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1.
Nat Commun ; 15(1): 4905, 2024 Jun 08.
Article in English | MEDLINE | ID: mdl-38851776

ABSTRACT

The moiré potential serves as a periodic quantum confinement for optically generated excitons, creating spatially ordered zero-dimensional quantum systems. However, a broad emission spectrum resulting from inhomogeneity among moiré potentials hinders the investigation of their intrinsic properties. In this study, we demonstrated a method for the optical observation of quantum coherence and interference of a single moiré exciton in a twisted semiconducting heterobilayer beyond the diffraction limit of light. We observed a single and sharp photoluminescence peak from a single moiré exciton following nanofabrication. Our findings revealed the extended duration of quantum coherence in a single moiré exciton, persisting beyond 10 ps, and an accelerated decoherence process with increasing temperature and excitation power density. Moreover, quantum interference experiments revealed the coupling between moiré excitons in different moiré potential minima. The observed quantum coherence and interference of moiré exciton will facilitate potential applications of moiré quantum systems in quantum technologies.

2.
Nat Commun ; 15(1): 5065, 2024 Jun 13.
Article in English | MEDLINE | ID: mdl-38871728

ABSTRACT

Excitons, pairs of electrons and holes, undergo a Bose-Einstein condensation at low temperatures. An important platform to study excitons is double-layer two-dimensional electron gases, with two parallel planes of electrons and holes separated by a thin insulating layer. Lowering this separation (d) strengthens the exciton binding energy, however, leads to the undesired interlayer tunneling, resulting in annihilation of excitons. Here, we report the observation of a sequences of robust exciton condensates (ECs) in double bilayer graphene twisted to ~ 10° with no insulating mid-layer. The large momentum mismatch between two graphene layers suppresses interlayer tunneling, reaching a d ~ 0.334 nm. Measuring the bulk and edge transport, we find incompressible states corresponding to ECs when both layers are in half-filled N = 0, 1 Landau levels (LLs). Theoretical calculations suggest that the low-energy charged excitation of ECs can be meron-antimeron or particle-hole pair, which relies on both LL index and carrier type. Our results establish a novel platform with extreme coupling strength for studying quantum bosonic phase.

3.
Nanotechnology ; 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38885618

ABSTRACT

Optical microscopy with white light illumination has been employed when obtaining exfoliated monolayer hexagonal boron nitride (1L hBN) films from a large number of randomly placed films on a substrate. However, real-time observation of 1L hBN using a color camera under white light illumination remains challenging since hBN is transparent in the visible wavelength range. The poor optical constant of 1L hBN films in microphotographs is significantly improved using a Si substrate coated with a SiNx thin-film (SiNx/Si). When observing hBN thin films on SiNx/Si using a color digital camera in an optical microscope under white light illumination, the clarity of the captured images depends on the thickness of the SiNx film (d). For direct real-time observation, the d was optimized based on quantitative chromatic studies tailored to Bayer filters of a color image sensor. Through image simulation, it was determined that the color difference between 1L hBN and the bare substrate is maximized at d = 59 or 70 nm, which was experimentally verified. The SiNx/Si with optimized d values visualized 1L hBN films without requiring significant contrast enhancement via image processing under white light illumination in real-time. Furthermore, the captured color photographs facilitate the reliable determination of the number of layers in few-layer hBN films using the contrast of the green channel of the images.

4.
Adv Sci (Weinh) ; : e2401840, 2024 Jun 18.
Article in English | MEDLINE | ID: mdl-38889272

ABSTRACT

Graphene is a unique platform for tunable opto-electronic applications thanks to its linear band dispersion, which allows electrical control of resonant light-matter interactions. Tuning the nonlinear optical response of graphene is possible both electrically and in an all-optical fashion, but each approach involves a trade-off between speed and modulation depth. Here, lattice temperature, electron doping, and all-optical tuning of third-harmonic generation are combined in a hexagonal boron nitride-encapsulated graphene opto-electronic device and demonstrate up to 85% modulation depth along with gate-tunable ultrafast dynamics. These results arise from the dynamic changes in the transient electronic temperature combined with Pauli blocking induced by the out-of-equilibrium chemical potential. The work provides a detailed description of the transient nonlinear optical and electronic response of graphene, which is crucial for the design of nanoscale and ultrafast optical modulators, detectors, and frequency converters.

5.
Nature ; 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38898282

ABSTRACT

Graphene-based, high-quality, two-dimensional electronic systems have emerged as a highly tunable platform for studying superconductivity1-21. Specifically, superconductivity has been observed in both electron- and hole-doped twisted graphene moiré systems1-17, whereas in crystalline graphene systems, superconductivity has so far been observed only in hole-doped rhombohedral trilayer graphene (RTG)18 and hole-doped Bernal bilayer graphene (BBG)19-21. Recently, enhanced superconductivity has been demonstrated20,21 in BBG because of the proximity to a monolayer WSe2. Here we report the observation of superconductivity and a series of flavour-symmetry-breaking phases in electron- and hole-doped BBG/WSe2 devices by electrostatic doping. The strength of the observed superconductivity is tunable by applied vertical electric fields. The maximum Berezinskii-Kosterlitz-Thouless transition temperature for the electron- and hole-doped superconductivity is about 210 mK and 400 mK, respectively. Superconductivities emerge only when the applied electric fields drive the BBG electron or hole wavefunctions towards the WSe2 layer, underscoring the importance of the WSe2 layer in the observed superconductivity. The hole-doped superconductivity violates the Pauli paramagnetic limit, consistent with an Ising-like superconductor. By contrast, the electron-doped superconductivity obeys the Pauli limit, although the proximity-induced Ising spin-orbit coupling is also notable in the conduction band. Our findings highlight the rich physics associated with the conduction band in BBG, paving the way for further studies into the superconducting mechanisms of crystalline graphene and the development of superconductor devices based on BBG.

6.
Article in English | MEDLINE | ID: mdl-38910437

ABSTRACT

In-memory computing may make it possible to realize non-von Neumann computing because the logic circuits are unified in the memory units. We investigated two types of in-memory logic operations, namely, two-input logic circuits and multifunctional artificial synapses. These were realized in a dual-gate antiambipolar transistor (AAT) with a ReS2/WSe2 heterojunction, in which polystyrene with a zinc phthalocyanine core (ZnPc-PS4) was incorporated as a memory layer. Here, reconfigurability is a key concept for both types of device operations and was achieved by merging the Λ-shaped transfer curve of the AAT and the nonvolatile memory effect of ZnPc-PS4. First, we achieved electrically reconfigurable two-input logic circuits. Versatile logic circuits such as AND, OR, NAND, NOR, and XOR circuits were demonstrated by taking advantage of the Λ-shaped transfer curve of the dual-gate AAT. Importantly, the nonvolatile memory function provided the electrical switching of the individual circuits between AND/OR, NAND/NOR, and XOR/NAND circuits with constant input signals. Second, the memory effect was applied to multifunctional artificial synapses. The inhibitory/excitatory and long-term potentiation/depression synaptic operations were electrically reconfigured simply by controlling one parameter (readout voltage), making three distinct responses possible even with the same presynaptic signals. These findings provide hints that may lead to the realization of new in-memory computing architectures beyond the current von Neumann computers.

7.
Nat Commun ; 15(1): 4735, 2024 Jun 03.
Article in English | MEDLINE | ID: mdl-38830857

ABSTRACT

Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton coupling, and exhibiting peculiar magneto-optics of exciton-polaritons. Here, we demonstrate that both exciton and magnetic transitions in bilayer and trilayer CrSBr are sensitive to voltage-controlled field-effect charging, exhibiting bound exciton-charge complexes and doping-induced metamagnetic transitions. Moreover, we demonstrate how these unique properties enable optical probes of local magnetic order, visualizing magnetic domains of competing phases across metamagnetic transitions induced by magnetic field or electrostatic doping. Our work identifies few-layer CrSBr as a rich platform for exploring collaborative effects of charge, optical excitations, and magnetism.

8.
Phys Rev Lett ; 132(20): 206903, 2024 May 17.
Article in English | MEDLINE | ID: mdl-38829069

ABSTRACT

Emitter dephasing is one of the key issues in the performance of solid-state single-photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single-photon emission. Here, we demonstrate that it is possible to tune and engineer the coherence of photons emitted from a single WSe_{2} monolayer quantum dot via selectively coupling it to a spectral cavity resonance. We utilize an open cavity to demonstrate spectral enhancement, leveling, and suppression of the highly asymmetric phonon sideband, finding excellent agreement with a microscopic description of the exciton-phonon dephasing in a truly two-dimensional system. Moreover, the impact of cavity tuning on the dephasing is directly assessed via optical interferometry, which points out the capability to utilize light-matter coupling to steer and design dephasing and coherence of quantum emitters in atomically thin crystals.

9.
Nano Lett ; 2024 Jun 04.
Article in English | MEDLINE | ID: mdl-38833415

ABSTRACT

We implement circuit quantum electrodynamics (cQED) with quantum dots in bilayer graphene, a maturing material platform that can host long-lived spin and valley states. Our device combines a high-impedance (Zr ≈ 1 kΩ) superconducting microwave resonator with a double quantum dot electrostatically defined in a graphene-based van der Waals heterostructure. Electric dipole coupling between the subsystems allows the resonator to sense the electric susceptibility of the double quantum dot from which we reconstruct its charge stability diagram. We achieve sensitive and fast detection of the interdot transition with a signal-to-noise ratio of 3.5 within 1 µs integration time. The charge-photon interaction is quantified in the dispersive and resonant regimes by comparing the resonator response to input-output theory, yielding a coupling strength of g/2π = 49.7 MHz. Our results introduce cQED as a probe for quantum dots in van der Waals materials and indicate a path toward coherent charge-photon coupling with bilayer graphene quantum dots.

10.
Science ; : eadp3575, 2024 Jun 06.
Article in English | MEDLINE | ID: mdl-38843354

ABSTRACT

The persistence of voltage-switchable collective electronic phenomena down to the atomic scale has extensive implications for area-efficient and energy-efficient electronics, especially in emerging nonvolatile memory technology. We investigate the performance of a ferroelectric field-effect transistor (FeFET) based on sliding ferroelectricity in bilayer boron nitride at room temperature. Sliding ferroelectricity represents a different form of atomically thin two-dimensional ferroelectrics, characterized by the switching of out-of-plane polarization through interlayer sliding motion. We examined the FeFET device employing monolayer graphene as the channel layer, which demonstrated ultrafast switching speeds on the nanosecond scale and high endurance exceeding 1011 switching cycles, comparable to state-of-the-art FeFET devices. These characteristics highlight the potential of two-dimensional sliding ferroelectrics for inspiring next-generation nonvolatile memory technology.

11.
Phys Rev Lett ; 132(21): 216903, 2024 May 24.
Article in English | MEDLINE | ID: mdl-38856288

ABSTRACT

Controlling interlayer excitons in Van der Waals heterostructures holds promise for exploring Bose-Einstein condensates and developing novel optoelectronic applications, such as excitonic integrated circuits. Despite intensive studies, several key fundamental properties of interlayer excitons, such as their binding energies and interactions with charges, remain not well understood. Here we report the formation of momentum-direct interlayer excitons in a high-quality MoSe_{2}/hBN/MoSe_{2} heterostructure under an electric field, characterized by bright photoluminescence (PL) emission with high quantum yield and a narrow linewidth of less than 4 meV. These interlayer excitons show electrically tunable emission energy spanning ∼180 meV through the Stark effect, and exhibit a sizable binding energy of ∼81 meV in the intrinsic regime, along with trion binding energies of a few millielectronvolts. Remarkably, we demonstrate the long-range transport of interlayer excitons with a characteristic diffusion length exceeding 10 µm, which can be attributed, in part, to their dipolar repulsive interactions. Spatially and polarization-resolved spectroscopic studies reveal rich exciton physics in the system, such as valley polarization, local trapping, and the possible existence of dark interlayer excitons. The formation and transport of tightly bound interlayer excitons with narrow linewidth, coupled with the ability to electrically manipulate their properties, open exciting new avenues for exploring quantum many-body physics, including excitonic condensate and superfluidity, and for developing novel optoelectronic devices, such as exciton and photon routers.

12.
Nano Lett ; 24(23): 6838-6843, 2024 Jun 12.
Article in English | MEDLINE | ID: mdl-38825784

ABSTRACT

Moiré superlattices, constituted by two-dimensional materials, demonstrate a variety of strongly correlated and topological phenomena including correlated insulators, superconductivity, and integer/fractional Chern insulators. In the realm of topological nontrivial Chern insulators within specific moiré superlattices, previous studies usually observe a single Chern number at a given filling factor in a device. Here we present the observation of gate-tunable Chern numbers within the Chern insulator state of an ABC-stacked trilayer graphene/hexagonal boron nitride moiré superlattice device. Near quarter filling, the moiré superlattice exhibits spontaneous valley polarization and distinct ferromagnetism associated with the Chern insulator states over a range of the displacement field. Surprisingly we find a transition of the Chern number from C = 3 to 4 as the displacement field is increased. Our observation of gate-tunable correlated Chern insulators suggests new ways to control and manipulate topological states in a moiré superlattice device.

13.
Nano Lett ; 24(23): 7077-7083, 2024 Jun 12.
Article in English | MEDLINE | ID: mdl-38828922

ABSTRACT

The study of exciton polarons has offered profound insights into the many-body interactions between bosonic excitations and their immersed Fermi sea within layered heterostructures. However, little is known about the properties of exciton polarons with interlayer interactions. Here, through magneto-optical reflectance contrast measurements, we experimentally investigate interlayer Fermi polarons for 2s excitons in WSe2/graphene heterostructures, where the excited exciton states (2s) in the WSe2 layer are dressed by free charge carriers of the adjacent graphene layer in the Landau quantization regime. First, such a system enables an optical detection of integer and fractional quantum Hall states (e.g., ν = ±1/3, ±2/3) of monolayer graphene. Furthermore, we observe that the 2s state evolves into two distinct branches, denoted as attractive and repulsive polarons, when graphene is doped out of the incompressible quantum Hall gaps. Our work paves the way for the understanding of the excited composite quasiparticles and Bose-Fermi mixtures.

14.
Phys Rev Lett ; 132(22): 226301, 2024 May 31.
Article in English | MEDLINE | ID: mdl-38877917

ABSTRACT

We demonstrate that the mode number of Andreev bound states in bilayer graphene Josephson junctions can be modulated by controlling the superconducting coherence length in situ. By exploiting the quadratic band dispersion of bilayer graphene, we control the Fermi velocity and thus the coherence length via the application of electrostatic gating. Tunneling spectroscopy of the Andreev bound states reveals a crossover from short to long Josephson junction regimes as we approach the charge neutral point of the bilayer graphene. Furthermore, analysis of different mode numbers of the Andreev energy spectrum allows us to estimate the phase-dependent Josephson current quantitatively. Our Letter provides a new way for studying multimode Andreev levels by tuning the Fermi velocity.

15.
ACS Appl Mater Interfaces ; 16(24): 31247-31253, 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38844450

ABSTRACT

As Coulomb drag near charge neutrality (CN) is driven by fluctuations or inhomogeneity in charge density, the topology should play an extremely important role. Interlinking Coulomb drag and topology could reveal how the system's nontrivial topology influences the electron-electron interactions at the quantum level. However, such an aspect is overlooked as most studies focus on symmetric drag systems without topology. To understand this topological aspect, we need to study Coulomb drag in an asymmetric system with a broken inversion symmetry and strong spin-orbit coupling (SOC). Here we experimentally demonstrate the energy-driven Coulomb drag in an asymmetric van der Waals heterostructure composed of black phosphorus and rhenium disulfide characterized by broken inversion symmetry. Temperature-dependent transport measurements near CN provide compelling evidence for the energy-driven Coulomb drag due to electron-hole coupling that is energetically favored in a broken-gap heterojunction, as confirmed by Hall coefficient sign reversal with temperature. Moreover, contrary to the symmetric devices, our results exhibit magnetic-field-free, i.e., topology-driven, Hall drag, revealing an intrinsic coupling between energy and charge modes. This is the manifestation of nonzero Berry curvature, akin to a magnetic field in momentum space, in a Rashba system, which arises from the SOC and broken inversion symmetry of the heterostructure.

16.
Nano Lett ; 24(22): 6722-6729, 2024 Jun 05.
Article in English | MEDLINE | ID: mdl-38717299

ABSTRACT

Double-layer quantum systems are promising platforms for realizing novel quantum phases. Here, we report a study of quantum oscillations (QOs) in a weakly coupled double-layer system composed of a large-angle twisted-double-bilayer graphene (TDBG). We quantify the interlayer coupling strength by measuring the interlayer capacitance from the QOs pattern at low temperatures, revealing electron-hole asymmetry. At high temperatures when SdHOs are thermally smeared, we observe resistance peaks when Landau levels (LLs) from two moiré minivalleys are aligned, regardless of carrier density; eventually, it results in a 2-fold increase of oscillating frequency in D, serving as compelling evidence of the magneto-intersub-band oscillations (MISOs) in double-layer systems. The temperature dependence of MISOs suggests that electron-electron interactions play a crucial role and the scattering times obtained from MISO thermal damping are correlated with the interlayer coupling strength. Our study reveals intriguing interplays among Landau quantization, moiré band structure, and scatterings.

17.
Nano Lett ; 24(22): 6529-6537, 2024 Jun 05.
Article in English | MEDLINE | ID: mdl-38789104

ABSTRACT

Contact resistance is a multifaceted challenge faced by the 2D materials community. Large Schottky barrier heights and gap-state pinning are active obstacles that require an integrated approach to achieve the development of high-performance electronic devices based on 2D materials. In this work, we present semiconducting PtSe2 field effect transistors with all-van-der-Waals electrode and dielectric interfaces. We use graphite contacts, which enable high ION/IOFF ratios up to 109 with currents above 100 µA µm-1 and mobilities of 50 cm2 V-1 s-1 at room temperature and over 400 cm2 V-1 s-1 at 10 K. The devices exhibit high stability with a maximum hysteresis width below 36 mV nm-1. The contact resistance at the graphite-PtSe2 interface is found to be below 700 Ω µm. Our results present PtSe2 as a promising candidate for the realization of high-performance 2D circuits built solely with 2D materials.

18.
Nat Commun ; 15(1): 4321, 2024 May 21.
Article in English | MEDLINE | ID: mdl-38773076

ABSTRACT

The flat bands in magic-angle twisted bilayer graphene (MATBG) provide an especially rich arena to investigate interaction-driven ground states. While progress has been made in identifying the correlated insulators and their excitations at commensurate moiré filling factors, the spin-valley polarizations of the topological states that emerge at high magnetic field remain unknown. Here we introduce a technique based on twist-decoupled van der Waals layers that enables measurement of their electronic band structure and-by studying the backscattering between counter-propagating edge states-the determination of the relative spin polarization of their edge modes. We find that the symmetry-broken quantum Hall states that extend from the charge neutrality point in MATBG are spin unpolarized at even integer filling factors. The measurements also indicate that the correlated Chern insulator emerging from half filling of the flat valence band is spin unpolarized and suggest that its conduction band counterpart may be spin polarized.

19.
Sci Adv ; 10(18): eadi3653, 2024 May 03.
Article in English | MEDLINE | ID: mdl-38691599

ABSTRACT

Manipulating the nanostructure of materials is critical for numerous applications in electronics, magnetics, and photonics. However, conventional methods such as lithography and laser writing require cleanroom facilities or leave residue. We describe an approach to creating atomically sharp line defects in hexagonal boron nitride (hBN) at room temperature by direct optical phonon excitation with a mid-infrared pulsed laser from free space. We term this phenomenon "unzipping" to describe the rapid formation and growth of a crack tens of nanometers wide from a point within the laser-driven region. Formation of these features is attributed to the large atomic displacement and high local bond strain produced by strongly driving the crystal at a natural resonance. This process occurs only via coherent phonon excitation and is highly sensitive to the relative orientation of the crystal axes and the laser polarization. Its cleanliness, directionality, and sharpness enable applications such as polariton cavities, phonon-wave coupling, and in situ flake cleaving.

20.
Nat Commun ; 15(1): 4254, 2024 May 18.
Article in English | MEDLINE | ID: mdl-38762501

ABSTRACT

Excitons in two-dimensional (2D) semiconductors have offered an attractive platform for optoelectronic and valleytronic devices. Further realizations of correlated phases of excitons promise device concepts not possible in the single particle picture. Here we report tunable exciton "spin" orders in WSe2/WS2 moiré superlattices. We find evidence of an in-plane (xy) order of exciton "spin"-here, valley pseudospin-around exciton filling vex = 1, which strongly suppresses the out-of-plane "spin" polarization. Upon increasing vex or applying a small magnetic field of ~10 mT, it transitions into an out-of-plane ferromagnetic (FM-z) spin order that spontaneously enhances the "spin" polarization, i.e., the circular helicity of emission light is higher than the excitation. The phase diagram is qualitatively captured by a spin-1/2 Bose-Hubbard model and is distinct from the fermion case. Our study paves the way for engineering exotic phases of matter from correlated spinor bosons, opening the door to a host of unconventional quantum devices.

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