then, we design a five-qubit quantum teleportation protocol and computationally verify its end-to-end operation including a simple but clear analysis on how the designed circuit can be affected by charge noise. With engineering details that are not well uncovered by experiments, our results demonstrate the advanced programmability of Silicon quantum dot systems, delivering the practical guidelines for potential designs of quantum information processes based on electrically defined Silicon quantum dot structures. △ Less

Submitted 4 October, 2024; v1 submitted 28 March, 2024; originally announced March 2024.

Comments: 13 pages, 7 figures

Electronic structure of above-room-temperature van der Waals ferromagnet Fe$_3$GaTe$_2$

Authors: Ji-Eun Lee, Shaohua Yan, Sehoon Oh, Jinwoong Hwang, Jonathan D. Denlinger, Choongyu Hwang, Hechang Lei, Sung-Kwan Mo, Se Young Park, Hyejin Ryu

Abstract: Fe$_3$GaTe$_2$, a recently discovered van der Waals ferromagnet, demonstrates intrinsic ferromagnetism above room temperature, necessitating a comprehensive investigation of the microscopic origins of its high Curie temperature ($\textit{T}$$_C$). In this study, we reveal the electronic structure of Fe$_3$GaTe$_2$ in its ferromagnetic ground state using angle-resolved photoemission spectroscopy an… ▽ More Fe$_3$GaTe$_2$, a recently discovered van der Waals ferromagnet, demonstrates intrinsic ferromagnetism above room temperature, necessitating a comprehensive investigation of the microscopic origins of its high Curie temperature ($\textit{T}$$_C$). In this study, we reveal the electronic structure of Fe$_3$GaTe$_2$ in its ferromagnetic ground state using angle-resolved photoemission spectroscopy and density functional theory calculations. Our results establish a consistent correspondence between the measured band structure and theoretical calculations, underscoring the significant contributions of the Heisenberg exchange interaction ($\textit{J}$$_{ex}$) and magnetic anisotropy energy to the development of the high-$\textit{T}$$_C$ ferromagnetic ordering in Fe$_3$GaTe$_2$. Intriguingly, we observe substantial modifications to these crucial driving factors through doping, which we attribute to alterations in multiple spin-splitting bands near the Fermi level. These findings provide valuable insights into the underlying electronic structure and its correlation with the emergence of high-$\textit{T}$$_C$ ferromagnetic ordering in Fe$_3$GaTe$_2$. △ Less

Submitted 14 March, 2024; originally announced March 2024.

Comments: 25 pages, 4 figures

Journal ref: Nano Lett. 23 (2023) 11526-11532

Quantum-centric Supercomputing for Materials Science: A Perspective on Challenges and Future Directions

Authors: Yuri Alexeev, Maximilian Amsler, Paul Baity, Marco Antonio Barroca, Sanzio Bassini, Torey Battelle, Daan Camps, David Casanova, Young Jai Choi, Frederic T. Chong, Charles Chung, Chris Codella, Antonio D. Corcoles, James Cruise, Alberto Di Meglio, Jonathan Dubois, Ivan Duran, Thomas Eckl, Sophia Economou, Stephan Eidenbenz, Bruce Elmegreen, Clyde Fare, Ismael Faro, Cristina Sanz Fernández, Rodrigo Neumann Barros Ferreira , et al. (102 additional authors not shown)

Abstract: Computational models are an essential tool for the design, characterization, and discovery of novel materials. Hard computational tasks in materials science stretch the limits of existing high-performance supercomputing centers, consuming much of their simulation, analysis, and data resources. Quantum computing, on the other hand, is an emerging technology with the potential to accelerate many of… ▽ More Computational models are an essential tool for the design, characterization, and discovery of novel materials. Hard computational tasks in materials science stretch the limits of existing high-performance supercomputing centers, consuming much of their simulation, analysis, and data resources. Quantum computing, on the other hand, is an emerging technology with the potential to accelerate many of the computational tasks needed for materials science. In order to do that, the quantum technology must interact with conventional high-performance computing in several ways: approximate results validation, identification of hard problems, and synergies in quantum-centric supercomputing. In this paper, we provide a perspective on how quantum-centric supercomputing can help address critical computational problems in materials science, the challenges to face in order to solve representative use cases, and new suggested directions. △ Less

Submitted 19 September, 2024; v1 submitted 14 December, 2023; originally announced December 2023.

Comments: 65 pages, 15 figures; comments welcome

Journal ref: Future Generation Computer Systems, Volume 160, November 2024, Pages 666-710

Nearly-room-temperature ferromagnetism and tunable anomalous Hall effect in atomically thin Fe4CoGeTe2

Authors: Shaohua Yan, Hui-Hui He, Yang Fu, Ning-Ning Zhao, Shangjie Tian, Qiangwei Yin, Fanyu Meng, Xinyu Cao, Le Wang, Shanshan Chen, Ki-Hoon Son, Jun Woo Choi, Hyejin Ryu, Shouguo Wang, Xiao Zhang, Kai Liu, Hechang Lei

Abstract: Itinerant ferromagnetism at room temperature is a key ingredient for spin transport and manipulation. Here, we report the realization of nearly-room-temperature itinerant ferromagnetism in Co doped Fe5GeTe2 thin flakes. The ferromagnetic transition temperature TC (~ 323 K - 337 K) is almost unchanged when thickness is down to 12 nm and is still about 284 K at 2 nm (bilayer thickness). Theoretical… ▽ More Itinerant ferromagnetism at room temperature is a key ingredient for spin transport and manipulation. Here, we report the realization of nearly-room-temperature itinerant ferromagnetism in Co doped Fe5GeTe2 thin flakes. The ferromagnetic transition temperature TC (~ 323 K - 337 K) is almost unchanged when thickness is down to 12 nm and is still about 284 K at 2 nm (bilayer thickness). Theoretical calculations further indicate that the ferromagnetism persists in monolayer Fe4CoGeTe2. In addition to the robust ferromagnetism down to the ultrathin limit, Fe4CoGeTe2 exhibits an unusual temperature- and thickness-dependent intrinsic anomalous Hall effect. We propose that it could be ascribed to the dependence of band structure on thickness that changes the Berry curvature near the Fermi energy level subtly. The nearly-room-temperature ferromagnetism and tunable anomalous Hall effect in atomically thin Fe4CoGeTe2 provide opportunities to understand the exotic transport properties of two-dimensional van der Waals magnetic materials and explore their potential applications in spintronics. △ Less

Submitted 22 December, 2025; v1 submitted 24 August, 2023; originally announced August 2023.

Comments: 9 pages, 4 figures, 1 table

Journal ref: Nanoscale 16, 1406 (2024)

Low-Thermal-Budget Ferroelectric Field-Effect Transistors Based on CuInP2S6 and InZnO

Authors: Hojoon Ryu, Junzhe Kang, Minseong Park, Byungjoon Bae, Zijing Zhao, Shaloo Rakheja, Kyusang Lee, Wenjuan Zhu

Abstract: In this paper, we demonstrate low-thermal-budget ferroelectric field-effect transistors (FeFETs) based on two-dimensional ferroelectric CuInP2S6 (CIPS) and oxide semiconductor InZnO (IZO). The CIPS/IZO FeFETs exhibit non-volatile memory windows of ~1 V, low off-state drain currents, and high carrier mobilities. The ferroelectric CIPS layer serves a dual purpose by providing electrostatic doping in… ▽ More In this paper, we demonstrate low-thermal-budget ferroelectric field-effect transistors (FeFETs) based on two-dimensional ferroelectric CuInP2S6 (CIPS) and oxide semiconductor InZnO (IZO). The CIPS/IZO FeFETs exhibit non-volatile memory windows of ~1 V, low off-state drain currents, and high carrier mobilities. The ferroelectric CIPS layer serves a dual purpose by providing electrostatic doping in IZO and acting as a passivation layer for the IZO channel. We also investigate the CIPS/IZO FeFETs as artificial synaptic devices for neural networks. The CIPS/IZO synapse demonstrates a sizeable dynamic ratio (125) and maintains stable multi-level states. Neural networks based on CIPS/IZO FeFETs achieve an accuracy rate of over 80% in recognizing MNIST handwritten digits. These ferroelectric transistors can be vertically stacked on silicon CMOS with a low thermal budget, offering broad applications in CMOS+X technologies and energy-efficient 3D neural networks. △ Less

Submitted 19 July, 2023; originally announced July 2023.

Content Addressable Memories and Transformable Logic Circuits Based on Ferroelectric Reconfigurable Transistors for In-Memory Computing

Authors: Zijing Zhao, Junzhe Kang, Ashwin Tunga, Hojoon Ryu, Ankit Shukla, Shaloo Rakheja, Wenjuan Zhu

Abstract: As a promising alternative to the Von Neumann architecture, in-memory computing holds the promise of delivering high computing capacity while consuming low power. Content addressable memory (CAM) can implement pattern matching and distance measurement in memory with massive parallelism, making them highly desirable for data-intensive applications. In this paper, we propose and demonstrate a novel… ▽ More As a promising alternative to the Von Neumann architecture, in-memory computing holds the promise of delivering high computing capacity while consuming low power. Content addressable memory (CAM) can implement pattern matching and distance measurement in memory with massive parallelism, making them highly desirable for data-intensive applications. In this paper, we propose and demonstrate a novel 1-transistor-per-bit CAM based on the ferroelectric reconfigurable transistor. By exploiting the switchable polarity of the ferroelectric reconfigurable transistor, XOR/XNOR-like matching operation in CAM can be realized in a single transistor. By eliminating the need for the complementary circuit, these non-volatile CAMs based on reconfigurable transistors can offer a significant improvement in area and energy efficiency compared to conventional CAMs. NAND- and NOR-arrays of CAMs are also demonstrated, which enable multi-bit matching in a single reading operation. In addition, the NOR array of CAM cells effectively measures the Hamming distance between the input query and stored entries. Furthermore, utilizing the switchable polarity of these ferroelectric Schottky barrier transistors, we demonstrate reconfigurable logic gates with NAND/NOR dual functions, whose input-output mapping can be transformed in real-time without changing the layout. These reconfigurable circuits will serve as important building blocks for high-density data-stream processors and reconfigurable Application-Specific Integrated Circuits (r-ASICs). The CAMs and transformable logic gates based on ferroelectric reconfigurable transistors will have broad applications in data-intensive applications from image processing to machine learning and artificial intelligence. △ Less

Submitted 7 July, 2023; originally announced July 2023.

Comparative Electronic Structures of the Chiral Helimagnets Cr1/3NbS2 and Cr1/3TaS2

Authors: Lilia S. Xie, Oscar Gonzalez, Kejun Li, Matteo Michiardi, Sergey Gorovikov, Sae Hee Ryu, Shannon S. Fender, Marta Zonno, Na Hyun Jo, Sergey Zhdanovich, Chris Jozwiak, Aaron Bostwick, Samra Husremovic, Matthew P. Erodici, Cameron Mollazadeh, Andrea Damascelli, Eli Rotenberg, Yuan Ping, D. Kwabena Bediako

Abstract: Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying… ▽ More Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying the relative strengths of the microscopic mechanisms giving rise to exotic spin textures. Here, we carry out a comparative study of the electronic structures of Cr1/3NbS2 and Cr1/3TaS2 using angle-resolved photoemission spectroscopy and density functional theory. We show that bands in Cr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2 and connect this result to bonding and orbital overlap in these materials. We also unambiguously distinguish exchange splitting from surface termination effects by studying the dependence of their photoemission spectra on polarization, temperature, and beam size. We find strong evidence that hybridization between intercalant and host lattice electronic states mediates the magnetic exchange interactions in these materials, suggesting that band engineering is a route toward tuning their spin textures. Overall, these results underscore how the modular nature of intercalated transition metal dichalcogenides translates variation in composition and electronic structure to complex magnetism. △ Less

Submitted 22 May, 2023; v1 submitted 15 May, 2023; originally announced May 2023.

Comments: 46 pages, 18 figures, 5 tables

Journal ref: Chemistry of Materials, 2023, 35, 7239-7251

magnetoARPES: Angle Resolved Photoemission Spectroscopy with Magnetic Field Control

Authors: Sae Hee Ryu, Garett Reichenbach, Chris M. Jozwiak, Aaron Bostwick, Peter Richter, Thomas Seyller, Eli Rotenberg

Abstract: Angle-Resolved Photoemission Spectroscopy (ARPES) is a premier technique for understanding the electronic excitations in conductive, crystalline matter, in which the induced photocurrent is collected and dispersed in energy and angle of emission to reveal the energy- and momentum-dependent single particle spectral function $A(\mathbf{k},ω)$. So far, ARPES in a magnetic field has been precluded due… ▽ More Angle-Resolved Photoemission Spectroscopy (ARPES) is a premier technique for understanding the electronic excitations in conductive, crystalline matter, in which the induced photocurrent is collected and dispersed in energy and angle of emission to reveal the energy- and momentum-dependent single particle spectral function $A(\mathbf{k},ω)$. So far, ARPES in a magnetic field has been precluded due to the need to preserve the electron paths between the sample and detector. In this paper we report progress towards "magnetoARPES", a variant of ARPES that can be conducted in a magnetic field. It is achieved by applying a microscopic probe beam ($\lesssim$ 10 $μ$m ) to a thinned sample mounted upon a special sample holder that generates magnetic field confined to a thin layer near the sample surface. In this geometry we could produce ARPES in magnetic fields up to around $\pm$ 100 mT. The magnetic fields can be varied from purely in-plane to nearly purely out-of-plane, by scanning the probe beam across different parts of the device. We present experimental and simulated data for graphene to explore the aberrations induced by the magnetic field. These results demonstrate the viability of the magnetoARPES technique for exploring symmetry breaking effects in weak magnetic fields. △ Less

Submitted 14 April, 2023; originally announced April 2023.

Comments: 21 pages, 6 figures

On the effects of strain, defects, and interactions on the topological properties of HfTe5

Authors: Na Hyun Jo, Omar A. Ashour, Zhixue Shu, Chris Jozwiak, Aaron Bostwick, Sae Hee Ryu, Kai Sun, Tai Kong, Sinead M. Griffin, Eli Rotenberg

Abstract: Topological insulators are characterized by spin-momentum-locked massless surface states which are robust under various perturbations. Manipulating such surface states is a topic of vigorous research, as a possible route for the realization of emergent many-body physics in topological systems. Thus far, time-reversal symmetry breaking via Coulomb and magnetic perturbations has been a dominant appr… ▽ More Topological insulators are characterized by spin-momentum-locked massless surface states which are robust under various perturbations. Manipulating such surface states is a topic of vigorous research, as a possible route for the realization of emergent many-body physics in topological systems. Thus far, time-reversal symmetry breaking via Coulomb and magnetic perturbations has been a dominant approach for the tuning of topological states. However, the effect of the structural degrees of freedom on quasi-particle dynamics in topological materials remains elusive. In this work, we demonstrate a transition in HfTe5 between distinct topological phases as a function of either Te vacancy concentration or applied strain; these phases are characterized theoretically as a transition from strong to weak topological insulator and experimentally by a transition from sharp surface states and Dirac crossing to a Fermi-liquid-like quasiparticle state in which these surface-localized features are heavily suppressed. Although vacancies can result in various consequences such as scattering, doping, and structural distortions, we show that changes in the lattice constants play the foremost role in determining the electronic structure, self-energy, and topological states of HfTe5. Our results demonstrate the possibility of using both defect chemistry and strain as control parameters for topological phase transitions and associated many-body physics. △ Less

Submitted 19 March, 2023; originally announced March 2023.

Journal ref: Phys. Rev. B 109, 235122 (2024)

In situ Imaging of an Anisotropic Layer-by-Layer Phase Transition in Few-Layer MoTe2

Authors: Chia-Hao Lee, Huije Ryu, Gillian Nolan, Yichao Zhang, Yangjin Lee, Siwon Oh, Hyeonsik Cheong, Kenji Watanabe, Takashi Taniguchi, Kwanpyo Kim, Gwan-Hyoung Lee, Pinshane Y. Huang

Abstract: Understanding the phase transition mechanisms in two-dimensional (2D) materials is a key to precisely tailor their properties at the nanoscale. Molybdenum ditelluride (MoTe2) exhibits multiple phases at room temperature, making it a promising candidate for phase-change applications. Here, we fabricate lateral 2H-Td interfaces with laser irradiation and probe their phase transitions from micro- to… ▽ More Understanding the phase transition mechanisms in two-dimensional (2D) materials is a key to precisely tailor their properties at the nanoscale. Molybdenum ditelluride (MoTe2) exhibits multiple phases at room temperature, making it a promising candidate for phase-change applications. Here, we fabricate lateral 2H-Td interfaces with laser irradiation and probe their phase transitions from micro- to atomic scales with in situ heating in the transmission electron microscope (TEM). By encapsulating the MoTe2 with graphene protection layers, we create an in situ reaction cell compatible with atomic resolution imaging. We find that the Td-to-2H phase transition initiates at phase boundaries at low temperatures (200-225 degree C) and propagates anisotropically along the b-axis in a layer-by-layer fashion. We also demonstrate a fully reversible 2H-Td-2H phase transition cycle, which generates a coherent 2H lattice containing inversion domain boundaries. Our results provide insights on fabricating 2D hetero-phase devices with atomically sharp and coherent interfaces. △ Less

Submitted 6 January, 2023; originally announced January 2023.

Comments: 38 pages, 5 figures, 9 supplementary figures, and supplementary information

A novel $\sqrt{19}\times\sqrt{19}$ superstructure in epitaxially grown 1T-TaTe$_2$

Authors: Jinwoong Hwang, Yeongrok Jin, Canxun Zhang, Tiancong Zhu, Kyoo Kim, Yong Zhong, Ji-Eun Lee, Zongqi Shen, Yi Chen, Wei Ruan, Hyejin Ryu, Choongyu Hwang, Jaekwang Lee, Michael F. Crommie, Sung-Kwan Mo, Zhi-Xun Shen

Abstract: The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in two-dimensional materials. We report a novel $\sqrt{19}\times\sqrt{19}$ charge order in few-layer thick 1T-TaTe$_2$ transition metal dichalcogenide films grown by molecular beam epitaxy, which has not been realized. Our photoemission and scanning probe me… ▽ More The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in two-dimensional materials. We report a novel $\sqrt{19}\times\sqrt{19}$ charge order in few-layer thick 1T-TaTe$_2$ transition metal dichalcogenide films grown by molecular beam epitaxy, which has not been realized. Our photoemission and scanning probe measurements demonstrate that monolayer 1T-TaTe$_2$ exhibits a variety of metastable charge density wave orders, including the $\sqrt{19}\times\sqrt{19}$ superstructure, which can be selectively stabilized by controlling the post-growth annealing temperature. Moreover, we find that only the $\sqrt{19}\times\sqrt{19}$ order persists in 1T-TaTe$_2$ films thicker than a monolayer, up to 8 layers. Our findings identify the previously unrealized novel electronic order in a much-studied transition metal dichalcogenide and provide a viable route to control it within the epitaxial growth process. △ Less

Submitted 4 October, 2022; originally announced October 2022.

Journal ref: Advanced materials 34, 2204579 (2022)

Exploring entanglement resource in Si quantum dot systems with operational quasiprobability approach

Authors: Junghee Ryu, Hoon Ryu

Abstract: We characterize the quantum entanglement of the realistic two-qubit signals that are sensitive to charge noises. Our working example is the time response generated from a silicon double quantum dot (DQD) platform, where a single-qubit rotation and a two-qubit controlled-NOT operation are conducted sequentially in time to generate arbitrary entangled states. In order to characterize the entanglemen… ▽ More We characterize the quantum entanglement of the realistic two-qubit signals that are sensitive to charge noises. Our working example is the time response generated from a silicon double quantum dot (DQD) platform, where a single-qubit rotation and a two-qubit controlled-NOT operation are conducted sequentially in time to generate arbitrary entangled states. In order to characterize the entanglement of two-qubit states, we employ the marginal operational quasiprobability (OQ) approach that allows negative values of the probability function if a given state is entangled. While the charge noise, which is omnipresent in semiconductor devices, severely affects logic operations implemented in the DQD platform, causing huge degradation in fidelity of unitary operations as well as resulting two-qubit states, the pattern in the OQ-driven entanglement strength turns out to be quite invariant, indicating that the resource of quantum entanglement is not significantly broken though the physical system is exposed to noise-driven fluctuations in exchange interaction between quantum dots. △ Less

Submitted 27 September, 2022; v1 submitted 30 March, 2022; originally announced March 2022.

Comments: 11 pages, 5 figures

Journal ref: Quantum 6, 827 (2022)

Evidence for a spinon Kondo effect in cobalt atoms on single-layer 1T-TaSe$_2$

Authors: Yi Chen, Wen-Yu He, Wei Ruan, Jinwoong Hwang, Shujie Tang, Ryan L. Lee, Meng Wu, Tiancong Zhu, Canxun Zhang, Hyejin Ryu, Feng Wang, Steven G. Louie, Zhi-Xun Shen, Sung-Kwan Mo, Patrick A. Lee, Michael F. Crommie

Abstract: Quantum spin liquids (QSLs) are highly entangled, disordered magnetic states that arise in frustrated Mott insulators and host exotic fractional excitations such as spinons and chargons. Despite being charge insulators some QSLs are predicted to exhibit gapless itinerant spinons that yield metallic behavior in the spin channel. We have deposited isolated magnetic atoms onto single-layer (SL) 1T-Ta… ▽ More Quantum spin liquids (QSLs) are highly entangled, disordered magnetic states that arise in frustrated Mott insulators and host exotic fractional excitations such as spinons and chargons. Despite being charge insulators some QSLs are predicted to exhibit gapless itinerant spinons that yield metallic behavior in the spin channel. We have deposited isolated magnetic atoms onto single-layer (SL) 1T-TaSe$_2$, a gapless QSL candidate, to experimentally probe how itinerant spinons couple to impurity spin centers. Using scanning tunneling spectroscopy we observe the emergence of new, impurity-induced resonance peaks at the 1T-TaSe$_2$ Hubbard band edges when cobalt adatoms are positioned to have maximal spatial overlap with the Hubbard band charge distribution. These resonance peaks disappear when the spatial overlap is reduced or when the magnetic impurities are replaced with non-magnetic impurities. Theoretical simulations using a modified Anderson impurity model integrated with a gapless quantum spin liquid show that these resonance peaks are consistent with a Kondo resonance induced by spinons combined with spinon-chargon binding effects that arise due to QSL gauge-field fluctuations. △ Less

Submitted 15 February, 2022; originally announced February 2022.

Journal ref: Nature Physics 18, 1335 (2022)

Devitalizing noise-driven instability of entangling logic in silicon devices with bias controls

Authors: Hoon Ryu, Ji-Hoon Kang

Abstract: The quality of quantum bits (qubits) in silicon is highly vulnerable to charge noise that is omni-present in semiconductor devices and is in principle hard to be suppressed. For a realistically sized quantum dot system based on a silicon-germanium heterostructure whose confinement is manipulated with electrical biases imposed on top electrodes, we computationally explore the noise-robustness of 2-… ▽ More The quality of quantum bits (qubits) in silicon is highly vulnerable to charge noise that is omni-present in semiconductor devices and is in principle hard to be suppressed. For a realistically sized quantum dot system based on a silicon-germanium heterostructure whose confinement is manipulated with electrical biases imposed on top electrodes, we computationally explore the noise-robustness of 2-qubit entangling operations with a focus on the controlled-X (CNOT) logic that is essential for designs of gate-based universal quantum logic circuits. With device simulations based on the physics of bulk semiconductors augmented with electronic structure calculations, we not only quantify the degradation in fidelity of single-step CNOT operations with respect to the strength of charge noise, but also discuss a strategy of device engineering that can significantly enhance noise-robustness of CNOT operations with almost no sacrifice of speed compared to the single-step case. Details of device designs and controls that this work presents can establish a rare but practical guideline for potential efforts to secure silicon-based quantum processors using an electrode-driven quantum dot platform. △ Less

Submitted 24 March, 2022; v1 submitted 9 February, 2022; originally announced February 2022.

Comments: 23 pages, 6 figures

Journal ref: Scientific Reports 12, 15200 (2022)

Charge order landscape and competition with superconductivity in kagome metals

Authors: Mingu Kang, Shiang Fang, Jonggyu Yoo, Brenden R. Ortiz, Yuzki Oey, Jonghyeok Choi, Sae Hee Ryu, Jimin Kim, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Efthimios Kaxiras, Joseph G. Checkelsky, Stephen D. Wilson, Jae-Hoon Park, Riccardo Comin

Abstract: In kagome metals AV3Sb5 (A = K, Rb, Cs), three-dimensional charge order (3D-CO) is the primary instability that sets the stage for other collective orders to emerge, including unidirectional stripe order, orbital flux order, electronic nematicity, and superconductivity. Here, we use high-resolution angle-resolved photoemission spectroscopy to determine the microscopic structure of three-dimensiona… ▽ More In kagome metals AV3Sb5 (A = K, Rb, Cs), three-dimensional charge order (3D-CO) is the primary instability that sets the stage for other collective orders to emerge, including unidirectional stripe order, orbital flux order, electronic nematicity, and superconductivity. Here, we use high-resolution angle-resolved photoemission spectroscopy to determine the microscopic structure of three-dimensional charge order (3D-CO) in AV3Sb5 and its interplay with superconductivity. Our approach is based on identifying an unusual splitting of kagome bands induced by 3D-CO, which provides a sensitive way to refine the spatial charge patterns in neighboring kagome planes. We found a marked dependence of the 3D-CO structure on composition and doping. The observed difference between CsV3Sb5 and the other compounds potentially underpins the double-dome superconductivity in CsV3(Sb,Sn)5 and the suppression of Tc in KV3Sb5 and RbV3Sb5. Our results provide fresh insights into the rich phase diagram of AV3Sb5. △ Less

Submitted 22 December, 2022; v1 submitted 3 February, 2022; originally announced February 2022.

Comments: 20 pages, 5 figures

Journal ref: Nature Materials (2022)

Direct observation of orbital driven strong interlayer coupling in puckered two-dimensional PdSe2

Authors: Jung Hyun Ryu, Jeong-Gyu Kim, Bongjae Kim, Kyoo Kim, Sooran Kim, Byeong-Gyu Park, Younghak Kim, Kyung-Tae Ko, Kimoon Lee

Abstract: Interlayer coupling between individual unit layers has played a critical role for layer-dependent properties in two-dimensional (2D) materials. While recent studies have revealed the significant degrees of interlayer interactions, the overall electronic structure of the 2D material has been mostly addressed by the intralayer interactions. Here, we report the direct observation of a highly dispersi… ▽ More Interlayer coupling between individual unit layers has played a critical role for layer-dependent properties in two-dimensional (2D) materials. While recent studies have revealed the significant degrees of interlayer interactions, the overall electronic structure of the 2D material has been mostly addressed by the intralayer interactions. Here, we report the direct observation of a highly dispersive single electronic band along the interlayer direction in puckered 2D PdSe2 as an experimental hallmark of strong interlayer couplings. Remarkably large band dispersion along kz-direction near Fermi level, which is even wider than the in-plane one, is observed by the angle-resolved photoemission spectroscopy measurement. Employing the X-ray absorption spectroscopy and density functional theory calculations, we reveal that the strong interlayer coupling in 2D PdSe2 originates from the unique directional bonding of Pd d orbitals associated with unexpected Pd 4d9 configuration, which consequently gives rise to the strong layer-dependency of the band gap. △ Less

Submitted 19 July, 2021; originally announced July 2021.

Journal ref: Small, 2022, Online Published

Twofold van Hove singularity and origin of charge order in topological kagome superconductor CsV3Sb5

Authors: Mingu Kang, Shiang Fang, Jeong-Kyu Kim, Brenden R. Ortiz, Sae Hee Ryu, Jimin Kim, Jonggyu Yoo, Giorgio Sangiovanni, Domenico Di Sante, Byeong-Gyu Park, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Efthimios Kaxiras, Stephen D. Wilson, Jae-Hoon Park, Riccardo Comin

Abstract: The layered vanadium antimonides AV3Sb5 (A = K, Rb, Cs) are a recently discovered family of topological kagome metals with a rich phenomenology of strongly correlated electronic phases including charge order and superconductivity. Understanding how the singularities inherent to the kagome electronic structure are linked to the observed many-body phases is a topic of great interest and relevance. H… ▽ More The layered vanadium antimonides AV3Sb5 (A = K, Rb, Cs) are a recently discovered family of topological kagome metals with a rich phenomenology of strongly correlated electronic phases including charge order and superconductivity. Understanding how the singularities inherent to the kagome electronic structure are linked to the observed many-body phases is a topic of great interest and relevance. Here, we combine angle-resolved photoemission spectroscopy and density functional theory to reveal multiple kagome-derived van Hove singularities (vHs) coexisting near the Fermi level of CsV3Sb5 and analyze their contribution to electronic symmetry breaking. Intriguingly, the vHs in CsV3Sb5 have two distinct flavors - p-type and m-type - which originate from their pure and mixed sublattice characters, respectively. This twofold vHs is unique property of the kagome lattice, and its flavor critically determines the pairing symmetry and ground states emerging in AV3Sb5 series. We establish that, among the multiple vHs in CsV3Sb5, the m-type vHs of the dxz/dyz kagome band and the p-type vHs of the dxy/dx2-y2 kagome band cross the Fermi level to set the stage for electronic symmetry breaking. The former band exhibits pronounced Fermi surface nesting, while the latter contributes via higher-order vHs. Our work reveals the essential role of kagome-derived vHs for the collective phenomena realized in the AV3Sb5 family, paving the way to a deeper understanding of strongly correlated topological kagome systems. △ Less

Submitted 5 November, 2021; v1 submitted 4 May, 2021; originally announced May 2021.

Comments: Submitted to Nature Physics on May 28th, 2021. A revised version will appear in Nature Physics

Single-Crystalline Metallic Films Induced by van der Waals Epitaxy on Black Phosphorus

Authors: Yangjin Lee, Han-gyu Kim, Tae Keun Yun, Jong Chan Kim, Sol Lee, Sung Jin Yang, Myeongjin Jang, Donggyu Kim, Huije Ryu, Gwan-Hyoung Lee, Seongil Im, Hu Young Jeong, Hyoung Joon Choi, Kwanpyo Kim

Abstract: The properties of metal-semiconductor junctions are often unpredictable because of non-ideal interfacial structures, such as interfacial defects or chemical reactions introduced at junctions. Black phosphorus (BP), an elemental two-dimensional (2D) semiconducting crystal, possesses the puckered atomic structure with high chemical reactivity, and the establishment of a realistic atomic-scale pictur… ▽ More The properties of metal-semiconductor junctions are often unpredictable because of non-ideal interfacial structures, such as interfacial defects or chemical reactions introduced at junctions. Black phosphorus (BP), an elemental two-dimensional (2D) semiconducting crystal, possesses the puckered atomic structure with high chemical reactivity, and the establishment of a realistic atomic-scale picture of BP's interface toward metallic contact has remained elusive. Here we examine the interfacial structures and properties of physically-deposited metals of various kinds on BP. We find that Au, Ag, and Bi form single-crystalline films with (110) orientation through guided van der Waals epitaxy. Transmission electron microscopy and X-ray photoelectron spectroscopy confirm that atomically sharp van der Waals metal-BP interfaces forms with exceptional rotational alignment. Under a weak metal-BP interaction regime, the BP's puckered structure play an essential role in the adatom assembly process and can lead to the formation of a single crystal, which is supported by our theoretical analysis and calculations. The experimental survey also demonstrates that the BP-metal junctions can exhibit various types of interfacial structures depending on metals, such as the formation of polycrystalline microstructure or metal phosphides. This study provides a guideline for obtaining a realistic view on metal-2D semiconductor interfacial structures, especially for atomically puckered 2D crystals. △ Less

Submitted 3 May, 2021; originally announced May 2021.

Comments: 27 pages, 5 figures

Journal ref: Chemistry of Materials, 2021

Observation of Kondo hybridization with an orbital-selective Mott phase in 4d Ca2-xSrxRuO4

Authors: Minsoo Kim, Junyoung Kwon, Choong H. Kim, Younsik Kim, Daun Chung, Hanyoung Ryu, Jongkeun Jung, Beom Seo Kim, Dongjoon Song, Jonathan D. Denlinger, Moonsup Han, Yoshiyuki Yoshida, Takashi Mizokawa, Wonshik Kyung, Changyoung Kim

Abstract: The heavy fermion state with Kondo-hybridization (KH), usually manifested in f-electron systems with lanthanide or actinide elements, was recently discovered in several 3d transition metal compounds without f-electrons. However, KH has not yet been observed in 4d/5d transition metal compounds, since more extended 4d/5d orbitals do not usually form flat bands that supply localized electrons appropr… ▽ More The heavy fermion state with Kondo-hybridization (KH), usually manifested in f-electron systems with lanthanide or actinide elements, was recently discovered in several 3d transition metal compounds without f-electrons. However, KH has not yet been observed in 4d/5d transition metal compounds, since more extended 4d/5d orbitals do not usually form flat bands that supply localized electrons appropriate for Kondo pairing. Here, we report a doping- and temperature-dependent angle-resolved photoemission study on 4d Ca2-xSrxRuO4, which shows the signature of KH. We observed a spectral weight transfer in the γ-band, reminiscent of an orbital-selective Mott phase (OSMP). The Mott localized γ-band induces KH with the itinerant \b{eta}-band, resulting in spectral weight suppression around the Fermi level. Our work is the first to demonstrate the evolution of the OSMP with possible KH among 4d electrons, and thereby expands the material boundary of Kondo physics to 4d multi-orbital systems. △ Less

Submitted 19 February, 2021; originally announced February 2021.

Tunable Kondo resonance at a pristine two-dimensional Dirac semimetal on a Kondo insulator

Authors: Jinwoong Hwang, Seungseok Lee, Ji-Eun Lee, Minhee Kang, Hyejin Ryu, Hyun-Jeong Joo, Jonathan Denlinger, Jae-Hoon Park, Choongyu Hwang

Abstract: Proximity of two different materials leads to an intricate coupling of quasiparticles so that an unprecedented electronic state is often realized at the interface. Here, we demonstrate a resonance-type many-body ground state in graphene, a non-magnetic two-dimensional Dirac semimetal, when grown on SmB6, a Kondo insulator, via thermal decomposition of fullerene molecules. This ground state is typi… ▽ More Proximity of two different materials leads to an intricate coupling of quasiparticles so that an unprecedented electronic state is often realized at the interface. Here, we demonstrate a resonance-type many-body ground state in graphene, a non-magnetic two-dimensional Dirac semimetal, when grown on SmB6, a Kondo insulator, via thermal decomposition of fullerene molecules. This ground state is typically observed in three-dimensional magnetic materials with correlated electrons. Above the characteristic Kondo temperature of the substrate, the electron band structure of pristine graphene remains almost intact. As temperature decreases, however, the Dirac fermions of graphene become hybridized with the Sm 4f states. Remarkable enhancement of the hybridization and Kondo resonance is observed with further cooling and increasing charge carrier density of graphene, evidencing the Kondo screening of the Sm 4f local magnetic moment by the conduction electrons of graphene at the interface. These findings manifest the realization of the Kondo effect in graphene by the proximity of SmB6 that is tuned by temperature and charge carrier density of graphene. △ Less

Submitted 11 February, 2021; originally announced February 2021.

Comments: 4 figures

Journal ref: Nano Lett. 20, 7973 (2020)

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

Authors: Shaobo Liu, Jie Yuan, Soonsang Huh, Hanyoung Ryu, Mingwei Ma, Wei Hu, Dong Li, Sheng Ma, Shunli Ni, Peipei Shen, Kui Jin, Li Yu, Changyoung Kim, Fang Zhou, Xiaoli Dong, Zhongxian Zhao

Abstract: 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 tetra… ▽ More 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. △ Less

Submitted 28 September, 2020; originally announced September 2020.

Comments: 18 pages, 5 figures

Imaging spinon density modulations in a 2D quantum spin liquid

Authors: Wei Ruan, Yi Chen, Shujie Tang, Jinwoong Hwang, Hsin-Zon Tsai, Ryan Lee, Meng Wu, Hyejin Ryu, Salman Kahn, Franklin Liou, Caihong Jia, Andrew Aikawa, Choongyu Hwang, Feng Wang, Yongseong Choi, Steven G. Louie, Patrick A. Lee, Zhi-Xun Shen, Sung-Kwan Mo, Michael F. Crommie

Abstract: Two-dimensional triangular-lattice antiferromagnets are predicted under some conditions to exhibit a quantum spin liquid ground state whose low-energy behavior is described by a spinon Fermi surface. Directly imaging the resulting spinons, however, is difficult due to their fractional, chargeless nature. Here we use scanning tunneling spectroscopy to image spinon density modulations arising from a… ▽ More Two-dimensional triangular-lattice antiferromagnets are predicted under some conditions to exhibit a quantum spin liquid ground state whose low-energy behavior is described by a spinon Fermi surface. Directly imaging the resulting spinons, however, is difficult due to their fractional, chargeless nature. Here we use scanning tunneling spectroscopy to image spinon density modulations arising from a spinon Fermi surface instability in single-layer 1T-TaSe$_2$, a two-dimensional Mott insulator. We first demonstrate the existence of localized spins arranged on a triangular lattice in single-layer 1T-TaSe$_2$ by contacting it to a metallic 1H-TaSe$_2$ layer and measuring the Kondo effect. Subsequent spectroscopic imaging of isolated, single-layer 1T-TaSe$_2$ reveals long-wavelength modulations at Hubbard band energies that reflect spinon density modulations. This allows direct experimental measurement of the spinon Fermi wavevector, in good agreement with theoretical predictions for a 2D quantum spin liquid. These results establish single-layer 1T-TaSe$_2$ as a new platform for studying novel two-dimensional quantum-spin-liquid phenomena. △ Less

Submitted 15 September, 2020; originally announced September 2020.

On-Stack Two-Dimensional Conversion of MoS2 into MoO3

Authors: Taeg Yeoung Ko, Areum Jeong, Wontaek Kim, Jinhwan Lee, Youngchan Kim, Jung Eun Lee, Gyeong Hee Ryu, Kwanghee Park, Dogyeong Kim, Zonghoon Lee, Min Hyung Lee, Changgu Lee, Sunmin Ryu

Abstract: Chemical transformation of existing two-dimensional (2D) materials can be crucial in further expanding the 2D crystal palette required to realize various functional heterostructures. In this work, we demonstrate a 2D 'on-stack' chemical conversion of single-layer crystalline MoS2 into MoO3 with a precise layer control that enables truly 2D MoO3 and MoO3/MoS2 heterostructures. To minimize perturbat… ▽ More Chemical transformation of existing two-dimensional (2D) materials can be crucial in further expanding the 2D crystal palette required to realize various functional heterostructures. In this work, we demonstrate a 2D 'on-stack' chemical conversion of single-layer crystalline MoS2 into MoO3 with a precise layer control that enables truly 2D MoO3 and MoO3/MoS2 heterostructures. To minimize perturbation of the 2D morphology, a nonthermal oxidation using O2 plasma was employed. The early stage of the reaction was characterized by a defect-induced Raman peak, drastic quenching of photoluminescence (PL) signals and sub-nm protrusions in atomic force microscopy images. As the reaction proceeded from the uppermost layer to the buried layers, PL and optical second harmonic generation signals showed characteristic modulations revealing a layer-by-layer conversion. The plasma-generated 2D oxides, confirmed as MoO3 by x-ray photoelectron spectroscopy, were found to be amorphous but extremely flat with a surface roughness of 0.18 nm, comparable to that of 1L MoS2. The rate of oxidation quantified by Raman spectroscopy decreased very rapidly for buried sulfide layers due to protection by the surface 2D oxides, exhibiting a pseudo-self-limiting behavior. As exemplified in this work, various on-stack chemical transformations can be applied to other 2D materials in forming otherwise unobtainable materials and complex heterostructures, thus expanding the palette of 2D material building blocks. △ Less

Submitted 10 August, 2020; originally announced August 2020.

Journal ref: 2D materials, 4, 2016, 014003

Static Rashba Effect by Surface Reconstruction and Photon Recycling in the Dynamic Indirect Gap of APbBr3 (A = Cs, CH3NH3) Single Crystals

Authors: Hongsun Ryu, Dae Young Park, K. McCall, Hye Ryung Byun, Yongjun Lee, Tae Jung Kim, Mun Seok Jeong, Jeongyong Kim, Mercouri G. Kanatzidis, Joon I. Jang

Abstract: Recently, halide perovskites have gained significant attention from the perspective of efficient spintronics owing to Rashba effect. This effect occurs as a consequence of strong spin-orbit coupling under noncentrosymmetric environment, which can be dynamic and/or static. However, there exist intense debates on the origin of broken inversion symmetry since the halide perovskites typically crystall… ▽ More Recently, halide perovskites have gained significant attention from the perspective of efficient spintronics owing to Rashba effect. This effect occurs as a consequence of strong spin-orbit coupling under noncentrosymmetric environment, which can be dynamic and/or static. However, there exist intense debates on the origin of broken inversion symmetry since the halide perovskites typically crystallize into a centrosymmetric structure. In order to clarify the issue, we examine both dynamic and static effects in the all-inorganic CsPbBr3 and organic-inorganic CH3NH3PbBr3 (MAPbBr3) perovskite single crystals by employing temperature- and polarization-dependent photoluminescence excitation spectroscopy. The perovskite single crystals manifest the dynamic effect by photon recycling in the indirect Rashba gap, causing dual peaks in the photoluminescence. But the effect vanishes in CsPbBr3 at low temperatures (< 50 K), accompanied by a striking color change of the crystal, arising presumably from lower degrees of freedom for inversion symmetry breaking associated with the thermal motion of the spherical Cs cation, compared with the polar MA cation in MAPbBr3. We also show that static Rashba effect occurs only in MAPbBr3 below 90 K due to surface reconstruction via MA-cation ordering, which likely extends across a few layers from the crystal surface to the interior. We further demonstrate that this static Rashba effect can be completely suppressed upon surface treatment with poly methyl methacrylate (PMMA) coating. We believe that our results provide a rationale for the Rashba effects in halide perovskites. △ Less

Submitted 25 August, 2020; v1 submitted 22 July, 2020; originally announced July 2020.

A plausible method of preparing the ideal p-n junction interface of a thermoelectric material by surface doping

Authors: Ji-Eun Lee, Jinwoong Hwang, Minhee Kang, Hyun-Jeong Joo, Hyejin Ryu, Kyoo Kim, Yongsam Kim, Namdong Kim, Anh Tuan Duong, Sunglae Cho, Sung-Kwan Mo, Choongyu Hwang, Imjeong Ho-Soon Yang

Abstract: Recent advances in two-dimensional (2D) crystals make it possible to realize an ideal interface structure that is required for device applications. Specifically, a p-n junction made of 2D crystals is predicted to exhibit an atomically well-defined interface that will lead to high device performance. Using angle-resolved photoemission spectroscopy, a simple surface treatment was shown to allow the… ▽ More Recent advances in two-dimensional (2D) crystals make it possible to realize an ideal interface structure that is required for device applications. Specifically, a p-n junction made of 2D crystals is predicted to exhibit an atomically well-defined interface that will lead to high device performance. Using angle-resolved photoemission spectroscopy, a simple surface treatment was shown to allow the possible formation of such an interface. Ta adsorption on the surface of a p-doped SnSe shifts the valence band maximum towards higher binding energy due to the charge transfer from Ta to SnSe that is highly localized at the surface due to the layered structure of SnSe. As a result, the charge carriers of the surface are changed from holes of its bulk characteristics to electrons, while the bulk remains as a p-type semiconductor. This observation suggests that the well-defined interface of a p-n junction with an atomically thin {\it n}-region is formed between Ta-adsorbed surface and bulk. △ Less

Submitted 18 July, 2020; originally announced July 2020.

Comments: 4 figures

Journal ref: Appl. Surf. Sci. 520, 146314 (2020)

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

Authors: Hanyoung Ryu, Yukiaki Ishida, Bongju Kim, Jeong Rae Kim, Woo Jin Kim, Yoshimitsu Kohama, Shusaku Imajo, Zhuo Yang, Wonshik Kyung, Sungsoo Hahn, Byungmin Sohn, Inkyung Song, Minsoo Kim, Soonsang Huh, Jongkeun Jung, Donghan Kim, Tae Won Noh, Saikat Das, Changyoung Kim

Abstract: 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 ch… ▽ More 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. △ Less

Submitted 25 January, 2021; v1 submitted 11 February, 2020; originally announced February 2020.

Journal ref: Phys. Rev. B 102, 041102 (2020)

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

Authors: Byungmin Sohn, Eunwoo Lee, Se Young Park, Wonshik Kyung, Jinwoong Hwang, Jonathan D. Denlinger, Minsoo Kim, Donghan Kim, Bongju Kim, Hanyoung Ryu, Soonsang Huh, Ji Seop Oh, Jong Keun Jung, Dongjin Oh, Younsik Kim, Moonsup Han, Tae Won Noh, Bohm-Jung Yang, Changyoung Kim

Abstract: 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 th… ▽ More 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. △ Less

Submitted 4 July, 2021; v1 submitted 10 December, 2019; originally announced December 2019.

Direct Band Gap Semiconducting Holey Graphyne: Structure, Synthesis and Potential Applications

Authors: Xinghui Liu1, Soo Min Cho, Shiru Lin, Eunbhin Yun, Eun Hee Baek, Zhongfang Chen, Do Hyun Ryu, Hyoyoung Lee

Abstract: Here we report two-dimensional (2D) single-crystalline holey-graphyne (HGY) created an interfacial two-solvent system through a Castro-Stephens coupling reaction from 1,3,5-tribromo-2,4,6-triethynylbenzene. HGY is a new type of 2D carbon allotrope whose structure is comprised of a pattern of six-vertex and eight-vertex rings. The carbon-carbon 2D network of HGY is alternately linked between benzen… ▽ More Here we report two-dimensional (2D) single-crystalline holey-graphyne (HGY) created an interfacial two-solvent system through a Castro-Stephens coupling reaction from 1,3,5-tribromo-2,4,6-triethynylbenzene. HGY is a new type of 2D carbon allotrope whose structure is comprised of a pattern of six-vertex and eight-vertex rings. The carbon-carbon 2D network of HGY is alternately linked between benzene rings and sp (carbon-carbon triple bond) bonding. The ratio of the sp over sp2 bonding is 50%. It is confirmed that HGY is stable by DFT calculation. The vibrational, optic, and electric properties of HGY are investigated theoretically and experimentally. It is a p-type semiconductor that embraces a natural direct band gap (~ 1.0 eV) with high hole mobility and electron mobility at room temperature. This report is expected to help develop a new types of carbon-based semiconductor devices with high mobility. △ Less

Submitted 8 July, 2019; originally announced July 2019.

Visualizing Exotic Orbital Texture in the Single-Layer Mott Insulator 1T-TaSe2

Authors: Yi Chen, Wei Ruan, Meng Wu, Shujie Tang, Hyejin Ryu, Hsin-Zon Tsai, Ryan Lee, Salman Kahn, Franklin Liou, Caihong Jia, Oliver R. Albertini, Hongyu Xiong, Tao Jia, Zhi Liu, Jonathan A. Sobota, Amy Y. Liu, Joel E. Moore, Zhi-Xun Shen, Steven G. Louie, Sung-Kwan Mo, Michael F. Crommie

Abstract: Mott insulating behavior is induced by strong electron correlation and can lead to exotic states of matter such as unconventional superconductivity and quantum spin liquids. Recent advances in van der Waals material synthesis enable the exploration of novel Mott systems in the two-dimensional limit. Here we report characterization of the local electronic properties of single- and few-layer 1T-TaSe… ▽ More Mott insulating behavior is induced by strong electron correlation and can lead to exotic states of matter such as unconventional superconductivity and quantum spin liquids. Recent advances in van der Waals material synthesis enable the exploration of novel Mott systems in the two-dimensional limit. Here we report characterization of the local electronic properties of single- and few-layer 1T-TaSe2 via spatial- and momentum-resolved spectroscopy involving scanning tunneling microscopy and angle-resolved photoemission. Our combined experimental and theoretical study indicates that electron correlation induces a robust Mott insulator state in single-layer 1T-TaSe2 that is accompanied by novel orbital texture. Inclusion of interlayer coupling weakens the insulating phase in 1T-TaSe2, as seen by strong reduction of its energy gap and quenching of its correlation-driven orbital texture in bilayer and trilayer 1T-TaSe2. Our results establish single-layer 1T-TaSe2 as a useful new platform for investigating strong correlation physics in two dimensions. △ Less

Submitted 16 May, 2019; v1 submitted 24 April, 2019; originally announced April 2019.

Journal ref: Nature Physics 16, 218-224 (2020)

Visualization of multifractal superconductivity in a two-dimensional transition metal dichalcogenide in the weak-disorder regime

Authors: Carmen Rubio-Verdú, Antonio M. García-García, Hyejin Ryu, Deung-Jang Choi, Javier Zaldívar, Shujie Tang, Bo Fan, Zhi-Xun Shen, Sung-Kwan Mo, José Ignacio Pascual, Miguel M. Ugeda

Abstract: Eigenstate multifractality is a distinctive feature of non-interacting disordered metals close to a metal-insulator transition, whose properties are expected to extend to superconductivity. While multifractality in three dimensions (3D) only develops near the critical point for specific strong-disorder strengths, multifractality in 2D systems is expected to be observable even for weak disorder. He… ▽ More Eigenstate multifractality is a distinctive feature of non-interacting disordered metals close to a metal-insulator transition, whose properties are expected to extend to superconductivity. While multifractality in three dimensions (3D) only develops near the critical point for specific strong-disorder strengths, multifractality in 2D systems is expected to be observable even for weak disorder. Here we provide evidence for multifractal features in the superconducting state of an intrinsic weakly disordered single-layer NbSe$_2$ by means of low-temperature scanning tunneling microscopy/spectroscopy. The superconducting gap, characterized by its width, depth and coherence peaks' amplitude, shows a characteristic spatial modulation coincident with the periodicity of the quasiparticle interference pattern. Spatial inhomogeneity of the superconducting gap width, proportional to the local order parameter in the weak-disorder regime, follows a log-normal statistical distribution as well as a power-law decay of the two-point correlation function, in agreement with our theoretical model. Furthermore, the experimental singularity spectrum f($α$) shows anomalous scaling behavior typical from 2D weakly disordered systems. △ Less

Submitted 20 March, 2020; v1 submitted 18 October, 2018; originally announced October 2018.

Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides with experiment and theory

Authors: Sara Barja, Sivan Refaely-Abramson, Bruno Schuler, Diana Y. Qiu, Artem Pulkin, Sebastian Wickenburg, Hyejin Ryu, Miguel M. Ugeda, Christoph Kastl, Christopher Chen, Choongyu Hwang, Adam Schwartzberg, Shaul Aloni, Sung-Kwan Mo, D. Frank Ogletree, Michael F. Crommie, Oleg V. Yazyev, Steven G. Louie, Jeffrey B. Neaton, Alexander Weber-Bargioni

Abstract: Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support from Transmission Electron Microscopy (TEM) and Scan… ▽ More Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support from Transmission Electron Microscopy (TEM) and Scanning Tunneling Microscopy (STM) images. However, TEM imaging measurements do not provide direct access to the electronic structure of individual defects; and while Scanning Tunneling Spectroscopy (STS) is a direct probe of local electronic structure, the interpretation of the chemical nature of atomically-resolved STM images of point defects in 2D-TMDs can be ambiguous. As a result, the assignment of point defects as vacancies or substitutional atoms of different kinds in 2D-TMDs, and their influence on their electronic properties, has been inconsistent and lacks consensus. Here, we combine low-temperature non-contact atomic force microscopy (nc-AFM), STS, and state-of-the-art ab initio density functional theory (DFT) and GW calculations to determine both the structure and electronic properties of the most abundant individual chalcogen-site defects common to 2D-TMDs. Surprisingly, we observe no IGS for any of the chalcogen defects probed. Our results and analysis strongly suggest that the common chalcogen defects in our 2D-TMDs, prepared and measured in standard environments, are substitutional oxygen rather than vacancies. △ Less

Submitted 6 March, 2020; v1 submitted 8 October, 2018; originally announced October 2018.

Journal ref: Nat Commun 10, 3382 (2019)

A Unique Crystal Structure of Ca$_2$RuO$_4$ in the Current Stabilized Semi-Metallic State

Authors: J. Bertinshaw, N. Gurung, P. Jorba, H. Liu, M. Schmid, D. T. Mantadakis, M. Daghofer, M. Krautloher, A. Jain, G. H. Ryu, O. Fabelo, P. Hansmann, G. Khaliullin, C. Pfleiderer, B. Keimer, B. J. Kim

Abstract: The electric-current stabilized semi-metallic state in the quasi-two-dimensional Mott insulator Ca$_2$RuO$_4$ exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and X-ray diffraction, we show that this non-equilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high press… ▽ More The electric-current stabilized semi-metallic state in the quasi-two-dimensional Mott insulator Ca$_2$RuO$_4$ exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and X-ray diffraction, we show that this non-equilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high pressure and epitaxial strain, which in turn leads to a distinct electronic band structure. Dynamical mean field theory calculations based on the crystallographically refined atomic coordinates and realistic Coulomb repulsion parameters indicate a semi-metallic state with partially gapped Fermi surface. Our neutron diffraction data show that the non-equilibrium behavior is homogeneous, with antiferromagnetic long-range order completely suppressed. These results provide a new basis for theoretical work on the origin of the unusual non-equilibrium diamagnetism in Ca$_2$RuO$_4$. △ Less

Submitted 21 May, 2019; v1 submitted 17 June, 2018; originally announced June 2018.

Comments: 12 pages, 3 figures, 1 table

Journal ref: Phys. Rev. Lett. 123, 137204 (2019)

Emergence of Kondo resonance in graphene intercalated with cerium

Authors: Jinwoong Hwang, Kyoo Kim, Hyejin Ryu, Jingul Kim, Ji-Eun Lee, Sooran Kim, Minhee Kang, Byeong-Gyu Park, Alessandra Lanzara, Jinwook Chung, Sung-Kwan Mo, Jonathan Denlinger, Byung Il Min, Choongyu Hwang

Abstract: The interaction between a magnetic impurity, such as cerium (Ce) atom, and surrounding electrons has been one of the core problems in understanding many-body interaction in solid and its relation to magnetism. Kondo effect, the formation of a new resonant ground state with quenched magnetic moment, provides a general framework to describe many-body interaction in the presence of magnetic impurity.… ▽ More The interaction between a magnetic impurity, such as cerium (Ce) atom, and surrounding electrons has been one of the core problems in understanding many-body interaction in solid and its relation to magnetism. Kondo effect, the formation of a new resonant ground state with quenched magnetic moment, provides a general framework to describe many-body interaction in the presence of magnetic impurity. In this Letter, a combined study of angle-resolved photoemission (ARPES) and dynamic mean-field theory (DMFT) on Ce-intercalated graphene shows that Ce-induced localized states near Fermi energy, $E_{\rm F}$, hybridized with the graphene $π$ band, exhibit gradual increase in spectral weight upon decreasing temperature. The observed temperature dependence follows the expectations from the Kondo picture in the weak coupling limit. Our results provide a novel insight how Kondo physics emerges in the sea of two-dimensional Dirac electrons. △ Less

Submitted 14 June, 2018; originally announced June 2018.

Comments: 17 pages, 4 figures

Journal ref: Nano. Lett. 18, 3661 (2018)

Holstein polaron in a valley-degenerate two-dimensional semiconductor

Authors: Mingu Kang, Sung Won Jung, Woo Jong Shin, Yeongsup Sohn, Sae Hee Ryu, Timur K. Kim, Moritz Hoesch, Keun Su Kim

Abstract: Two-dimensional (2D) crystals have emerged as a class of materials with tuneable carrier density. Carrier doping to 2D semiconductors can be used to modulate manybody interactions and to explore novel composite particles. Holstein polaron is a small composite particle of an electron carrying a cloud of self-induced lattice deformation (or phonons), which has been proposed to play a key role in hig… ▽ More Two-dimensional (2D) crystals have emerged as a class of materials with tuneable carrier density. Carrier doping to 2D semiconductors can be used to modulate manybody interactions and to explore novel composite particles. Holstein polaron is a small composite particle of an electron carrying a cloud of self-induced lattice deformation (or phonons), which has been proposed to play a key role in high-temperature superconductivity and carrier mobility in devices. Here, we report the discovery of Holstein polarons in a surface-doped layered semiconductor, MoS2, where a puzzling 2D superconducting dome with the critical temperature of 12 K was found recently. Using a high-resolution band mapping of charge carriers, we found strong band renormalizations collectively identified as a hitherto unobserved spectral function of Holstein polarons. The unexpected short-range nature of electron-phonon (e-ph) coupling in MoS2 can be explained by its valley degeneracy that enables strong intervalley coupling mediated by acoustic phonons. The coupling strength is found to gradually increase along the superconducting dome up to the intermediate regime, suggesting bipolaronic pairing in 2D superconductivity. △ Less

Submitted 28 May, 2018; originally announced May 2018.

Journal ref: Nature Materials, published online (2018)

Electric Field-Tuned Topological Phase Transition in Ultra-Thin Na3Bi - Towards a Topological Transistor

Authors: James L. Collins, Anton Tadich, Weikang Wu, Lidia C. Gomes, Joao N. B. Rodrigues, Chang Liu, Jack Hellerstedt, Hyejin Ryu, Shujie Tang, Sung-Kwan Mo, Shaffique Adam, Shengyuan A. Yang, Michael. S. Fuhrer, Mark T. Edmonds

Abstract: The electric field induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor [1-4]. In this scheme an electric field can switch 'on' the ballistic flow of charge and spin along dissipationless edges of the two-dimensional (2D) quantum spin Hall insulator [5-9], and when 'off' is a conventional insulator with… ▽ More The electric field induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor [1-4]. In this scheme an electric field can switch 'on' the ballistic flow of charge and spin along dissipationless edges of the two-dimensional (2D) quantum spin Hall insulator [5-9], and when 'off' is a conventional insulator with no conductive channels. Such as topological transistor is promising for low-energy logic circuits [4], which would necessitate electric field-switched materials with conventional and topological bandgaps much greater than room temperature, significantly greater than proposed to date [6-8]. Topological Dirac semimetals(TDS) are promising systems in which to look for topological field-effect switching, as they lie at the boundary between conventional and topological phases [3,10-16]. Here we use scanning probe microscopy/spectroscopy (STM/STS) and angle-resolved photoelectron spectroscopy (ARPES) to show that mono- and bilayer films of TDS Na3Bi [3,17] are 2D topological insulators with bulk bandgaps >400 meV in the absence of electric field. Upon application of electric field by doping with potassium or by close approach of the STM tip, the bandgap can be completely closed then re-opened with conventional gap greater than 100 meV. The large bandgaps in both the conventional and quantum spin Hall phases, much greater than the thermal energy kT = 25 meV at room temperature, suggest that ultrathin Na3Bi is suitable for room temperature topological transistor operation. △ Less

Submitted 4 February, 2019; v1 submitted 21 May, 2018; originally announced May 2018.

Journal ref: Nature 564, 390 (2018)

Observation of Topologically Protected States at Crystalline Phase Boundaries in Single-layer WSe2

Authors: Miguel M. Ugeda, Artem Pulkin, Shujie Tang, Hyejin Ryu, Quansheng Wu, Yi Zhang, Dillon Wong, Zahra Pedramrazi, Ana Martín-Recio, Yi Chen, Feng Wang, Zhi-Xun Shen, Sung-Kwan Mo, Oleg V. Yazyev, Michael F. Crommie

Abstract: Transition metal dichalcogenide (TMD) materials are unique in the wide variety of structural and electronic phases they exhibit in the two-dimensional (2D) single-layer limit. Here we show how such polymorphic flexibility can be used to achieve topological states at highly ordered phase boundaries in a new quantum spin Hall insulator (QSHI), 1T'-WSe2. We observe helical states at the crystallograp… ▽ More Transition metal dichalcogenide (TMD) materials are unique in the wide variety of structural and electronic phases they exhibit in the two-dimensional (2D) single-layer limit. Here we show how such polymorphic flexibility can be used to achieve topological states at highly ordered phase boundaries in a new quantum spin Hall insulator (QSHI), 1T'-WSe2. We observe helical states at the crystallographically-aligned interface between quantum a spin Hall insulating domain of 1T'-WSe2 and a semiconducting domain of 1H-WSe2 in contiguous single layers grown using molecular beam epitaxy (MBE). The QSHI nature of single-layer 1T'-WSe2 was verified using ARPES to determine band inversion around a 120 meV energy gap, as well as STM spectroscopy to directly image helical edge-state formation. Using this new edge-state geometry we are able to directly confirm the predicted penetration depth of a helical interface state into the 2D bulk of a QSHI for a well-specified crystallographic direction. The clean, well-ordered topological/trivial interfaces observed here create new opportunities for testing predictions of the microscopic behavior of topologically protected boundary states without the complication of structural disorder. △ Less

Submitted 7 November, 2018; v1 submitted 5 February, 2018; originally announced February 2018.

Comments: https://www.nature.com/articles/s41467-018-05672-w

Journal ref: Nature Communications 9, 3401 (2018)

Universal Mechanism of Band-Gap Engineering in Transition-Metal Dichalcogenides

Authors: Mingu Kang, Beomyoung Kim, Sae Hee Ryu, Sung Won Jung, Jimin Kim, Luca Moreschini, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Keun Su Kim

Abstract: Two-dimensional (2D) van-der-Waals semiconductors have emerged as a class of materials with promising device characteristics owing to the intrinsic bandgap. For realistic applications, the ideal is to modify the bandgap in a controlled manner by a mechanism that can be generally applied to this class of materials. Here, we report the observation of a universally tunable bandgap in the family of bu… ▽ More Two-dimensional (2D) van-der-Waals semiconductors have emerged as a class of materials with promising device characteristics owing to the intrinsic bandgap. For realistic applications, the ideal is to modify the bandgap in a controlled manner by a mechanism that can be generally applied to this class of materials. Here, we report the observation of a universally tunable bandgap in the family of bulk 2H transition metal dichalcogenides (TMDs) by in situ surface doping of Rb atoms. A series of angle-resolved photoemission spectra unexceptionally shows that the bandgap of TMDs at the zone corners is modulated in the range of 0.8 ~ 2.0 eV, which covers a wide spectral range from visible to near infrared, with a tendency from indirect to direct bandgap. A key clue to understand the mechanism of this bandgap engineering is provided by the spectroscopic signature of symmetry breaking and resultant spin splitting, which can be explained by the formation of 2D electric dipole layers within the surface bilayer of TMDs. Our results establish the surface Stark effect as a universal mechanism of bandgap engineering based on the strong 2D nature of van-der-Waals semiconductors. △ Less

Submitted 30 November, 2017; originally announced November 2017.

Journal ref: Nano Lett. 17, 1610-1615 (2017)