arXiv subjects

Kenji Watanabe

Publications and source records attributed to Kenji Watanabe.

At least 397 records · Page 22Linked to original sources

arXiv2025

Super-Moiré Spin Textures in Twisted Antiferromagnets

Stacking two-dimensional (2D) layered materials offers a powerful platform to engineer electronic and magnetic states. In general, the resulting states, such as Moiré magnetism, have a periodicity at the length scale of the Moiré unit cell. Here, we report a new type of magnetism -- dubbed a super-Moiré magnetic state -- which is characterized by long-range magnetic textures extending beyond the single Moiré unit cell -- in twisted double bilayer chromium triiodide (tDB CrI$_3$). We found that at small twist angles, the size of the spontaneous magnetic texture increases with twist angle, opposite to the underlying Moiré periodicity. The spin-texture size reaches a maximum of about 300 nm in 1.1$°$ twisted devices, an order of magnitude larger than the underlying Moiré wavelength, and vanishes at twist angles above 2$°$. Employing scanning quantum spin magnetometry, the obtained vector field maps suggest the formation of antiferromagnetic Néel-type skyrmions spanning multiple Moiré cells. The twist-angle-dependent study combined with large-scale atomistic simulations suggests that complex magnetic competition between the Dzyaloshinskii--Moriya interaction, magnetic anisotropy, and exchange interactions controlled by the relative rotation of the layers produces the topological textures which arise in the super-Moiré spin orders.

quant-ph↗

arXiv2025

Mapping the twist angle dependence of quasi-Brillouin zones in doubly aligned graphene/BN heterostructures

When monolayer graphene is crystallographically aligned to hexagonal boron nitride (BN), a moiré superlattice is formed, producing characteristic satellite Dirac peaks in the electronic band structure. Aligning a second BN layer to graphene creates two coexisting moiré patterns, which can interfere to produce periodic, quasi-periodic or non-periodic superlattices, depending on their relative alignment. Here, we investigate one of the simplest realizations of such a double-moiré structure, graphene encapsulated between two BN layers, using dynamically rotatable van der Waals heterostructures. Our setup allows \textit{in situ} control of the top BN alignment while keeping the bottom BN fixed. By systematically mapping the charge transport as a function of BN angular alignment, we identify the simultaneous signatures of the original moirés, super-moirés, and a third set of features corresponding to quasi-Brillouin zones (qBZ) formed when the system's periodicity becomes ill-defined. Comparing our measurements with theoretical models, we provide the first experimental mapping of the qBZs as a function of angular alignment. Our results establish a direct experimental link between moiré interference and qBZ formation, opening new avenues for engineering electronic structures in multi-aligned 2D heterostructures.

cond-mat.mes-hall↗

arXiv2025

Spin injection and emission helicity switching in a 2D perovskite/WSe2 heterostructure

The initialization and control of a long-lived spin population in lead halide perovskites are prerequisites for their use in spintronic applications. Here, we demonstrate circular polarization of the interlayer exciton emission in a (BA)2PbI4/WSe2 monolayer heterostructure. The helicity of this emission is controlled by tuning the energy of the excitation laser through the manifold of exciton resonances of the WSe2 monolayer, together with an emerging interlayer absorption feature of the heterostructure. Theoretical calculations show that this resonance arises from hybridized (BA)2PbI4/WSe2 states in the valence band. This hybrid character enables its observation in both linear absorption and ultrafast pump-probe spectroscopies, and plays a key role in controlling the sign of the helicity of the interlayer exciton emission. The tunable spin polarization demonstrated here, with the WSe2 monolayer effectively acting as a tunable spin filter, represents an important step toward the use of 2D perovskites in opto-spintronic applications.

cond-mat.mtrl-sci↗

arXiv2025

Sliding Disassembly of van der Waals Heterostructures

Many recent advances in our understanding of two-dimensional (2D) electron systems stem from van der Waals (vdW) heterostructures. The assembly process relies on the weak bonding across interfaces between layered vdW compounds, making it possible to construct exceptionally clean heterostructures from chemically and structurally distinct materials - a challenging task for traditional thin-film growth techniques. Here we demonstrate an additional, dynamic degree of freedom afforded by vdW interfaces, wherein we use microstructured polymer stamps to disassemble and reconfigure vdW heterostructures by sliding. We apply this technique to alter the dielectric environment of monolayer graphene, perform scanning tunneling microscopy on semiconducting and air-sensitive monolayers, and manipulate strain-sensitive moiré materials. Together these demonstrations suggest a new paradigm for assembling and dynamically modifying van der Waals heterostructures, with the potential to reveal new insights into 2D electron systems.

cond-mat.mes-hall↗

arXiv2025

Does Moire Matter? Critical Moire Dependence with Quantum Fluctuations in Graphene Based Integer and Fractional Chern Insulators

Rhombohedral multilayer graphene has emerged as a powerful platform for investigating flat-band-driven correlated phenomena, yet most aspects remain not understood. In this work, we systematically study the moire-dependent band topology in rhombohedral hexalayer graphene. For the first time we demonstrate that the moire twist angle plays a crucial role in the formation of the moire Chern insulators in rhombohedral hexalayer graphene/hexagonal boron nitride (RHG/hBN) moire superlattices. In the moire-distant regime at filling factor v = 1, only systems with a twist angle θ < 1.1° exhibit an integer moire Chern insulator, while the fractional Chern insulator at v = 2/3 requires smaller twist angle to be stabilized. Our theoretical modelling, which includes quantum fluctuations and exact diagonalization results, suggests that mean-field theory, which has been widely adopted, does not explain the twist-angle dependence of the v = 1 phase diagram, and that correlation effects are crucial. Moreover, we realize two distinct stacking configurations ( /Xi=0 and /Xi=1) between graphene and hBN, and find that both cases can yield a Chern insulator at v = 1. Our experimental work upends the current mean-field paradigm, illuminates how quantum fluctuations and moiré effects shape the RHG/hBN phase diagram, and paves the way for future understanding and engineering of topological correlated states in rhombohedral graphene moire systems.

cond-mat.mes-hall↗

arXiv2025

Atomically-resolved exciton emission from single defects in MoS$_2$

Understanding how atomic defects shape the nanoscale optical properties of two-dimensional (2D) semiconductors is essential for advancing quantum technologies and optoelectronics. Using scanning tunneling spectroscopy (STS) and luminescence (STML), we correlate the atomic structure and optical fingerprints of individual defects in monolayer MoS$_2$. A bilayer of hexagonal boron nitride (hBN) effectively decouples MoS$_2$ from the graphene substrate, increasing its band gap and extending the defect charge state lifetime. This enables the observation of sharp STML emission lines from MoS$_2$ excitons and trions exhibiting nanoscale sensitivity to local potential fluctuations. We identify the optical signatures of common point defects in MoS$_2$: sulfur vacancies (Vac$_\text{S}^-$), oxygen substitutions (O$_\text{S}$), and negatively charged carbon-hydrogen complexes (CH$_\text{S}^-$). While Vac$_\text{S}^-$ and O$_\text{S}$ only suppress pristine excitonic emission, CH$_\text{S}^-$ generate defect-bound exciton complexes ($A^-X$) about 200\,meV below the MoS$_2$ exciton. Sub-nanometer-resolved STML maps reveal large spectral shifts near charged defects, concurrent with the local band bending expected for band-to-defect optical transitions. These results establish an atomically precise correlation between structure, electronic states, and optical response, enabling deterministic engineering of quantum emitters in 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

Optical Injection and Detection of Long-Lived Interlayer Excitons in van der Waals Heterostructures

Interlayer excitons in semiconducting bilayers separated by insulating hBN layers constitute a promising platform for investigation of strongly correlated bosonic phases. Here, we report an optical method for the generation and characterization of long-lived interlayer excitons. We confirm the presence of tightly bound interlayer excitons by measuring 1s and 2s intralayer excitons in each layer concurrently. Using a pump-probe technique, we find interlayer exciton lifetimes up to 8.8 $μ$s, increasing with the thickness of the hBN. With optical access to long-lived interlayer excitons, our approach provides a new route to explore degenerate Bose--Fermi mixtures of excitons and itinerant electrons with high spatial and temporal resolution.

cond-mat.mes-hall↗

arXiv2025

Mapping the moiré potential in multi-layer rhombohedral graphene

Rhombohedral graphene (rG) aligned with hexagonal boron nitride (hBN) has been shown to host flat bands that stabilize various strongly correlated quantum phases, including Mott insulators, integer, and fractional quantum anomalous Hall phases. In this work, we use scanning tunneling microscopy/spectroscopy (STM/STS) to visualize the dispersion of flat bands with doping and applied displacement fields in a hBN-aligned rhombohedral trilayer graphene (rtG)/hBN moiré superlattice. In addition to the intrinsic flat bands of rtG induced by the displacement field, we observe low-energy features originating from moiré potential-induced band folding. Real-space variations of the spectroscopic features allow us to quantify the spatial structure of the moiré potential at the rtG/hBN interface. Importantly, we find that accurately capturing the moiré site-dependent spectra requires incorporating a moiré potential acting on the top graphene layer with a sign opposite to that of the bottom layer into the continuum model. Our results thus provide key experimental and theoretical insights into understanding the role of the moire superlattice in rG/hBN heterostructures.

cond-mat.mes-hall↗

arXiv2025

Thermoelectric effect at the quantum Hall-superconductor interface

The interfaces of quantum Hall insulators with superconductors have emerged as a promising platform to realise interesting physics that may be relevant for topologically protected quantum computing. However, these interfaces can host other effects which obscure the detection of the desired excitations. Here we present measurements of the thermoelectric effect at the quantum Hall-superconductor interface. We explain the heat transport by considering the formation of a hotspot at the interface, which results in a non-equilibrium distribution of electrons that can propagate across the superconductor through vortex cores. The observed thermoelectric effect results in a voltage which changes sign on quantum Hall plateaus and responds to the rearrangement of vortices in the wire. These observations highlight the complex interplay of thermal and charge phenomena at the quantum Hall -- superconductor interfaces and should be considered when interpreting transport measurements in similar systems.

cond-mat.mes-hall↗

arXiv2025

Investigating the Ferroelectric Potential Landscape of 3R-MoS$_2$ through Optical Measurements

In recent years, sliding ferroelectricity has emerged as a topic of significant interest due to its possible application in non-volatile, reconfigurable storage devices. This phenomenon is unique to two-dimensional van der Waals materials, where out-of-plane ferroelectric polarization switching is induced by relative in-plane sliding of adjacent layers. The intrinsic stacking order influences the resulting polarization, creating distinct polarization regions separated by domain walls. These regions and the domain walls can be manipulated using an applied vertical electric field, enabling a switchable system that retains the environmental robustness of van der Waals materials under ambient conditions. This study investigates 3R-MoS$_2$ using various optical measurement techniques at room temperature. The spatially resolved optical measurements reveal apparent signal changes corresponding to different ferroelectric stacking orders and variations in layer count. Our findings demonstrate that fast optical mapping at room temperature is a reliable method for probing ferroelectric potential steps in 3R-stacked MoS$_2$ samples, thereby facilitating the identification of the ferroelectric configuration. This approach does not require a conductive substrate or an electrical contact to the sample, making it more versatile than traditional atomic force probe techniques.

cond-mat.mtrl-sci↗

arXiv2025

Non-ohmic to ohmic crossover in the breakdown of the quantum Hall states in graphene under broadband excitations

Graphene, through the coexistence of large cyclotron gaps and small spin and valley gaps, offers the possibility to study the breakdown of the quantum Hall effect across a wide range of energy scales. In this work, we investigate the breakdown of the QHE in high-mobility graphene Corbino devices under broadband excitation ranging from DC up to 10 GHz. We find that the conductance is consistently described by variable range hopping (VRH) and extract the hopping energies from both temperature and field-driven measurements. Using VRH thermometry, we are able to distinguish between a cold and hot electron regime, which are dominated by non-ohmic VRH and Joule heating, respectively. Our results demonstrate that breakdown in the quantum Hall regime of graphene is governed by a crossover from non-ohmic, field-driven VRH to ohmic, Joule-heating-dominated transport.

cond-mat.mes-hall↗

arXiv2025

Twist-tuned exchange and hysteresis in a bilayer van der Waals magnet

Moiré superlattices in twisted bilayers enable profound reconstructions of the electronic bandstructure, giving rise to correlated states with remarkable tunability. Extending this paradigm to van der Waals magnets, twisting creates spatially varying interlayer exchange interactions that stabilize emergent spin textures and the coexistence of ferromagnetic and antiferromagnetic domains. Here, we demonstrate the emergence of robust magnetic hysteresis in bilayer CrSBr upon twisting by an angle of ~ 3°. This is observed as the corresponding hysteretic evolution of the exciton energy, that directly correlates with the bilayer magnetic state, in magnetic field dependent photoluminescence measurements. A two-sublattice model captures this behavior, attributing it to the twist-induced reduction of interlayer exchange that stabilizes both parallel and antiparallel spin configurations across a broad field range. Comparison with experiment enables quantitative extraction of the effective exchange strength. Remarkably, the system exhibits coherent averaging across the moiré supercell, yielding an effective monodomain response characterized by switching into the antiferromagnetic state, rather than forming spin textures or fragmented domains. Spatially resolved measurements further uncover local variations in hysteresis loops, consistent with position-dependent modulation of the average exchange interaction. Our results establish twist engineering as a powerful route to programmable magnetic memories in two-dimensional magnets, harnessing the robustness of antiferromagnetic order.

cond-mat.mtrl-sci↗

arXiv2025

Skyrmionic Transport and First Order Phase Transitions in Twisted Bilayer Graphene Quantum Hall Ferromagnet

Large-angle twisted bilayer graphene (TBLG) realizes a multicomponent quantum Hall (QH) platform of spin, valley and layer pseudospins with strong Coulomb interaction-driven symmetry broken phases. Here, we investigate the low energy Landau-level spectrum of layer-decoupled TBLG and identify skyrmion-textured charged excitations and a field-induced insulating transition to an intervalley coherent state at zero-filling factor. Symmetric potential difference perpendicular to TBLG demonstrated layer coherent population of ground states with uniform energy barriers, while the charge imbalance in the layers at finite displacement field led to multidomain nucleation and a pronounced hysteresis in the exchange-dominated transport regime suggesting first order phase transitions between different QH ferromagnetic ground states.

cond-mat.mes-hall↗

arXiv2025

Frequency as a Clock: Synchronization and Intrinsic Recovery in Graphene Transistor Dynamics

Hysteresis and memory effects in graphene field-effect transistors (GFETs) offer unique opportunities for neuromorphic computing, sensing, and memory applications, yet their physical origins remain debated due to competing volatile and nonvolatile interpretations. Here, we present a unified dynamic model that captures the essential physics of the GFET response under periodic gate modulation, accounting for both intrinsic relaxation processes and externally driven charge transfer. By modeling non-equilibrium carrier dynamics as a competition between injection and reabsorption rates, we uncover two distinct regimes: one governed by intrinsic, frequency-independent relaxation and another exhibiting frequency-locked behavior where the response is tied to the external drive. This distinction resolves apparent nonvolatile effects and explains loop invariance in floating-gate structures via displacement current-driven charge injection. Our framework predicts the evolution of the hysteresis loop shape, amplitude, and direction across a wide range of driving conditions, offering a versatile tool for interpreting experimental results and guiding the design of next-generation graphene-based electronic systems.

cond-mat.mes-hall↗

arXiv2025

Electronic origin of reorganization energy in interfacial electron transfer

Electron transfer (ET) reactions underpin energy conversion and chemical transformations in both biological and abiological systems. The efficiency of any ET process relies on achieving a desired ET rate within an optimal driving force range. Marcus theory provides a microscopic framework for understanding the activation free energy, and thus the rate, of ET in terms of a key parameter: the reorganization energy. For electrified solid-liquid interfaces, it has long been conventionally understood that only factors in the electrolyte phase are responsible for determining the reorganization energy and the electronic density of states (DOS) of the electrode serves only to dictate the number of thermally accessible channels for ET. Here we show instead that the electrode DOS plays a central role in governing the reorganization energy, far outweighing its conventionally assumed role. Using atomically layered heterostructures, we tune the DOS of graphene and measure outer-sphere ET kinetics. We find the ensuing variation in ET rate arises from strong modulation in a reorganization energy associated with image potential localization in the electrode. This work redefines the traditional paradigm of heterogeneous ET kinetics, revealing a deeper role of the electrode electronic structure in interfacial reactivity.

cond-mat.mtrl-sci↗

arXiv2025

Direct observation of band structure modifications from monolayer WSe2 to Janus WSSe

Janus monolayer transition metal dichalcogenides (TMDs), created by post-growth substitution of the top chalcogen layer, represent a new direction for engineering 2D crystal properties. However, their rapid ambient degradation and the difficulty of obtaining large-area monolayer samples have limited the available experimental probes, leaving their detailed electronic structure near the Fermi level largely unexplored. In this work, by performing micro-focused angle-resolved photoemission spectroscopy (μ-ARPES) on an identical sample transformed from monolayer WSe2 to Janus WSSe via a H2 plasma-assisted chalcogen-exchange method, we reveal the evolution of its electronic band structure. We observe ARPES signature consistent with the Rashba-type spin splitting due to broken horizontal mirror symmetry, and a significant upward shift of the highest valence band at the Γ-point by approximately 160 meV. These direct observations clarify the key electronic modifications that govern the material's properties and provide a pathway for band engineering in Janus TMDs.

cond-mat.mtrl-sci↗

arXiv2025

Sliding multiferroicity in hexagonal stacked CrI3

Developing new multiferroics at the two-dimensional (2D) limit with energy-efficient magnetoelectric coupling can inform the interplay physics of novel orders and advance on-chip high-performance computing applications. Here we apply stacking order engineering to create a new type of 2D multiferroics, namely sliding multiferroics, based on polar hexagonal stacked (H-stacked) CrI3. This new stacking order removes structural inversion symmetry and gives rise to room temperature sliding ferroelectricity, as confirmed by Raman spectroscopy, second harmonic generation spectroscopy and electrical transport measurements. Building upon the gate-dependent reflective magnetic circular dichroism, first-principles calculations, and modeling, sliding ferroelectricity is shown to interplay with an emergent interfacial ferromagnetism via interlayer spin-polarized charge transfer. This coupling mechanism results in non-volatile magnetic switching by as low as 0.4V across the H-stacked CrI3. Our demonstration introduces polar stacking order engineering of 2D magnets as a general approach to create non-volatile 2D multiferroics with efficient magnetoelectric coupling, paving the way for low-power electronics and spintronics at the atomically thin limit.

cond-mat.mtrl-sci↗

arXiv2025

Electrically modulated light-emitting diodes driven by resonant and antiresonant tunneling between Cr$_2$Ge$_2$Te$_6$ electrodes

Exploring the electron tunneling mechanisms in diverse materials systems constitutes a versatile strategy for tailoring the properties of optoelectronic devices. In this domain, bipolar vertical tunneling junctions composed of van der Waals materials with vastly different electronic band structures enable simultaneous injection of electrons and holes into an optically active material, providing a universal blueprint for light-emitting diodes (LEDs). Efficient modulation of the injection efficiency has previously been demonstrated by creating resonant states within the energy barrier formed by the luminescent material. Here, we present an alternative approach towards resonant tunneling conditions by fabricating tunneling junctions composed entirely from gapped materials: Cr$_2$Ge$_2$Te$_6$ as electrodes, hBN as a tunneling barrier, and monolayer WSe$_2$ as a luminescent medium. The characterization of such LEDs revealed a nonmonotonous evolution of the electroluminescence intensity with the tunneling bias. The dominant role driving the characteristics of the electron tunneling was associated with the relative alignment of the density of states in Cr$_2$Ge$_2$Te$_6$ electrodes. The unique device architecture introduced here presents a universal pathway towards LEDs operating at room temperature with electrically modulated emission intensity.

cond-mat.mtrl-sci↗