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Kenji Watanabe

Publications and source records attributed to Kenji Watanabe.

At least 1,009 records · Page 56Linked to original sources

Liquid-activated quantum emission from pristine hexagonal boron nitride for nanofluidic sensing

Liquids confined down to the atomic scale can show radically new properties. However, only indirect and ensemble measurements operate in such extreme confinement, calling for novel optical approaches enabling direct imaging at the molecular level. Here, we harness fluorescence originating from single-photon emitters at the surface of hexagonal boron nitride (hBN) for molecular imaging and sensing in nanometrically confined liquids. The emission originates from the chemisorption of organic solvent molecules onto native surface defects, revealing single-molecule dynamics at the interface through spatially correlated activation of neighboring defects. Emitter spectra further offer a direct readout of local dielectric properties, unveiling increasing dielectric order under nanometer-scale confinement. Liquid-activated native hBN defects bridge the gap between solid-state nanophotonics and nanofluidics, opening new avenues for nanoscale sensing and optofluidics.

cond-mat.mes-hall↗

Magnetism-induced band-edge shift as mechanism for magnetoconductance in CrPS$_4$ transistors

Transistors realized on 2D antiferromagnetic semiconductor CrPS$_4$ exhibit large magnetoconductance, due to magnetic-field-induced changes in magnetic state. The microscopic mechanism coupling conductance and magnetic state is not understood. We identify it by analyzing the evolution of the parameters determining the transistor behavior -- carrier mobility and threshold voltage -- with temperature and magnetic field. For temperatures T near the Néel temperature $T_N$, the magnetoconductance originates from a mobility increase due to the applied magnetic field that reduces spin fluctuation induced disorder. For $T << T_N$, instead, what changes is the threshold voltage, so that increasing the field at fixed gate voltage increases the density of accumulated electrons. The phenomenon is explained by a conduction band-edge shift correctly predicted by \emph{ab-initio} calculations. Our results demonstrate that the bandstructure of CrPS$_4$ depends on its magnetic state and reveal a mechanism for magnetoconductance that had not been identified earlier.

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Exciton Superposition across Moiré States in a Semiconducting Moiré Superlattice

Moiré superlattices of semiconducting transition metal dichalcogenides (TMDCs) enable unprecedented spatial control of electron wavefunctions in an artificial lattice with periodicities more than ten times larger than that of atomic crystals, leading to emerging quantum states with fascinating electronic and optical properties. The breaking of translational symmetry further introduces a new degree of freedom inside each moiré unit cell: high symmetry points of energy minima called moiré sites, behaving as spatially separated quantum dots. The superposition of a quasiparticle wavefunction between different moiré sites will enable a new platform for quantum information processing but is hindered by the suppressed electron tunneling between moiré sites. Here we demonstrate the superposition between two moiré sites by constructing an angle-aligned trilayer WSe2/monolayer WS2 moiré heterojunction. The two moiré sites with energy minimum allow the formation of two different interlayer excitons, with the hole residing in either moiré site of the first WSe2 layer interfacing the WS2 layer and the electron in the third WSe2 layer. An external electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe2 layer, realizing the continuous tuning of interlayer exciton hopping between two moiré sites. Therefore, a superposition of the two interlayer excitons localized at different moiré sites can be realized, which can be resolved in the electric-field-dependent optical reflectance spectra, distinctly different from that of the natural trilayer WSe2 in which the moiré modulation is absent. Our study illustrates a strategy of harnessing the new moiré site degree of freedom for quantum information science, a new direction of twistronics.

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Berry Curvature Signatures in Chiroptical Excitonic Transitions

The topology of the electronic band structure of solids can be described by its Berry curvature distribution across the Brillouin zone. We theoretically introduce and experimentally demonstrate a general methodology based on the measurement of energy- and momentum-resolved optical transition rates, allowing to reveal signatures of Berry curvature texture in reciprocal space. By performing time- and angle-resolved photoemission spectroscopy of atomically thin WSe$_2$ using polarization-modulated excitations, we demonstrate that excitons become an asset in extracting the quantum geometrical properties of solids. We also investigate the resilience of our measurement protocol against ultrafast scattering processes following direct chiroptical transitions.

cond-mat.mtrl-sci↗

Measurements of Correlated Insulator Gaps in a Transition Metal Dichalcogenide Moiré Superlattice

Moiré superlattices of transitional metal dichalcogenides exhibit strong electron-electron interaction that has led to experimental observations of Mott insulators and generalized Wigner crystals. In this letter, we report direct measurements of the thermodynamic gaps of these correlated insulating states in a dual-gate WS2/WSe2 moiré bilayer. We employ the microwave impedance microscopy to probe the electronic features in both the graphene top gate and the moiré bilayer, from which we extract the doping dependence of the chemical potential of the moiré bilayer and the energy gaps for various correlated insulating states utilizing the Landau quantization of graphene. These gaps are relatively insensitive to the application of an external electric field to the WS2/WSe2 moiré bilayer.

cond-mat.str-el↗

High mobility transport in isotopically-enriched $^{12}$C and $^{13}$C exfoliated graphene

Graphene quantum dots are promising candidates for qubits due to weak spin-orbit and hyperfine interactions. The hyperfine interaction, controllable via isotopic purification, could be the key to further improving the coherence. Here, we use isotopically enriched graphite crystals of both $^{12}$C and $^{13}$C grown by high-pressure-high-temperature method to exfoliate graphene layers. We fabricated Hall bar devices and performed quantum transport measurements, revealing mobilities exceeding $10^{5}$$\textrm{cm}^{2}/Vs$ and a long mean free path of microns, which are as high as natural graphene. Shubnikov-de Haas oscillations, quantum Hall effect up to the filling factor of one, and Brown-Zak oscillations due to the alignment of hBN and graphene are observed thanks to the high mobility. These results constitute a material platform for physics and engineering of isotopically-enriched graphene qubits.

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Tunable quantum interferometer for correlated moiré electrons

Magic-angle twisted bilayer graphene (MATBG) can host an intriguing variety of gate-tunable correlated states, including superconducting and correlated insulator states. Junction-based superconducting devices, such as Josephson junctions and SQUIDs, have been introduced recently and enable the exploration of the charge, spin, and orbital nature of superconductivity and the coherence of moiré electrons in MATBG. However, complementary fundamental coherence effects - in particular, the Little-Parks effect in a superconducting and the Aharonov-Bohm effect in a normal conducting ring - remained to be observed. Here, we report the observation of both these phenomena in a single gate-defined ring device where we can embed a superconducting or normal conducting ring in a correlated or band insulator. We directly observe the Little-Parks effect in the superconducting phase diagram as a function of density and magnetic field, confirming the effective charge of $2e$. By measuring the Aharonov-Bohm effect, we find that in our device, the coherence length of normal conducting moiré electrons exceeds a few microns at 50 mK. Surprisingly, we also identify a regime characterized by $h/e$-periodic oscillations but with superconductor-like nonlinear transport. Taken together, these experiments establish a novel device platform in MATBG, and more generally in tunable 2D materials, to unravel the nature of superconductivity and other correlated quantum states in these materials.

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Modulating the electrochemical intercalation of graphene interfaces with $α$-RuCl$_3$ as a solid-state electron acceptor

Intercalation reactions modify the charge density in van der Waals (vdW) materials through coupled electronic-ionic charge accumulation, and are susceptible to modulation by interlayer hybridization in vdW heterostructures. Here, we demonstrate that charge transfer between graphene and $α$-RuCl$_3$, which dopes the graphene positively, greatly favors the intercalation of lithium ions into graphene-based vdW heterostructures. We systematically tune this effect on Li$^+$ ion intercalation, modulating the intercalation potential, by using varying thicknesses of hexagonal boron nitride (hBN) as spacer layers between graphene and $α$-RuCl$_3$. Confocal Raman spectroscopy and electronic transport measurements are used to monitor electrochemical intercalation and density functional theory computations help quantify charge transfer to both $α$-RuCl$_3$ and graphene upon Li intercalation. This work demonstrates a versatile approach for systematically modulating the electrochemical intercalation behavior of two-dimensional layers akin to electron donating/withdrawing substituent effects used to tune molecular redox potentials.

cond-mat.mtrl-sci↗

Surface recombination and out of plane diffusivity of free excitons in hexagonal boron nitride

We present a novel experimental protocol using Cathodoluminescence measurements as a function of the electron incident energy to study both exciton diffusion in a directional way and surface exciton recombination. Our approach overcomes the challenges of anisotropic diffusion and the limited applicability of existing methods to the bulk counterparts of 2D materials. The protocol is then applied at room and at cryogenic temperatures to four bulk hexagonal boron nitride crystals grown by different synthesis routes. The exciton diffusivity depends on the sample quality but not on the temperature, indicating it is limited by defect scattering even in the best quality crystals. The lower limit for the diffusivity by phonon scattering is 0.2 cm$^{2}$.s$^{-1}$. Diffusion lengths were as much as 570 nm. Finally, the surface recombination velocity exceeds 10$^{5}$ cm$^{2}$.s$^{-1}$, at a level similar to silicon or diamond. This result reveals that surface recombination could strongly limit light-emitting devices based on 2D materials.

cond-mat.mtrl-sci↗

Quantum control of exciton wavefunctions in 2D semiconductors

Excitons -- bound electron-hole pairs -- play a central role in light-matter interaction phenomena, and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over the quantum mechanical state of excitons in semiconductor heterostructures. Here, we demonstrate a technique for creating tailored and tunable potential landscapes for optically active excitons in 2D semiconductors that enables in-situ wavefunction shaping at the nanoscopic lengthscale. Using nanostructured gate electrodes, we create localized electrostatic traps for excitons in diverse geometries such as quantum dots and rings, and arrays thereof. We show independent spectral tuning of multiple spatially separated quantum dots, which allows us to bring them to degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wavefunctions in optical reflection and photoluminescence measurements. Our work introduces a new approach to engineering exciton dynamics and interactions at the nanometer scale, with implications for novel optoelectronic devices, topological photonics, and many-body quantum nonlinear optics.

cond-mat.mes-hall↗

Long distance electron-electron scattering detected with point contacts

We measure electron transport through point contacts in an electron gas in AlGaAs/GaAs heterostructures and graphene for a range of temperatures, magnetic fields and electron densities. We find a magnetoconductance peak around B = 0. With increasing temperature, the width of the peak increases monotonically, while its amplitude first increases and then decreases. For GaAs point contacts the peak is particularly sharp at relatively low temperatures $T\approx$1.5 K: the curve rounds on a scale of few tens of $μ$T hinting at length scales of several millimeters for the corresponding scattering processes. We propose a model based on the transition between different transport regimes with increasing temperature: from ballistic transport to few electron-electron scatterings to hydrodynamic superballistic flow to hydrodynamic Poiseuille-like flow. The model is in qualitative and, in many cases, quantitative agreement with the experimental observations.

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Valley Isospin Controlled Fractional Quantum Hall States in Bilayer Graphene

A two-dimensional electron system placed in a magnetic field develops Landau levels, where strong Coulomb interactions lead to the appearance of many-body correlated ground states. Quantum numbers similar to the electron spin enable the understanding and control of complex ground state order and collective excitations. Owing to its spin, valley and orbital degrees of freedom, Bernal-stacked bilayer graphene offers a rich platform to pursue correlated phenomena in two dimensions. In this work, we fabricate dual-gated Bernal-stacked bilayer graphene devices and demonstrate unprecedented fine control over its valley isospin degrees of freedom using a perpendicular electric field. Higher sample quality enables us to probe regimes obscured by disorder in previous studies. We present evidence for a new even-denominator fractional quantum Hall state at filling factor ν = 5/2. The 5/2 state is found to be spontaneously valley polarized in the limit of vanishing valley Zeeman splitting, consistent with a theoretical prediction made regarding the spin polarization of the Moore-Read state. In the vicinity of the even-denominator fractional quantum Hall states, we observe the appearance of the predicted Levin-Halperin daughter states of the Moore-Read Pfaffian wave function at ν= 3/2, 7/2, and -1/2 and of the anti-Pfaffian at ν= 5/2. These observations suggest the breaking of particle-hole symmetry in bilayer graphene. We construct a comprehensive valley polarization phase diagram for the Jain sequence fractional states surrounding filling factor 3/2. These results are well explained by a two-component composite fermion model, further demonstrating the SU(2) nature of the valley isospin in bilayer graphene. Our experiment paves the path for future efforts of manipulating the valley isospin in bilayer graphene to engineer exotic topological orders and quantum information processes.

cond-mat.mes-hall↗

Energy gap of the even-denominator fractional quantum Hall state in bilayer graphene

Bernal bilayer graphene hosts even denominator fractional quantum Hall states thought to be described by a Pfaffian wave function with nonabelian quasiparticle excitations. Here we report the quantitative determination of fractional quantum Hall energy gaps in bilayer graphene using both thermally activated transport and by direct measurement of the chemical potential. We find a transport activation gap of 5.1K at B = 12T for a half-filled N=1 Landau level, consistent with density matrix renormalization group calculations for the Pfaffian state. However, the measured thermodynamic gap of 11.6K is smaller than theoretical expectations for the clean limit by approximately a factor of two. We analyze the chemical potential data near fractional filling within a simplified model of a Wigner crystal of fractional quasiparticles with long-wavelength disorder, explaining this discrepancy. Our results quantitatively establish bilayer graphene as a robust platform for probing the non-Abelian anyons expected to arise as the elementary excitations of the even-denominator state.

cond-mat.mes-hall↗

Interplay of valley polarized dark trion and dark exciton-polaron in monolayer WSe2

The interactions between charges and excitons involve complex many-body interactions at high densities. The exciton-polaron model has been adopted to understand the Fermi sea screening of charged excitons in monolayer transition metal dichalcogenides. The results provide good agreement with absorption measurements, which are dominated by dilute bright exciton responses. Here we investigate the Fermi sea dressing of spin-forbidden dark excitons in monolayer WSe2. With a Zeeman field, the valley-polarized dark excitons show distinct p-doping dependence in photoluminescence when the carriers reach a critical density. This density can be interpreted as the onset of strongly modified Fermi sea interactions and shifts with increasing exciton density. Through valley-selective excitation and dynamics measurements, we also infer an intervalley coupling between the dark trions and exciton-polarons mediated by the many-body interactions. Our results reveal the evolution of Fermi sea screening with increasing exciton density and the impacts of polaron-polaron interactions, which lay the foundation for understanding electronic correlations and many-body interactions in 2D systems.

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Quadrupolar Excitons and Hybridized Interlayer Mott Insulator in a Trilayer Moiré Superlattice

Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe2-WS2-WSe2 trilayer moiré superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe2 valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe2 layers share one hole laterally confined in one moiré unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions.

cond-mat.mes-hall↗

Evidence for chiral supercurrent in quantum Hall Josephson junctions

Hybridizing superconductivity with the quantum Hall (QH) effects has major potential for designing novel circuits capable of inducing and manipulating non-Abelian states for topological quantum computation. However, despite recent experimental progress towards this hybridization, concrete evidence for a chiral QH Josephson junction -- the elemental building block for coherent superconducting-QH circuits -- is still lacking. Its expected signature is an unusual chiral supercurrent flowing in QH edge channels, which oscillates with a specific $2ϕ_0$ magnetic flux periodicity ($ϕ_0=h/2e$ is the superconducting flux quantum, $h$ the Planck constant and $e$ the electron charge). Here, we show that ultra-narrow Josephson junctions defined in encapsulated graphene nanoribbons exhibit such a chiral supercurrent, visible up to 8 teslas, and carried by the spin-degenerate edge channel of the QH plateau of resistance $h/2e^2\simeq 12.9$ k$Ω$. We observe reproducible $2ϕ_0$-periodic oscillation of the supercurrent, which emerges at constant filling factor when the area of the loop formed by the QH edge channel is constant, within a magnetic-length correction that we resolve in the data. Furthermore, by varying the junction geometry, we show that reducing the superconductor/normal interface length is pivotal to obtain a measurable supercurrent on QH plateaus, in agreement with theories predicting dephasing along the superconducting interface. Our findings mark a critical milestone along the path to explore correlated and fractional QH-based superconducting devices that should host non-Abelian Majorana and parafermion zero modes.

cond-mat.mes-hall↗

Observation of Fractionally Quantized Anomalous Hall Effect

The integer quantum anomalous Hall (QAH) effect is a lattice analog of the quantum Hall effect at zero magnetic field. This striking transport phenomenon occurs in electronic systems with topologically nontrivial bands and spontaneous time-reversal symmetry breaking. Discovery of its putative fractional counterpart in the presence of strong electron correlations, i.e., the fractional quantum anomalous Hall (FQAH) effect, would open a new chapter in condensed matter physics. Here, we report the direct observation of both integer and fractional QAH effects in electrical measurements on twisted bilayer MoTe$_2$. At zero magnetic field, near filling factor $ν= -1$ (one hole per moiré unit cell) we see an extended integer QAH plateau in the Hall resistance $R_\text{xy}$ that is quantized to $h/e^2 \pm 0.1 \%$ while the longitudinal resistance $R_\text{xx}$ vanishes. Remarkably, at $ν=-2/3$ and $-3/5$ we see plateau features in $R_\text{xy}$ at $3h/2e^2 \pm 1\%$ and $5h/3e^2 \pm 3\%$, respectively, while $R_\text{xx}$ remains small. All these features shift linearly in an applied magnetic field with slopes matching the corresponding Chern numbers $-1$, $-2/3$, and $-3/5$, precisely as expected for integer and fractional QAH states. In addition, at zero magnetic field, $R_\text{xy}$ is approximately $2h/e^2$ near half filling ($ν= -1/2$) and varies linearly as $ν$ is tuned. This behavior resembles that of the composite Fermi liquid in the half-filled lowest Landau level of a two-dimensional electron gas at high magnetic field. Direct observation of the FQAH and associated effects paves the way for researching charge fractionalization and anyonic statistics at zero magnetic field.

cond-mat.mes-hall↗

Non-linear and negative effective diffusivity of optical excitations in moiré-free heterobilayers

Interlayer exciton diffusion is studied in atomically-reconstructed MoSe2/WSe2 heterobilayers with suppressed disorder. Local atomic registry is confirmed by characteristic optical absorption, circularly-polarized photoluminescence, and g-factor measurements. Using transient microscopy we observe propagation properties of interlayer excitons that are independent from trapping at moiré- or disorder-induced local potentials. Confirmed by characteristic temperature dependence for free particles, linear diffusion coefficients of interlayer excitons at liquid helium temperature and low excitation densities are almost 1000 times higher than in previous observations. We further show that exciton-exciton repulsion and annihilation contribute nearly equally to non-linear propagation by disentangling the two processes in the experiment and simulations. Finally, we demonstrate effective shrinking of the light-emission over time across several 100's of picoseconds at the transition from exciton- to the plasma-dominated regimes. Supported by microscopic calculations for bandgap renormalization to identify Mott threshold, this indicates transient crossing between rapidly expanding, short-lived electron-hole plasma and slower, long-lived exciton populations.

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