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Kenji Watanabe

Publications and source records attributed to Kenji Watanabe.

At least 109 records · Page 6Linked to original sources

Layer-Number-Controlled Symmetry Breaking and Surface-State Transport in Rhombohedral Graphene Multilayers

Rhombohedral multilayer graphene hosts layer-polarized flat bands, providing an intriguing platform for correlated and topological electronic states; however, the role of layer number in governing symmetry breaking and surface screening remains elusive. Here we prepare rhombohedral graphene multilayers and systematically conduct electrical transport measurements. We uncover an unconventional layer dependence of phase transitions: the critical displacement field (D$_{c}$) for the layer-antiferromagnetic (LAF)-to-semimetal transitions remains constant across tetralayer to hexalayer graphene, whereas the D$_{c}$ for semimetal-to-layer-polarized-insulator (LPI) transition increases with layer number, defying unscreened Coulomb interaction models. In hexalayer graphene, surface-state-dominated transport emerges, with Landau levels (LLs) and resistive peaks selectively controlled by adjacent gates, a signature of strong interlayer screening absent in thinner stacks. High magnetic fields reveal valley-layer-locked LLs and dissipative states possibly from interlayer backscattering, highlighting the presence of decoupled surface states. Our findings establish layer number as a key tuning knob for engineering correlated and topological phases in rhombohedral graphene multilayers.

cond-mat.mes-hall↗

Polarization engineered all 2D Graphene/Ferroelectric hybrid for persistence-free photoresponse

Graphene-based van der Waals hybrid photodetectors typically work on trap-mediated photogating mechanism, exhibiting high sensitivity, but under-perform in the fast detection of repetitive optical signals. Designing photodetectors that are simultaneously fast and highly sensitive has therefore remained difficult. In this work, we realize both attributes by integrating atomically thin sliding ferroelectrics in the design architecture, thereby uniting semiconducting properties with intrinsic polarization fields capable of efficiently governing interfacial photocarrier dynamics. We report a bilayer graphene-bilayer MoS2 (with MoS2 in a rhombohedrally stacked (3R) configuration) van der Waals photodetector with edge-contacted dual-gated field-effect transistor architecture. The photo-induced modulation in spontaneous out-of-plane polarization of 3R-MoS2 and selective confinement of charge carriers in bilayer graphene under an out-of-plane displacement field results in a tunable persistence-free photoresponse. Here, the photoinduced polarization change in 3R-MoS2 produces an optically controlled gating effect that alters the electrostatic environment of bilayer graphene, resulting in a temperature-independent photoresponse with rapid response times of the order of 10's of milliseconds (limited by the measurement instrument). We demonstrate reproducible detection of optical signals and examine the photon-counting resolution of this structure in high-sensitivity regimes, where we determine its internal quantum efficiency to be 10 percent with minimum detectable photon number of 31 in single shot measurements. This work highlights the functionality of 3R-MoS2 in manipulating the interfacial charge dynamics and establishes the hybrid of graphene and ferroelectric 3R-MoS2 as a promising platform for ultra-sensitive optoelectronic devices.

cond-mat.mes-hall↗

Thermodynamic evidence for interaction-driven first-order topological quantum phase transitions

Topological quantum phase transitions in non interacting systems occur through continuous gap closing and reopening. In strongly interacting systems, however, competing ordered states have long been predicted to drive first order transitions, although this possibility has remained experimentally unresolved. Recent transport studies of correlated phases in charge neutral rhombohedral graphene were interpreted as evidence for continuous topological transitions. Here, using nanoSQUID on tip magnetometry, we directly image the local orbital magnetization of a spin orbit proximitized rhombohedral graphene quantum anomalous Hall (QAH) state. We provide the first real space visualization of a QAH phase with a record Chern number, reconstruct its local thermodynamic gap, and track the evolution of its magnetization across competing correlated states. Combined with self consistent Hartree Fock calculations, these measurements show that the sequential transitions between the layer antiferromagnetic, QAH, and layer polarized insulating states are first order, accompanied by discontinuous changes in orbital magnetization. Near the phase boundaries, we observe fluctuating magnetic domains, providing direct microscopic evidence of phase coexistence between nearly degenerate competing ordered states. Together, these observations provide the first direct thermodynamic evidence for first order topological quantum phase transitions and establish a microscopic framework for understanding interaction driven topological quantum phase transitions through phase competition and coexistence.

cond-mat.mes-hall↗

Observation of metastable chiral domain walls in a topological magnet

The interplay between topology and correlation can give rise to exotic collective excitations. The integer and fractional quantum anomalous Hall (QAH) magnets recently discovered in two-dimensional (2D) flatband systems are predicted to host spin excitations distinct from those in conventional magnets. Experimentally, nevertheless, these new excitations remain largely unexplored. Here we investigate spin-valley excitations in a twisted MoTe2 moiré superlattice using resonant ultrafast pump-probe spectroscopy. We observe a metastable spin-valley excitation in the QAH magnet below T ~ 3.7 K that survives reverse magnetic field several times larger than the saturation field. The behavior of this excitation is sharply distinct from ordinary domain walls and magnons, indicating a new type of spin-valley textures unique to topological magnets. We propose that these textures are chiral domain walls with an in-plane winding of the pseudospin order parameter along the domain wall. Their metastability arises from the interplay between the topological winding in real space and the quantum geometry of the parent bands in momentum space through a universal mechanism. These chiral domain walls govern the nonequilibrium dynamics of QAH magnets and may play a central role in their stability. Our study highlights intrinsic quantum geometry effects on spin excitations in topological magnets; and provides key insights into the fundamental mechanism limiting stability of topological protection.

cond-mat.mes-hall↗

Strongly Enhanced Charge-Density Waves and Correlated Insulating State in Atomically Thin 1$T$-TaS$_2$

We investigate thickness-dependent charge-density-wave (CDW) transitions in 1$T$-TaS$_2$ using temperature-dependent Raman spectroscopy and electrical transport. Raman measurements show that the incommensurate, nearly commensurate, and commensurate CDW phases persist down to the monolayer limit. As the thickness is reduced, the transition temperatures increase, accompanied by an orders-of-magnitude rise in sheet resistance and a sharp reduction in the carrier localization length. The first-order hysteretic CCDW-NCCDW transition is uniquely absent in the monolayer. Calculations suggest that the enhanced CDW in thin layers originates from strengthened Coulomb interactions due to reduced out-of-plane screening, particularly in the nonlocal component. These findings highlight the cooperative roles of electron correlation, electron-phonon interaction, and interlayer coupling in shaping the ground state and transition dynamics of atomically thin 1$T$-TaS$_2$, opening pathways for engineering correlated phases in two-dimensional CDW systems.

cond-mat.str-el↗

Wigner polarons reveal Wigner crystal dynamics in a monolayer semiconductor

Wigner crystals, lattices made purely of electrons, are a quintessential paradigm of studying correlation-driven quantum phase transitions. Despite decades of research, the internal dynamics of Wigner crystals has remained extremely challenging to access, with most experiments probing only static order or collective motion. Here, we establish monolayer WSe2 as a new materials platform to host zero-field Wigner crystals and then demonstrate that exciton spectroscopy provides a direct means to probe both static and dynamic properties of these electron lattices. We uncover striking optical resonances that we identify as Wigner polarons, quasiparticles formed when the electron lattice is locally distorted by exciton-Wigner crystal coupling. We further achieve all-optical control of spins in the Wigner crystal, directly probing valley-dependent Wigner polaron scattering well above the magnetic ordering temperature and in the absence of any external magnetic field. Finally, we demonstrate optical melting of the Wigner crystal and observe intriguingly different responses of the umklapp (static) and Wigner polaron (dynamic) resonances to optical excitation. Our results open up exciting new avenues for elucidating electron dynamics and achieving ultrafast optical control of interaction-driven quantum phase transitions in strongly correlated electron systems.

cond-mat.mes-hall↗

Visualizing orbital magnetism in electron doped rhombohedral multilayer graphene

Electron doped rhombohedral multilayer graphene at high displacement field features an exceptionally flat band minimum with near-ideal quantum geometry. Experiments in this regime observe the formation of a 'quarter metal,' in which the electron liquid condenses into a single spin- and valley flavor. Remarkably, recent experiments have found a zero resistance state in the same region of the density- and displacement-field-tuned parameter space, attributed to the formation of a chiral superconductor from an orbitally ferromagnetic normal state. Here, we use nanoSQUID-on-tip magnetometry to map the orbital magnetization of electron-doped rhombohedral graphene devices ranging in thickness between 3 and 15 layers. Magnetization within the quarter metal phases peaks at finite density, consistent with concentration of the Berry curvature in a finite-momentum 'ring of fire'. Correlating transport and local magnetometry data in a superconducting tetralayer sample reveals a finite orbital ferromagnetic moment, providing direct evidence of valley polarization in the superconducting ground state. We further show that widely observed stochastic switching of the resistivity in both metallic and superconducting regimes arises from a density-tuned sign change in the valley-resolved total magnetic moment. This leads to the formation of metastable magnetic domains under typical gate control sequences and can also be harnessed for electric-field controlled switching of the magnetization across the entire device. Finally, high resolution measurements of the magnetization across a superconducting transition allow us to put an upper bound on the 'condensation magnetization' of 0.1 Bohr magneton per carrier, placing a strong quantitative restriction on theoretical models for ferromagnetic superconductivity.

cond-mat.mes-hall↗

Counterdirectional Exciton and Trion Motion in Applied Electric Field

Charged excitonic complexes are central to the optoelectronic and many-body properties of semiconductors, yet their real-space transport dynamics remain largely unexplored. Here, we report the direct optical observation of trion motion under an applied electric field. The trions exhibit electrically driven drift with velocities approaching {$10^5~\mathrm{m/s}$}. Unexpectedly, the trion flow induces a pronounced back-action on coexisting neutral excitons, driving them in the opposite direction and giving rise to counterpropagating exciton-trion transport. Our results reveal an interaction-driven nonequilibrium transport regime of mixed excitonic fluids and establish a direct route for imaging the dynamics of more complex charged quasiparticles, including doubly charged excitons.

physics.optics↗

Correlating spin and optical properties of quantum emitters in hBN

Optically addressable spin defects in hexagonal boron nitride (hBN) are well suited for near-surface quantum sensing. They offer bright, wavelength-tunable single-photon emission with high optically detected magnetic resonance (ODMR) contrast at room temperature. Here we controllably synthesise a high density of spin-complex defects in carbon-doped hBN flakes. We find that the zero-field splitting parameter D is directly correlated with the zero-phonon line of an emitter, while the ODMR contrast shows no such correlation. We further analyse an individual narrowband defect showing 68% ODMR contrast and enhance its photon collection by ~40% using a solid immersion lens. By advancing both the practical synthesis of the spin complexes and the understanding of their microscopic origin, our results move us toward the deterministic creation of ODMR-active quantum emitters

quant-ph↗

Alloy engineering of excitonic properties in TMD monolayers

We investigate monolayer MoS$_{2x}$Se$_{2(1-x)}$ alloys across the full composition range using optical spectroscopy. We demonstrate continuous tuning of the optical gap over $\sim$0.35 eV, accompanied by a systematic reduction of the B--A exciton splitting, in agreement with density functional theory calculations. Temperature-dependent measurements reveal a progressive increase of the average phonon energy from Se-rich to S-rich alloys that follows a simple reduced-mass scaling model. Polarization-resolved spectroscopy further shows a monotonic increase of the circular polarization from nearly zero in MoSe$_2$ to $\sim$15\% in MoS$_2$ at 78 K. The observed evolution of the polarization is attributed to alloy-induced modifications of the electronic structure that modify bright--dark exciton mixing and the associated valley depolarization. These findings establish alloy engineering as an effective strategy for controlling excitonic properties in TMD monolayers.

cond-mat.mtrl-sci↗

Surface-Selective Probe of Spin-Triplet Superconductivity in Rhombohedral Graphene

Superconductivity in rhombohedral graphene has been observed across many layer numbers, with mounting evidence pointing toward spin-triplet pairing, yet complementary probes of the superconducting spin structure remain needed. Here we use one-sided WS$_2$ proximity in rhombohedral pentalayer graphene (R5G) as a surface-selective spin-orbit probe. The induced Ising spin-orbit coupling is strongest for carriers localized near the WS$_2$ interface, allowing the displacement field to tune the overlap between superconducting carriers and the spin-orbit perturbation. We observe a strongly asymmetric superconducting landscape: two robust pockets, SC1 and SC2, survive only on mutually opposite signs of displacement field, while a third pocket, SC3, is substantially weaker. Gate-tracking features, quantum oscillations, and self-consistent band-structure calculations identify the layer polarization and Fermi-surface character of the relevant carriers. The robust superconducting states are absent or strongly weakened when the active high-DOS carriers are polarized toward the WS$_2$ interface. Since Ising spin-orbit coupling is compatible with time-reversed spin-singlet pairing but competes with same-spin intervalley triplet pairing by canting or pinning the parent spin texture, this surface-selective suppression provides additional evidence for spin-triplet superconductivity involving both hole-like and electron-like carriers. Our results establish one-sided TMD proximity as a displacement-field-tunable probe of superconducting spin structure in rhombohedral graphene.

cond-mat.mes-hall↗

Valley polarization of moiré interlayer exciton complexes driven by many-body interactions

Localized interlayer excitons (IX) in moiré transition metal dichalcogenide heterostructures can both probe and participate in many-body states hosted by the moiré superlattice. When the IX density is small compared to the moiré lattice density, the formation of incompressible charge crystals at fractional electronic moiré fillings modifies exciton-charge scattering, leading to enhanced lifetimes in photoluminescence (PL) measurements. At high IX densities, the exciton dynamics are altered by the emergence of an excitonic Mott insulator and the formation of doubly-occupied sites (IXX). Here, we investigate the IX PL lifetime and valley polarization in an R-type $\mathrm{WSe_2}$/$\mathrm{WS_2}$ bilayer across a wide range of IX and charge densities. While previous studies reported a decrease of polarization in time-integrated measurements in charge-incompressible phases, our results show that this arises not from enhanced intervalley scattering, but from a dilution of the valley polarization by the dramatic enhancement of IX lifetimes. At high excitation densities, we probe the dynamics of the IXX and show that despite the nominal antiparallel valley configuration of the two constituent excitons, a strong, anomalous valley polarization develops as the IXX population decays. Our results shed light on the complex exciton and valley dynamics of IX and demonstrate that they are strongly modified by the rich many-body physics of moiré heterobilayers.

cond-mat.mes-hall↗

Magnetic Field Reorganization of Electronic States in Moiré Bilayer Graphene

Magnetic fields are widely used to diagnose quantum phases in two-dimensional systems through quantum oscillations or by tuning spin and valley polarizations, but magnetic fields can also reshape the underlying electronic structure. Here, using a bilayer graphene/hBN moiré system, we reveal a rich magnetic field induced evolution of the semiclassical orbit network, encompassing Lifshitz transitions, magnetic breakdown, and scattering between coexisting electron and hole pockets. At magnetic fields of 1 T to 2 T, quantum oscillation frequencies and the Hall density change markedly over a broad carrier density range, signaling magnetic breakdown and magnetic Lifshitz transitions. This evolution is valley contrasting: Berry curvature hot spots near the breakdown junctions enhance magnetic breakdown in the K valley while suppressing it in the K$^\prime$ valley, whereas valley-antisymmetric orbital magnetic moments split the corresponding Lifshitz transitions. The resulting valley-selective trajectories manifest at higher fields as valley-symmetry-breaking Hofstadter gaps. At elevated temperatures and low magnetic fields, scattering between coexisting electron and hole pockets produces nearly density-independent resistance oscillations whose frequency tracks the sum of their Fermi surface areas, persisting after conventional Onsager oscillations are thermally washed out. Our results provide a unified picture of how modest magnetic fields reorganize moiré electronic states as the system evolves from semiclassical transport toward the Hofstadter regime.

cond-mat.mes-hall↗

Layer-Hybridized Wigner Crystals in MoSe2/WS2 Moiré Superlattice

Transition metal dichalcogenide moiré heterobilayers with type-II band alignment provide a versatile platform for layer-polarized generalized Wigner crystals, in which strong Coulomb interactions drive charge ordering at fractional lattice fillings. With a finite interlayer band offset, an out-of-plane electric field can tune layer-resolved moiré bands through resonance and enable controllable interlayer hybridization. Although hybridized Mott insulators have been previously demonstrated, whether fractional charge-ordered states can survive such hybridization remains elusive. Here we drive an H-stacked MoSe2/WS2 moiré heterobilayer through a type-I-to-type-II band-alignment transition and realize layer-hybridized Mott insulator and generalized Wigner crystals. For fillings below one electron per moiré cell, tunneling delocalizes electrons and modifies Wigner crystallization. However, above one electron per cell, Coulomb repulsion overcomes tunneling and favors layer-separated occupation, stabilizing stronger charge-ordered states. These results establish electrically tunable hybridized moiré heterobilayers as a powerful platform for engineering correlated charge order and exploring fractional Chern phases and emergent magnetism.

cond-mat.mes-hall↗

Dual-Mode Exciton Coupling in Epitaxially Registered Organic-Inorganic 2D Heterocrystals

Two-dimensional (2D) heterocrystals comprising molecules and semiconductors can serve as an ideal platform for studying interfacial excitons and for future optoelectronic applications, yet the energy and charge flow across these atomically sharp interfaces remain unclear. In this work, we investigated PTCDA-MoS2 as a prototypical 2D organic-inorganic heterostructure and revealed dual-mode exciton coupling between the constituent crystals. Monolayer-resolved PTCDA molecular crystals were grown on monolayer MoS2 via physical vapor assembly, and their crystallographic details, including the stacking angle, were determined by electron diffraction. Upon the formation of the heterostructures, PTCDA's photoluminescence was completely quenched because of organic-to-inorganic hole transfer, whereas that of MoS2 increased markedly with PTCDA thickness. Using differential reflectance and photoluminescence excitation spectroscopy, we found that the enhancement arises from two distinct mechanisms. Ground-state charge transfer injects holes into MoS2, which suppresses negative trion formation and enhances the radiative recombination of neutral excitons. In addition, resonant energy transfer, enabled by spectral overlap between PTCDA and MoS2, diverts excitation energy from PTCDA to MoS2. Our findings reconcile previously proposed mechanisms and establish a unified framework in which charge and energy transfer cooperate to govern exciton coupling at organic-inorganic interfaces.

cond-mat.mtrl-sci↗

Charge Tunable Optical Nonlinearity of Moiré Exciton-Polaritons

Transition metal dichalcogenides represent a versatile platform to study strong light-matter interactions based on excitons and electrons in ordered lattices. Twist-engineering of moiré structures further enables the manipulation of the polaritonic nonlinearities via engineering the exciton landscape on the nanoscale. In this work, we demonstrate in-situ control of the optical saturation-based nonlinearity of moiré exciton-polaritons by phase space restriction via charge doping. Strong exciton-photon coupling is established in a gate-controllable MoTe$_2$-MoSe$_2$ heterobilayer, embedded in a spectrally-tunable open cavity. A small gate voltage can effectively lower the necessary polariton density by one order of magnitude to achieve a similar nonlinear saturation effect as in the charge-neutral case. Our microscopic description successfully explains the observed phenomena in the framework of Pauli blocking for the moiré superlattices with charge preoccupation.

cond-mat.mes-hall↗

Optical switching of magnetic order in few-layer CrSBr

Manipulating magnetism with light is crucial for both fundamental understanding and technological advancements of information storage devices. The layered antiferromagnet CrSBr, part of the recently emerging class of two-dimensional van der Waals magnets, offers a unique path towards optical control of magnetism via magneto-excitons, which allow optical readout of the spin alignment and also provide a strong absorption channel. Here, we use exciton absorption and photoluminescence to demonstrate optical switching of the magnetic order in bi- and trilayer CrSBr. Using a continuous-wave laser with a power as low as a few microwatts at near-critical external magnetic fields, we demonstrate both local and remote switching of the magnetic configuration in extended lateral domains and further employ this mechanism to deterministically prepare the zero-field magnetic configuration. Our results establish optical switching as a useful means of controlling magnetism in CrSBr, with potential applications in magneto-optoelectronic devices.

cond-mat.mes-hall↗

Lifshitz transitions and isospin polarization in twist-decoupled monolayer-bilayer graphene

Bernal-stacked bilayer graphene (BLG) hosts correlated electronic phases tied to low-energy Lifshitz transitions at saddle points in its valence band. To access this regime, ultralow charge disorder and control over a vertical electric field are simultaneously required. Here, we employ a twist-decoupled monolayer (MLG) to bias a proximal BLG in the absence of an external displacement field (D). We thereby reveal three-fold degenerate quantum Hall states at D = 0, with multiple transitions driven by doping, magnetic and electric field. Spontaneous broken symmetry in the vicinity of the valence band edge is signaled by the emergence of quantum oscillations with anomalous frequencies and large quasiparticle mass. These results indicate that electronic interactions in BLG are preserved in presence of an atomically close MLG, while showcasing the potential of CVD-grown graphene multilayers for the exploration of correlated phases of matter.

cond-mat.mes-hall↗