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Kenji Watanabe

Publications and source records attributed to Kenji Watanabe.

At least 199 records · Page 11Linked to original sources

Strain-programmable exciton diffusion in moiré heterostructures

Moiré superlattices in van der Waals heterostructures have recently gained significant attention as an intriguing platform for studying correlated electronic systems and exotic excitonic properties. Previous reports, however, focused on creating and modulating moiré heterostructures through interlayer twisting or lattice constant mismatches, limiting controls on symmetry of heterostructures. In this work, we show that strain significantly alters the geometry of moiré superlattices by breaking the C3 rotational symmetry. We realize strain-induced moiré superlattices by intentionally regulating interlayer strain in WSe2-MoSe2 heterostructures, which is manifested by linearly polarized interlayer exciton emission coupled to the strain direction. Furthermore, interlayer exciton diffusion was preferentially guided along the stretched moiré superlattice orientations over a wide spatial range, reflecting the strain-modified moiré potentials. Our work highlights strain tuning as a versatile tool for designing moiré superlattices and programming excitonic transport, which opens pathways for van der Waals logic and information processing devices.

cond-mat.mes-hall↗

Layer-parity-dependent interfacial coupling in Nb$_3$Cl$_8$/graphene van der Waals heterostructures

Strongly correlated two-dimensional systems provide compelling platforms for investigating exotic quantum phenomena. Niobium chloride (Nb$_3$Cl$_8$), a single-band Mott insulator, exhibits a remarkable out-of-plane polarization in its topmost layer that oscillates with layer parity, manifesting as an odd-even effect. Using atomic force microscopy (AFM) and Kelvin probe force microscopy (KPFM), this layer-parity-dependent polarization can be effectively characterized through surface morphology and potential mapping, enabling the unambiguous identification of different surface phases. We then fabricated dual-gate Hall devices by coupling different surface phases of Nb$_3$Cl$_8$ with monolayer graphene to investigate how the topmost-layer out-of-plane polarization influences interfacial coupling and the resulting transport behavior. Our results reveal significant phase-dependent variations in charge transfer, carrier densities, and hybridization gaps (25.2 meV for Phase 1 and 30.0 meV for Phase 2). Density functional theory calculations corroborate these experimental findings, showing that distinct out-of-plane polarizations in the topmost layer lead to different orbital overlaps and interfacial coupling strengths. These findings highlight the critical importance of surface polarization and orbital orientation in engineering the properties of strongly correlated van der Waals heterostructures.

cond-mat.mtrl-sci↗

Layer-parity-defined surface polarization in Nb$_3$Cl$_8$ for excitonic modulation at van der Waals interfaces

The intrinsic symmetry breaking in the breathing kagome lattice of layered Nb$_3$Cl$_8$ provides a unique mechanism for realizing electrically polar surfaces. In each monolayer, the trimerization of Nb atoms breaks inversion and mirror symmetries, generating an out-of-plane electric dipole. The AB-stacked $α$ phase arranges adjacent layer dipoles antiferroelectrically, leaving the uncompensated surface polarization strictly governed by layer parity. Here, using atomic force microscopy operated in Kelvin probe force microscopy mode, we directly visualize layer-dependent polarization states in exfoliated Nb$_3$Cl$_8$ flakes and resolve a pronounced odd-even oscillation of the surface electrostatic potential. Beyond this parity-locked antiferroelectric order, we further identify intralayer polar domains in which local atomic reconstructions of the breathing kagome network reverse the out-of-plane dipole of the surface layer, producing ferroelectric-like stacking configurations. By interfacing monolayer MoSe$_2$ with Nb$_3$Cl$_8$, we demonstrate that these surface-polarization textures effectively modulate adjacent excitonic emission through domain-dependent interfacial band alignment and charge transfer. Our findings establish Nb$_3$Cl$_8$ as an intrinsic layer-polarized van der Waals platform and show that layer parity provides powerful structural degree of freedom for programming excitonic and optoelectronic responses at van der Waals interfaces.

cond-mat.mtrl-sci↗

Layer-Polarization-Driven Metal-Insulator Transition in multi-band Graphene Moire' Superlattices

Graphene/hBN moiré superlattices provide a highly tunable platform for exploring emergent quantum phases in low-dimensional systems. Here, we investigate the moiré superlattice formed between hBN and ABA-stacked trilayer graphene (TLG), an inherently multi-band system. We demonstrate that the moiré potential is not merely a perturbation but a tool to hybridize the distinct massless and massive electronic sectors of TLG. By applying a perpendicular displacement field to tune layer polarization, we drive a fundamental reconstruction of the electronic band structure. Specifically, increasing the displacement field evolves the system from a multi-band regime to an effectively single-band regime at low energies, accompanied by a metal--insulator transition at the hole-doped secondary Dirac point. This transition originates from a redistribution of carriers across graphene layers that selectively enhances their coupling to the extrinsic moiré potential. Quantum capacitance measurements provide direct evidence for the suppression of the density of states at the hole-side secondary Dirac point, consistent with gap opening and the emergence of a displacement-field-tuned band gap. Theoretical calculations reproduce these observations and identify layer-selective coupling to the moiré potential as the underlying mechanism. These results demonstrate electrical control of an emergent insulating phase in a low-dimensional moiré system, and highlight that layer polarization and layer-selective coupling in multi-band moiré heterostructures provide a powerful route for engineering topological and correlated phases through band structure reconstruction and electron interactions.

cond-mat.mes-hall↗

1/3 Fractional and Gapless Integer Quantum Anomalous Hall States in Rhombohedral Graphene

The fractional quantum anomalous Hall (FQAH) effect occurs in moiré superlattices in both twisted bilayer MoTe$_2$ and rhombohedral $n$-layer graphene aligned to hexagonal boron nitride (R$n$G/hBN) as a novel quantum phase driven by intertwined electron correlation and topology. Although several fractional states in the Jain sequence have been identified, the $1/3$ state, the most robust and fundamental state in conventional fractional quantum Hall (FQH) systems, was missing in either FQAH system. Determining whether it exists would have a major impact on understanding the mechanism of FQAH, especially in the theoretically still-debated R$n$G/hBN system. Here we report the FQAH effect at moiré filling factor $ν= 1/3$ in R$5$G/hBN moiré superlattice devices, through a combination of quantum capacitance and transport measurements. By tuning the displacement field, we observed a topological phase transition from a $1/3$ fractional Chern insulator (FCI) to a trivial charge density wave state. With the inclusion of the $1/3$ state, the FQAH states in R$5$G/hBN now exhibit a surprising level of particle-hole symmetry about half-filling, closely resembling the behavior of FQH states in the lowest Landau level. Additionally, we perform compressibility and transport measurements at a filling of one electron per moiré unit cell, $ν=1$, and also for $ν\lesssim 1$, where previous transport measurements displayed the extended quantum anomalous Hall (EQAH) effect. While our transport measurements show no change between the integer quantum anomalous Hall state (IQAH) and the EQAH region, compressibility measurements reveal a distinct transition from a gapped IQAH state to a gapless and highly compressible EQAH state. Our direct thermodynamic characterization of the rich phase diagram paves the way to engineering of anyon braiding and non-Abelian quasiparticles at zero magnetic field.

cond-mat.mes-hall↗

Fermiology and the Candidate Chiral Superconductor in Rhombohedral Tetralayer Graphene

Chiral superconductivity, in which the phase of the superconducting order parameter winds in momentum space, has long been sought for its close link to topological superconductivity. Recent work reported a superconductor in rhombohedral multilayer graphene emerging from a time-reversal symmetry broken normal state, suggesting that it could be a chiral superconductor. However, the possibility of chirality depends on the symmetry and structure of the normal-state Fermi surface, which have not been directly measured. Here we measure quantum oscillations in rhombohedral tetralayer graphene over a broad range of the phase diagram, including the superconducting region. At densities well above the onset of superconductivity, we reproduce previously-reported oscillations consistent with a spin- and valley-polarized quarter metal with a single simply-connected Fermi pocket. As the carrier density is reduced, we find a transition to a complex "multitone" state that persists through the superconducting region. This state's spectrum of quantum oscillations is incompatible with a simply-connected quarter metal. The next-simplest candidate normal states suggested by our microscopic modeling (fully-polarized annular, nematic, and three-pocket states) are inconsistent with our measurements, albeit difficult to rule out entirely. The normal state is thus seen to be richer than previously envisaged, reshaping the search for the superconducting mechanism and the possible chirality of the pairing channel.

cond-mat.supr-con↗

Fractional High-Chern Insulator in Twisted Rhombohedral Graphene

The realization of fractional Chern insulators opens up the possibility of exploring fractionally charged excitations and anyonic statistics in the absence of a magnetic field. A central question is whether lattice-based systems can give rise to radically new states, distinct from those observed in traditional fractional quantum Hall systems. In this work, we investigate a new type of moiré flat band system composed of Bernal bilayer graphene and rhombohedral tetralayer graphene. We discover an unprecedented richness of quantum anomalous Hall insulators with Chern numbers from C = 1 to C = 7 at v = 1 and around v = 3. Remarkably, we observe an exotic fractional Chern insulator with C = 7/3 around v = 2/3 which is beyond all known fractional Chern insulators described by either the Jain sequence or current high Chern theory. Our work expands the understanding of fractionally charged excitations beyond the Landau level basis and offers a new moire platform for exploring anyons.

cond-mat.mes-hall↗

Mechanochemical Nano-Writing of an Atomically Thin Metal

Mechanical energy accelerates many physicochemical processes, including materials syntheses that are hard to produce with thermal energy alone. However, physical understanding connecting applied mechanical forces with internal stresses and ensuing reaction mechanisms is lacking. Here we demonstrate mechanical force-enabled synthesis and nanoscale patterning to metallize a two-dimensional (2D) material, producing an atomically-thin superconducting material. Localized force applied by atomic force microscope tips to van der Waals (vdW) encapsulated stacks of 2D bilayer MoTe2 and adjacent source Pd guides 2D Pd7MoTe2 growth with 50 nm lateral resolution. Force accelerates reaction kinetics exponentially per Eyring's stress-assisted thermal activation model, reducing synthesis temperatures from ~200 °C to near-room temperature. Finite element simulations, density functional theory, and ab-initio grand canonical Monte Carlo calculations show that tip-induced compression facilitates Pd chemisorption to tensile-strained MoTe2 that converts to uniform Pd7MoTe2. This demonstrates a new, generalizable paradigm for nanoscale synthesis of quantum materials, and high-precision engineering of superconductivity.

cond-mat.mes-hall↗

Moiré enabled spin pumping and preservation in MoSe2/WS2 heterobilayers

The spin degree of freedom is a fundamental quantum mechanical attribute with implications spanning from magnetism to quantum computing. Consequently, the relaxation of spin states for extended, Bloch electrons in solids has been studied for decades as it defines many of their properties and applications. We show that moiré patterns in layered materials can extend spin relaxation times by two orders of magnitude to 1 millisecond and beyond. This is achieved by suppressing spin mixing for electrons in 2D semiconductor heterostructures, particularly in the MoSe2/WS2 system, as we elucidate both experimentally and theoretically. The extended longitudinal lifetime facilitates spin alignment over 50% using only nanowatt levels of optical power. Our findings highlight the potential of moiré engineering for future quantum sensing and information processing.

cond-mat.mes-hall↗

Ferroelectric-tunable quantum nonlinearity of chiral Bloch electrons in a moiré system

Sliding ferroelectricity in van der Waals materials shows great potential for designing robust memory devices. However, its thermodynamic behaviors and the coupling with certain quantum effects remain largely unexplored. Here, we demonstrate ferroelectric control over quantum nonlinear transport in a hexagonal boron nitride (hBN) encapsulated twisted double-bilayer graphene moiré heterostructure. The ferroelectricity is attributed to the presence of rhombohedral stacking in the top hBN, confirmed by both electrical transport and optical second harmonic generation (SHG) measurements. Remarkably, the polarization magnitude remains temperature-independent across 1.7-200 K, while nucleation time exhibits thermally activated behavior, decreasing with increasing temperature. Furthermore, we demonstrate a ferroelectric-switchable nonlinear Hall effect, attributed to the chiral scattering induced by Berry curvature, with outstanding fatigue-resistant and nonvolatility, demonstrating direct coupling between sliding ferroelectricity and quantum geometric properties. Our results establish sliding ferroelectrics as a platform for exploring electrically programmable Berry curvature physics.

cond-mat.mes-hall↗

Tailoring pure valley-Zeeman spin-orbit coupling in WSe$_2$-encapsulated monolayer graphene

Engineering proximity effects in twisted van der Waals heterostructures offers a powerful platform for designing electronic properties. While theoretical predictions of quantum interference in transition metal dichalcogenide-encapsulated graphene can selectively control the spin-orbit coupling component, experimental realizations have remained elusive. Here, we report pure valley-Zeeman spin-orbit coupling in monolayer graphene, achieved by encapsulation between two parallel twisted WSe$_2$ monolayers. We observed a symmetry-enforced reordering of Landau levels, which is driven by the competition between the fixed valley-Zeeman energy and the magnetic-field-dependent cyclotron energy. This reordering is characterized by a transition from symmetry-broken states in the quantum Hall effect to a restored fourfold degeneracy with integer or half-integer quantum Hall sequences. We also demonstrate the ability to completely quench the proximity spin-orbit coupling by tuning the encapsulated geometry.

cond-mat.mes-hall↗

Second-Order Synaptic Memory using Inherent Plasticity of Moiré Superlattices

Achieving synaptic functionality electronically in a single-element quantum material is a fundamental challenge, as conventional methods rely on the introduction of extrinsic charge-traps or polar components. Here, we demonstrate that twisted double bilayer graphene (tDBLG) moiré superlattices, composed purely of carbon, exhibit electronic hysteresis and plasticity in presence of twist-angle disorder. Inversion symmetry breaking at the moiré length scales also gives rise to second-order nonlinear electrical response via disorder-mediated extrinsic mechanisms. Such second-order nonlinearity is highly tunable in both sign and magnitude by varying carrier concentration and vertical displacement field. We harness the coexistence of electronic plasticity and second-order nonlinearity to realize a second-order synaptic memory device. Our findings establish strained moiré carbon systems as a powerful new platform for energy-efficient neuromorphic computing, demonstrating that complex electronic functionality can emerge purely from symmetry breaking physics in a single-element material.

cond-mat.mes-hall↗

Ferroelectric hysteresis in singly aligned graphene-hBN moiré superlattices

Ferroelectric materials have the unique ability to maintain an electric polarization which can be reversed under an external applied electric field. This property makes them valuable for applications such as non-volatile random-access memories, transducers, actuators and electro optic modulators. Recently, emergent unconventional ferroelectricity has been demonstrated in moiré superlattices of bilayer graphene and hexagonal boron nitride (hBN) hosting non centrosymmetric stacking order. Whether this phenomenon is also present in noncentrosymmetric single layer graphene (SLG)-hBN moiré superlattices is still under debate. Here we demonstrate a ferroelectric response in an SLG-hBN moiré superlattice. Through Hall measurements, we pinpoint the origin of the hysteretic behavior to abnormal charge screening due to the moiré superlattice band and estimate the spontaneous polarization magnitude in the moiré superlattice structure. Temperature dependent measurements confirm that the hysteretic behavior persists from 2K up to room temperature, opening opportunities for high-mobility, ultrathin non-volatile devices

cond-mat.mes-hall↗

Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers

We report light emission from the moire superlattice of a twisted bilayer of tungsten diselenide (WSe2/WSe2) encapsulated in insulating hexagonal boron nitride (hBN). The low-temperature photoluminescence (PL) spectroscopy reveals signatures of moire-potential induced strong interlayer excitonic emission and phonon-assisted recombination, while the twisting significantly suppresses the emission from localized defect-bound excitons. The moire potential redistributes carriers into indirect valleys, thereby enhancing recombination efficiency and stabilizing the interlayer excitons. Our findings establish that precise control of twist angle and dielectric environment provides a new route for engineering excitonic systems for exploring exciton-phonon interactions and associated quantum phenomena in transition metal dichalcogenides.

cond-mat.mes-hall↗

Noncollinear spin textures and 90° domain walls in twisted XY magnets

Twisted moiré magnets are promising in exploring noncollinear magnetic phases, yet current experimental studies have been restricted to uniaxial magnets, limiting the accessible phase space. Here, we demonstrate noncollinear moiré magnetism based on XY magnet CrCl3. The tunneling magnetoconductance of twisted CrCl3 exhibits multiple field-driven transitions in small-twist-angle devices, attributed to the coexisting antiferromagnetic and ferromagnetic domains with distinct susceptibilities. The inferred spin configuration depends on the layer number, reflecting the interlayer coupling strength between twisted layers. This moiré magnetism is remarkably robust, persisting up to twisted double nine-layer stacks. Combined with micromagnetic simulations, we identify the ground state as the predicted "twisted-s" phase featuring 90° domain walls. Finally, we demonstrate voltage control of these noncollinear phases, highlighting the electrically tunable twist-spintronics.

cond-mat.mes-hall↗

Impact of Disorder Dynamics and Multi-Domain Kinetics on the Sliding Ferroelectricity of CVD-Grown 3R-WSe2 Bilayers

Sliding ferroelectricity in van der Waals (vdW) layered systems has emerged as a promising route toward non-volatile nanoscale devices, where interlayer displacement in non-centrosymmetric bilayers generates an out-of-plane polarization. In particular, 3R-stacked bilayer transition metal dichalcogenides (TMDs) grown via chemical vapor deposition (CVD) have been shown to host such polarization due to broken inversion symmetry. However, a detailed investigation of the 2D ferroelectric (FE) properties of CVD-grown 2D films, particularly the role of intrinsic disorder, such as structural defects and domain structure, remains poorly understood. Here, we investigate the FE switching characteristics of CVD-grown 3R-stacked WSe2 using a graphene-based ferroelectric field-effect transistor (graphene-FE-FET) architecture, where graphene serves as a highly sensitive probe of induced charge modulation due to polarization switching of FEs. We show that the growth-induced structural disorder significantly impacts polarization switching, while multi-domain kinetics governs the evolution of the FE response. These findings provide important insights into the design and optimization of FE devices based on vdW materials.

cond-mat.mtrl-sci↗

Thickness-driven crossover from conventional to chiral nonreciprocal superconductivity in kagome metal CsV3Sb5

Superconductivity and its potential applications are governed by the symmetry of the superconducting order parameter. In the kagome metal CsV3Sb5, most bulk studies indicate conventional s-wave pairing. However, ultrathin flakes exhibit nonreciprocal transport, in particular a zero-field superconducting diode effect, which requires broken inversion and time-reversal symmetries. Here, using thickness dependent transport measurements, we observe the emergence of non-reciprocal second-harmonic magnetotransport signals and a zero-field superconducting diode effect, accompanied by a pronounced reduction of the out-of-plane coherence length with decreasing thickness. Upper critical field measurements further reveal a dimensional crossover from three-dimensional superconductivity in bulk to two-dimensional superconductivity in thin flakes. These findings indicate a thickness-induced chiral superconducting phase that breaks both inversion and time-reversal symmetries in the two-dimensional limit. Our work not only clarifies long-standing controversies regarding the pairing symmetry in CsV3Sb5, but also establishes thin-flake kagome superconductors as a versatile platform for engineering nonreciprocal quantum devices and exploring emergent topological phases.

cond-mat.supr-con↗

Topological spin-texture transitions in van der Waals magnets revealed by X-ray Fourier transform holography

Nontrivial topological spin-textures, such as skyrmions, merons, bimerons, and skyrmioniums, are envisioned as robust building blocks for future memory and logic devices. Controllable transformations between these states require a quantum-mechanical description of electronic degrees of freedom and atomic-scale insight beyond existing phenomenological models. Here, we report an atomic-scale investigation of topological phase transitions and their protection in the two-dimensional van der Waals ferromagnet Fe$_3$GeTe$_2$ (FGT) using a combined experimental-theoretical approach. Synchrotron-based Fourier transform holography directly images labyrinth domains, isolated skyrmions, mixed labyrinth-skyrmion phases, and skyrmion bags with high spatial resolution. We compare these observations to simulations based on an electronic lattice Hamiltonian that captures both metallicity and relativistic spin-orbit coupling in FGT. By systematically exploring a broad range of temperatures and magnetic fields, we map the mechanisms governing topological transitions and their stability. This sequential-integrated experimental-theoretical framework advances understanding of spin-texture interactions and enables precise control of external tuning parameters. Our results establish a platform for creating, stabilizing, and manipulating topological states, paving the way for engineered spin-texture transitions in next-generation spintronic technologies.

cond-mat.mtrl-sci↗