arXiv subjects

Kenji Watanabe

Publications and source records attributed to Kenji Watanabe.

At least 595 records · Page 33Linked to original sources

arXiv2025

Quantifying hydrogen bonding using electrically tunable nanoconfined water

Hydrogen bonding plays a crucial role in biology and technology, yet it remains poorly understood and quantified despite its fundamental importance. Traditional models, which describe hydrogen bonds as electrostatic interactions between electropositive hydrogen and electronegative acceptors, fail to quantitatively capture bond strength, directionality, or cooperativity, and cannot predict the properties of complex hydrogen-bonded materials. Here, we introduce a novel approach that conceptualizes the effect of hydrogen bonds as elastic dipoles in an electric field, which captures a wide range of hydrogen bonding phenomena in various water systems. Using gypsum, a hydrogen bond heterostructure with two-dimensional structural crystalline water, we calibrate the hydrogen bond strength through an externally applied electric field. We show that our approach quantifies the strength of hydrogen bonds directly from spectroscopic measurements and reproduces a wide range of key properties of confined water reported in the literature. Using only the stretching vibration frequency of confined water, we can predict hydrogen bond strength, local electric field, O-H bond length, and dipole moment. Our work also introduces hydrogen bond heterostructures - a new class of electrically and chemically tunable materials that offer stronger, more directional bonding compared to van der Waals heterostructures, with potential applications in areas such as catalysis, separation, and energy storage.

cond-mat.mes-hall↗

arXiv2025

Superlative spin transport of holes in ultra-thin black phosphorus

The development of energy-efficient spin-based hybrid devices that can perform functions such as logic, communication, and storage requires the ability to control and transport highly polarized spin currents over long distances in semiconductors. While traditional semiconductors such as silicon support spin transport, the effects of carrier type and concentration on important spin parameters are not well understood due to the need for extrinsic doping, which can cause additional momentum and hence spin scattering. Two-dimensional semiconductors, on the other hand, offer the ability to tune carrier type and concentration through field effect gating and inherently have long intrinsic spin lifetimes, making them a desirable platform for spin transport. Here, we study gate-tunable spin transport across narrow band-gap black phosphorus-based spin valves which enable us to systematically investigate spin transport with varying hole and electron concentrations under non-local geometry. Our findings demonstrate exceptional pure spin transport that approaches intrinsic limit, particularly in the low hole doping range. We achieved record non-local signals reaching 350 Ω and spin lifetimes exceeding 16 ns. Contrary to the behaviour seen in typical semiconductors, we find that the spin transport performance of holes in black phosphorus is significantly better than that of electrons, with the Elliott-Yafet process being the primary spin scattering mechanism. The observation of gate-tunable nanosecond spin lifetimes and colossal pure spin signals in both p- and n-type black phosphorus offers promising prospects for the development of novel semiconducting spintronics devices requiring sharp p-n interfaces.

cond-mat.mes-hall↗

arXiv2025

Signatures of Chiral Superconductivity in Rhombohedral Graphene

Chiral superconductors are unconventional superconducting states that break time reversal symmetry spontaneously and typically feature Cooper pairing at non-zero angular momentum. Such states may host Majorana fermions and provide an important platform for topological physics research and fault-tolerant quantum computing. Despite intensive search and prolonged studies of several candidate systems, chiral superconductivity has remained elusive so far. Here we report the discovery of robust unconventional superconductivity in rhombohedral tetra- and penta-layer graphene in the absence of moiré superlattice effects. We observed two superconducting states in the gate-induced flat conduction bands with Tc up to 300 mK and charge density ne as low as 2.4*1011 cm-2 in three tetralayer and two pentalayer devices. Spontaneous time-reversal-symmetry-breaking (TRSB) due to electron's orbital motion is found, and several observations indicate the chiral nature of these superconducting states, including: 1. In the superconducting state, Rxx shows magnetic hysteresis in varying out-of-plane magnetic field B, which is absent from all other superconductors; 2. the superconducting states are immune to in-plane magnetic field and are developed within a spin- and valley-polarized quarter-metal phase; 3. the normal states show anomalous Hall signals at zero magnetic field and magnetic hysteresis. We also observed a critical B of up to 1.4 Tesla, higher than any graphene superconductivity reported so far and indicates a strong-coupling superconductivity close to the BCS-BEC crossover. Our observations establish a pure carbon material for the study of topological superconductivity, and pave the way to explore Majorana modes and topological quantum computing.

cond-mat.mes-hall↗

arXiv2025

Density-dependent spin susceptibility and effective mass in monolayer MoSe2

Atomically thin MoSe2 is a promising platform for investigating quantum phenomena due to its large effective mass, high crystal quality, and strong spin-orbit coupling. In this work, we demonstrate a triple-gate device design with bismuth contacts, enabling reliable ohmic contact down to low electron densities, with a maximum Hall mobility of approximately 22,000 cm2/Vs. Low-temperature transport measurements illustrate metal-insulator transitions, and density-dependent quantum oscillation sequences. Enhanced spin susceptibility and density-dependent effective mass are observed, attributed to interaction effects and valley polarization. These findings establish monolayer MoSe2 as a versatile platform for further exploring interaction-driven quantum states.

cond-mat.mes-hall↗

arXiv2025

A Van der Waals Moiré Bilayer Photonic Crystal Cavity

Enhancing light-matter interactions with photonic structures is critical in classical and quantum nanophotonics. Recently, Moiré twisted bilayer optical materials have been proposed as a promising means towards a tunable and controllable platform for nanophotonic devices, with proof of principle realisations in the near infrared spectral range. However, the realisation of Moiré photonic crystal (PhC) cavities has been challenging, due to a lack of advanced nanofabrication techniques and availability of standalone transparent membranes. Here, we leverage the properties of the van der Waals material hexagonal Boron Nitride to realize Moiré bilayer PhC cavities. We design and fabricate a range of devices with controllable twist angles, with flatband modes in the visible spectral range (~ 450 nm). Optical characterization confirms the presence of spatially periodic cavity modes originating from the engineered dispersion relation (flatband). Our findings present a major step towards harnessing a two-dimensional van der Waals material for the next-generation of on chip, twisted nanophotonic systems.

physics.optics↗

arXiv2025

Unveiling resilient superconducting fluctuations in atomically thin NbSe$_2$ through Higgs mode spectroscopy

We report a combined electrical transport and optical study of the superconductivity in atomically thin NbSe$_2$. When subjected to an out-of-plane magnetic field, an anomalous metallic state emerges, characterized by a finite longitudinal resistance and a vanishing Hall resistance, suggesting the presence of particle-hole symmetry. We establish a superconducting Higgs mode in atomically thin samples, which reveals enduring superconducting fluctuations that withstand unexpectedly high reduced magnetic fields. These findings provide evidence of robust locally paired electrons in the anomalous metallic state, affirming its bosonic nature.

cond-mat.supr-con↗

arXiv2025

Spin-valley locked excited states spectroscopy in a one-particle bilayer graphene quantum dot

Current semiconductor qubits rely either on the spin or on the charge degree of freedom to encode quantum information. By contrast, in bilayer graphene the valley degree of freedom, stemming from the crystal lattice symmetry, is a robust quantum number that can therefore be harnessed for this purpose. The simplest implementation of a valley qubit would rely on two states with opposite valleys as in the case of a single-carrier bilayer graphene quantum dot immersed in a small perpendicular magnetic field ($B_\perp\lesssim 100$mT). However, the single-carrier quantum dot excited states spectrum has not been resolved to date in the relevant magnetic field range. Here, we fill this gap, by measuring the parallel and perpendicular magnetic field dependence of this spectrum with an unprecedented resolution of $4μ$eV. We use a time-resolved charge detection technique that gives us access to individual tunnel events. Our results come as a direct verification of the predicted spectrum and establish a new upper-bound on inter-valley mixing, equal to our energy resolution. Our charge detection technique opens the door to measuring the relaxation time of a valley qubit in a single-carrier bilayer graphene quantum dot.

cond-mat.mes-hall↗

arXiv2025

Quadrupolar Excitons in MoSe$_2$ Bilayers

The quest for platforms to generate and control exotic excitonic states has greatly benefited from the advent of transition metal dichalcogenide (TMD) monolayers and their heterostructures. Among the unconventional excitonic states, quadrupolar excitons - a superposition of two dipolar excitons with anti-aligned dipole moments - are of great interest for applications in quantum simulations and for the investigation of many-body physics. Here, we unambiguously demonstrate the emergence of quadrupolar excitons in natural MoSe$_2$ homobilayers, whose energy shifts quadratically in electric field. In contrast to trilayer systems, MoSe$_2$ homobilayers have many advantages, which include a larger coupling between dipolar excitons. Our experimental observations are complemented by many-particle theory calculations offering microscopic insights in the formation of quadrupolar excitons. Our results suggest TMD homobilayers as ideal platform for the engineering of excitonic states and their interaction with light and thus candidate for carrying out on-chip quantum simulations.

cond-mat.mes-hall↗

arXiv2025

Spin-Valley Protected Kramers Pair in Bilayer Graphene

The intrinsic valley degree of freedom makes bilayer graphene (BLG) a unique platform for semiconductor qubits. The single-carrier quantum dot (QD) ground state exhibits a two-fold degeneracy, where the two states that constitute a Kramers pair, have opposite spin and valley quantum numbers. Because of the valley-dependent Berry curvature, an out-of-plane magnetic field breaks the time-reversal symmetry of this ground state and a qubit can be encoded in the spin-valley subspace. The Kramers states are protected against known spin- and valley-mixing mechanisms because mixing requires a simultaneous change of both quantum numbers. Here, we fabricate a tunable QD device in Bernal BLG and measure a spin-valley relaxation time for the Kramers states of ${38~\mathrm{s}}$, which is two orders of magnitude longer than the ${0.4~\mathrm{s}}$ measured for purely spin-blocked states. We also show that the intrinsic Kane-Mele spin-orbit splitting enables a Kramers doublet single-shot readout even at zero magnetic field with a fidelity above ${99\%}$. If these long-lived Kramers states also possess long coherence times and can be effectively manipulated, electrostatically defined QDs in BLG may serve as long-lived semiconductor qubits, extending beyond the spin qubit paradigm.

cond-mat.mes-hall↗

arXiv2025

Preserving Twist-Angle in Marginally Twisted Double-Bilayer Graphene Devices During Fabrication

Twisted van der Waals heterostructures provide a platform for studying a wide range of electron correlation phenomena, including unconventional superconductivity and correlated insulating states. However, fabricating such devices is challenging due to the difficulty in achieving and maintaining homogeneous twist-angles. Here, we present a fabrication method to preserve the twist-angle with minimal deformation. We fabricated marginally twisted double-bilayer graphene (mTDBG) stacks and directly imaged the resulting triangular superlattice periodicity via scattering-type scanning near-field optical microscopy (s-SNOM). This technique enabled us to monitor twist-angle deformation at each fabrication step, paving the way for more reliable device fabrication and facilitating the exploration of twist-angle-dependent physics.

cond-mat.mes-hall↗

arXiv2025

Kerr non-linearity enhances the response of a graphene Josephson bolometer

Highly sensitive, broadband bolometers are of great interest because of their versatile usage in wide areas starting from dark matter search, radio astronomy, material science, and qubit readouts in cQED experiments. There have been different realizations of bolometers using superconducting thin films, nanowires, quantum dots, and various 2D materials in the recent past. The challenge is to have a single device that combines high sensitivity, broad bandwidth, a fast readout mechanism, and low noise. Here we demonstrate the first usage of a Josephson parametric amplifier (JPA) as a highly sensitive bolometer. Our key finding is the Kerr non-linearity of the JPA boosts the device's sensitivity. When the bolometer is biased in the non-linear regime, it enhances the sideband signals (~100 times), resulting in an order of magnitude improvement in sensitivity compared to the linear regime. In the non-linear biasing of the device, we achieve a NEP~500 aW/sqrt(Hz). Our bolometer offers a fast detection scheme with a thermal time constant of 4.26 us and an intrinsic JPA time constant of 70 ns. Our device's broadband and fast operation are key and new compared to previously studied graphene-based bolometers. In our device, the gate voltage tunability and the possibility of multiplexing combined with the sensitive bolometric performance offer an opportunity for integrated quantum sensor arrays. Our work demonstrates a way forward to enhance the performance of quantum sensors based on 2D materials by leveraging the inherent non-linear response.

cond-mat.mes-hall↗

arXiv2025

Electric field tunable bands in doubly aligned bilayer graphene hBN moire superlattice

In this letter, we demonstrate electric field-induced band modification of an asymmetrically twisted hBN/BLG/hBN supermoire lattice. Distinct from unaligned BLG/hBN systems, we observe regions in the density-displacement field (n-D) plane where the device conductance is independent of n and decreases as |D| increases. This distinction arises due to the angle asymmetry between the layers, which induces field-controlled layer polarization. We identify D-dependent additional band gaps near the charge neutrality point that appear in the conduction (valence) band for negative (positive) D values. In the quantum Hall regime, new 6-fold degenerate Landau levels are observed. Our findings establish that in an asymmetric supermoire heterostructure, an external vertical displacement field affects the valence and conduction bands very differently and sheds light on the asymmetric conductance patterns noted in previous studies.

cond-mat.mes-hall↗

arXiv2025

Experimental signature of layer skyrmions and implications for band topology in twisted WSe2 bilayers

Transition metal dichalcogenide (TMD) twisted homobilayers have been established as an ideal platform for studying strong correlation phenomena, as exemplified by the recent discovery of fractional Chern insulator (FCI) states in twisted MoTe2 and Chern insulators (CI) and unconventional superconductivity in twisted WSe2 (tWSe2). In these systems, nontrivial topology in the strongly layer-hybridized regime can arise from a spatial patterning of interlayer tunneling amplitudes and layer-dependent potentials that yields a lattice of layer skyrmions. Here we report on experimental signatures of skyrmion textures in the layer degree of freedom of Rhombohedral-stacked (R-stacked) tWSe2 homobilayers. This observation is based on scanning tunneling spectroscopy that separately resolves the Gamma-valley and K-valley moiré electronic states. We show that Gamma-valley states are subjected to a moiré potential with an amplitude of ~ 120 meV. At ~150 meV above the Gamma-valley, the K-valley states are subjected to a weaker moiré potential of ~30 meV. Most significantly, we reveal opposite layer polarizations of the K-valley at the MX and XM sites within the moiré unit cell, confirming the theoretically predicted layer skyrmion texture. The dI/dV mappings allow the parameters that enter the continuum model of moiré bands in twisted TMD bilayers to be determined experimentally, further establishing a direct correlation between the shape of the LDOS profile in real space and the topology of topmost moiré band.

cond-mat.mes-hall↗

arXiv2025

Impact of Spin-Orbit Coupling on Superconductivity in Rhombohedral Graphene

Spin-orbit coupling (SOC) has played an important role in many topological and correlated electron materials. In graphene-based systems, SOC induced by transition metal dichalcogenide (TMD) at proximity was shown to drive topological states and strengthen superconductivity. However, in rhombohedral multilayer graphene, a robust platform for electron correlation and topology, superconductivity and the role of SOC remain largely unexplored. Here we report transport measurements of TMD-proximitized rhombohedral trilayer graphene (RTG). We observed a new hole-doped superconducting state SC4 with Tc = 230 mK. On the electron-doped side, we identified a new isospin-symmetry breaking three-quarter-metal (TQM) phase and observed the nearby weak superconducting state SC3 is significantly enhanced. Surprisingly, the original superconducting state SC1 in bare RTG is strongly suppressed in the presence of TMD - opposite to the effect of SOC on all other graphene superconductivities. Our observations form the basis of exploring superconductivity and non-Abelian quasiparticles in rhombohedral graphene devices.

cond-mat.supr-con↗

arXiv2025

Tunable Fractional Chern Insulators in Rhombohedral Graphene Superlattices

Fractional Chern insulators (FCIs) showing a transport effect with fractionally quantized Hall plateaus emerging under zero magnetic field, provide a radically new opportunity to engineer topological quantum electronics. By construction of topological flat band with moire engineering, intrinsic FCIs have been observed in twisted MoTe2 system and rhombohedral pentalayer graphene/hBN moire superlattices with anomalous Hall resistivity quantization number C <= 2/3 including the gapless composite Fermi-liquid state with C = 1/2. Here, we experimentally demonstrate a new system of rhombohedral hexalayer graphene (RHG)/hBN moire superlattices, which exhibit both integer and fractional quantum anomalous Hall effects with rich tunability including electric displacement field, perpendicular magnetic field and in-plane magnetic field. By tuning the electrical and magnetic fields at 0 < v < 1, we have observed a quantum phase transition showing a sign reversal of the Hall resistivity at finite magnetic fields. Surprisingly, the FCI state at v = 2/3 survives in the phase transitions, exhibiting a robust quantized Hall resistivity across both phases. Finally we have further demonstrated the indispensable role moire potential plays in the formation of the flat Chern band from a theoretical perspective. Our work has established RHG/hBN moire superlattices as a promising platform for exploring quasi-particles with fractional charge and non-Abelian anyons at zero magnetic field.

cond-mat.mes-hall↗

arXiv2025

Competition between excitonic insulators and quantum Hall states in correlated electron-hole bilayers

Excitonic insulators represent a unique quantum phase of matter, providing a rich ground for studying exotic quantum bosonic states. Strongly coupled electron-hole bilayers, which host stable dipolar exciton fluids with an exciton density that can be adjusted electrostatically, offer an ideal platform to investigate correlated excitonic insulators. Based on electron-hole bilayers made of MoSe2/hBN/WSe2 heterostructures, here we study the behavior of excitonic insulators in a perpendicular magnetic field. We report the observation of excitonic quantum oscillations in both Coulomb drag signals and electrical resistance at low to medium magnetic fields. Under a strong magnetic field, we identify multiple quantum phase transitions between the excitonic insulator phase and the bilayer quantum Hall insulator phase. These findings underscore the interplay between the electron-hole interactions and Landau level quantization that opens new possibilities for exploring quantum phenomena in composite bosonic insulators.

cond-mat.mes-hall↗

arXiv2025

Charge state tuning of spin defects in hexagonal boron nitride

Boron vacancies in hexagonal boron nitride (hBN) are among the most extensively studied optically active spin defects in van der Waals crystals, due to their promising potential to develop two-dimensional (2D) quantum sensors. In this letter, we demonstrate the tunability of the charge state of boron vacancies in ultrathin hBN layers, revealing a transition from the optically active singly negatively charged state to the optically inactive doubly negatively charged state when sandwiched between graphene electrodes. Notably, there is a photoluminescence quenching of a few percent upon the application of a bias voltage between the electrodes. Our findings emphasize the critical importance of considering the charge state of optically active defects in 2D materials, while also showing that the negatively charged boron vacancy remains robust against external perpendicular electric fields. This stability makes it a promising candidate for integration into various van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

Spin-forbidden excitations in the magneto-optical spectra of CrI$_3$ tuned by covalency

Spin-forbidden ($ΔS \neq 0$) multiplet excitations and their coupling to magnetic properties are of increasing importance for magneto-optical studies of correlated materials. Nonetheless, the mechanisms for optically brightening these transitions and their generality remain poorly understood. Here, we report magnetic circular dichroism (MCD) spectroscopy on the van der Waals (vdW) ferromagnet (FM) CrI$_3$. Previously unreported spin-forbidden ($ΔS = 1$) ${}^4A_{2\mathrm{g}} \to{}^2E_\mathrm{g}/{}^2T_{1\mathrm{g}}$ Cr${}^{3+}$ $dd$ excitations are observed near the ligand-to-metal charge transfer (LMCT) excitation threshold. The assignment of these excitations and their Cr$^{3+}$ multiplet character is established through complementary Cr $L_3$-edge resonant inelastic X-ray scattering (RIXS) measurements along with charge transfer multiplet (CTM) calculations and chemical trends in the chromium trihalide series (CrX$_3$, X = Cl, Br, I). We utilize the high sensitivity of MCD spectroscopy to study the thickness dependent optical response. The spin-forbidden excitations remain robust down to the monolayer limit and exhibit a significant magnetic field tunability across the antiferromagnetic to FM transition in few-layer samples. This behavior is associated to changes in the metal-ligand covalency with magnetic state, as supported by our CTM analysis. Our results clarify the magneto-optical response of CrI$_3$ and identify covalency as a central mechanism for the brightening and field-tunability of spin-forbidden multiplet excitations.

cond-mat.str-el↗