hBN Layers Research Articles

Scanning probe spectroscopy of sulfur vacancies and MoS2 monolayers in side-contacted van der Waals heterostructures

Abstract We investigate the interplay between vertical tunneling and lateral transport phenomena in electrically contacted van der Waals heterostructures made from monolayer MoS2, hBN, and graphene. We compare data taken by low-temperature scanning tunneling spectroscopy to results from room-temperature conductive atomic force spectroscopy on monolayer MoS2 with sulfur vacancies and with varying hBN layers. We show that for thick hBN barrier layers, where tunneling currents into the conductive substrate are suppressed, a side-contact still enables addressing the defect states in the STM via the lateral current flow. Few-layer hBN realizes an intermediate regime in which the competition between vertical tunneling and lateral transport needs to be considered. The latter is relevant for device structures with both a thin tunneling barrier and a side contact to the semiconducting layers.

Scanning Microwave Impedance Microscopy for Characterization of Graphene Systems Encapsulated by Hexagonal Boron Nitride

Scanning microwave impedance microscopy (sMIM) is a near‐field technique that enables the characterization of conductive materials with a resolution down to 1 nm. In hexagonal boron nitride (hBN)‐encapsulated devices, microwaves emitted from the sMIM tip penetrate and reach with the underlying 2D materials, allowing for the mapping of local conductivity variations. Using twisted bilayer graphene, it is demonstrated that this technique can characterize moiré patterns through hBN flakes up to 2.5 nm thick. Additionally, it is showed that sMIM can distinguish between conductive and insulating materials in samples encapsulated by hBN layers exceeding 15 nm. A key finding is that signal decay due to encapsulation is intrinsically linked to the tip's condition. This work overcomes limitations in the application of twistronics, enabling the verification of the periodicity of moiré patterns in high‐quality encapsulated devices between electrical contacts.

Highly Tunable Moiré Superlattice Potentials in Twisted Hexagonal Boron Nitrides.

Moiré superlattice of twisted hexagonal boron nitride (hBN) has emerged as an advanced atomically thin van der Waals interfacial ferroelectricity platform. Nanoscale periodic ferroelectric moiré potentials in twisted hBN allow the hosting of remote Coulomb superlattice potentials to adjacent 2D materials. Therefore, the new strategies for engineering moiré length, angle, and potential strength are essential for developing programmable quantum materials. Here, it demonstrates the realization of twisted hBN-based moiré superlattice platforms and visualizes the moiré domains and ferroelectric properties using Kelvin probe force microscopy (KPFM). Also, the regular moiré superlattice in the large area is reported. It offers the possibility to reproduce uniform moiré structures with precise control piezo stage stacking and heat annealing. It demonstrates cumulative multi-ferroelectric polarization and multi-level domains with multiple angle mismatched interfaces. Additionally, it observes the quasi-1D anisotropic moiré domains and show the highest resolution analysis of the local built-in strain between adjacent hBN layers compared to the conventional methods. Furthermore, in-situ manipulation of moiré potential is demonstrated using femtosecond pulse laser, which results in the optical phonon-induced atomic displacement at the hBN moiré interfaces. The results pave the way to develop precisely programmable moiré superlattice platforms and investigate strongly correlated physics.

Modulation of hybrid plasmon phonon polaritons mode in circular cylindrical three-layer graphene waveguide

In this present research article, we have investigated analytically the characteristics of the fundamental mode of hybrid surface plasmon phonon polariton (HSPPhPs) mode in a circular cylindrical three-layer graphene (CTLG) waveguide structure. The dispersion equation of HSPPhPs is derived by using Maxwell’s equations and continuity conditions of tangential components of electric and magnetic fields in cylindrical geometry. The dispersion curve has been illustrated and thoroughly examined in relation to the effects of temperature and chemical potential (μc) of graphene, as well as variations in the thickness of silicon dioxide (SiO2) and hexagonal boron nitride (hBN) layers, and found that in the presence of hBN, the effective mode index exhibits hyperbolic behavior with wave number. Up to the first Reststrahlen band (∼830.57 cm⁻¹), it varies slightly with graphene temperature; increasing graphene's (μc) lowers the index, while a thicker hBN layer reduces it, whereas the index increases with SiO₂ layer thickness. Also, we looked at how the CTLG waveguide structure is affected by the electric field distribution, phase speed, and propagation length.

Spatial photoinduced doping of graphene/hBN heterostructures characterized by quantum Hall transport

Abstract Doped semiconductors are a central and crucial component of all integrated circuits. By using a combination of white light and a focused laser beam, and exploiting hexagonal boron nitride (hBN) defect states, heterostructures of hBN/Graphene/hBN are photodoped in-operando, reproducibly and reversibly. We demonstrate device geometries with spatially-defined doping type and magnitude. After each optical doping procedure, magnetotransport measurements including quantum Hall measurements are performed to characterize the device performance. In the unipolar (p+–p–p+ and n–n+–n) configurations, we observe quantization of the longitudinal resistance, proving well-defined doped regions and interfaces that are further analyzed by Landauer–Buttiker modeling. Our unique measurements and modeling of these optically doped devices reveal a complete separation of the p- and n-Landau level edge states. The non-interaction of the edge states results in an observed ‘insulating’ state in devices with a bi-polar p–n–p configuration that is uncommon and has not been measured previously in graphene devices. This insulating state could be utilized in high-performance graphene electrical switches. These quantitative magnetotransport measurements confirm that these doping techniques can be applied to any two-dimensional materials encapsulated within hBN layers, enabling versatile, rewritable circuit elements for future computing and memory applications.

Deterministic fabrication of graphene hexagonal boron nitride moiré superlattices

The electronic properties of moiré heterostructures depend sensitively on the relative orientation between layers of the stack. For example, near-magic-angle twisted bilayer graphene (TBG) commonly shows superconductivity, yet a TBG sample with one of the graphene layers rotationally aligned to a hexagonal Boron Nitride (hBN) cladding layer provided experimental observation of orbital ferromagnetism. To create samples with aligned graphene/hBN, researchers often align edges of exfoliated flakes that appear straight in optical micrographs. However, graphene or hBN can cleave along either zig-zag or armchair lattice directions, introducing a [Formula: see text] ambiguity in the relative orientation of two flakes. By characterizing the crystal lattice orientation of exfoliated flakes prior to stacking using Raman and second-harmonic generation for graphene and hBN, respectively, we unambiguously align monolayer graphene to hBN at a near-[Formula: see text], not [Formula: see text], relative twist angle. We confirm this alignment by torsional force microscopy of the graphene/hBN moiré on an open-face stack, and then by cryogenic transport measurements, after full encapsulation with a second, nonaligned hBN layer. This work demonstrates a key step toward systematically exploring the effects of the relative twist angle between dissimilar materials within moiré heterostructures.

Interfacial negative biexcitons in a monolayer WS2/InGaN quantum dots heterostructure

In this work, we fabricated a Van der Waals heterostructure of monolayer (ML) WS2 and InGaN quantum dots (QDs). This heterostructure is divided into coupled and uncoupled regions based on the thickness of the inserted hBN layer. Upon measuring its PL spectra, we identified an interfacial negative biexciton, which consists of a trion in ML WS2 and an exciton in QDs, in the coupled region. This interfacial negative biexciton features the negative charge of the trion and the quantum confinement of QDs, with its relative intensity showing a strong dependence on the excitation photon energy and featuring a significant threshold. Our work highlights the effective coupling within the mixed-dimensional heterostructure, offering new prospects for the study of many-body physics.

Electrical switching of spin-polarized light-emitting diodes based on a 2D CrI3/hBN/WSe2 heterostructure

Spin-polarized light-emitting diodes (spin-LEDs) convert the electronic spin information to photon circular polarization, offering potential applications including spin amplification, optical communications, and advanced imaging. The conventional control of the emitted light’s circular polarization requires a change in the external magnetic field, limiting the operation conditions of spin-LEDs. Here, we demonstrate an atomically thin spin-LED device based on a heterostructure of a monolayer WSe2 and a few-layer antiferromagnetic CrI3, separated by a thin hBN tunneling barrier. The CrI3 and hBN layers polarize the spin of the injected carriers into the WSe2. With the valley optical selection rule in the monolayer WSe2, the electroluminescence exhibits a high degree of circular polarization that follows the CrI3 magnetic states. Importantly, we show an efficient electrical tuning, including a sign reversal, of the electroluminescent circular polarization by applying an electrostatic field due to the electrical tunability of the few-layer CrI3 magnetization. Our results establish a platform to achieve on-demand operation of nanoscale spin-LED and electrical control of helicity for device applications.

Phonon transport in vacancy induced defective stanene/hBN van der Waals heterostructure

In this study, Non-Equilibrium Molecular Dynamics (NEMD) simulation is employed to investigate the phonon thermal conductivity (PTC) of Sn/hBN van der Waals heterostructures with different vacancy-induced defects. We deliberately introduce three types of vacancies in Sn/hBN bilayer point vacancies, bivacancies, and edge vacancies at various concentrations ranging from 0.25% to 2%, to examine their effects on PTC across temperatures from 100 K to 600 K. The key findings of our work are (i) PTC declines monotonically with increasing vacancy concentration for all types of vacancies, with a maximum reduction of ∼62% observed at room temperature compared to its pristine form. (ii) The position of defects has an impact on PTC, with a larger decrease observed when defects are present in the hBN layer and a smaller decrease when defects are in the Sn layer. (iii) The type of vacancy also influences PTC, with point vacancies causing the most substantial reduction, followed by bivacancies, and edge vacancies having the least effect. A 2% defect concentration results in a ∼62% decrease in PTC for point vacancies, ∼51% for bivacancies, and ∼32% for edge vacancies. (iv) Finally, our results indicate that for a given defect concentration, PTC decreases as temperature increases. The impact of temperature on thermal conductivity is less pronounced compared to the effect of vacancies for the defective Sn/hBN bilayer. The presence of vacancies and elevated temperatures enhance phonon-defect and phonon–phonon scattering, leading to changes in the phonon density of states (PDOS) profile and the distribution of phonons across different frequencies of Sn/hBN bilayer, thus affecting its thermal conductivity. This work offers new insights into the thermal behavior of vacancy-filled Sn/hBN heterostructures, suggesting potential pathways for modulating thermal conductivity in bilayer van der Waals heterostructures for applications in thermoelectric, optoelectronics, and nanoelectronics in future.

Enhanced Long-Term Stability of Crystalline Nickel-Boride (Ni23B6) Electrocatalyst by Encapsulation with Hexagonal Boron Nitride.

Nickel boride catalysts show great potential as low-cost and efficient alternatives to noble-metal catalysts in acidic media; however, synthesizing and isolating a specific phase and composition of nickel boride is nontrivial, and issues persist in their long-term stability as electrocatalysts. Here, a single-crystal nickel boride, Ni23B6, is reported which exhibits high electrocatalytic activity for the hydrogen evolution reaction (HER) in an acidic solution, and that its poor long-term stability can be overcome via encapsulation by single-crystal trilayer hexagonal boron nitride (hBN) film. Interestingly, hBN-covered Ni23B6 on a Ni substrate shows an identical overpotential of 52mV at a current density of 10mA cm-2 to that of bare Ni23B6. This phenomenon indicates that the single-crystalline hBN layer is catalytically transparent and does not obstruct HER activation. The hBN/Ni23B6/Ni has remarkable long-term stability with negligible changes to its polarization curves for 2000 cycles, whereas the Ni23B6/Ni shows significant degradation after 650 cycles. Furthermore, chronoamperometric measurements indicate that stability is preserved for >20h. Long-term stability tests also reveal that the surface morphology and chemical structure of the hBN/Ni23B6/Ni electrode remain preserved. This work provides a model for the practical design of robust and durable electrochemical catalysts through the use of hBN encapsulation.

Full phonon dispersion along the stacking direction in nanoscale van der Waals materials by picosecond acoustics

Phonon dispersion in crystals determines many important material properties, but its measurement usually requires large-scale facilities and is limited to bulk samples. Here, we demonstrate the measurement of full phonon dispersion along the stacking direction in nanoscale systems by using picosecond acoustics. A heterostructure sample was prepared consisting of layers of hexagonal boron nitride (hBN) sandwiching a thin layer of black phosphorus (BP), within which a strain pulse was generated by photoexcitation and observed with an optical probe in the BP layer. The strain pulse traverses to the few nanometer thick hBN layers, where it propagates to the edge and echoes back, like acoustic waves in Newton’s cradle. The echoes returning to the BP layer provide information on the frequency-dependent time-of-flight and group velocity dispersion of the sample system. The microscopic origin of the photoinduced strain pulse generation and its propagation is revealed from first principles. Phonon frequency combs observed in the Fourier transform spectrum confirm the strain wave round trips and demonstrate the feasibility of determining group velocity dispersion through photoacoustics.

Large-Area Synthesis and Fabrication of Few-Layer hBN/Monolayer RGO Heterostructures for Enhanced Contact Surface Potential.

Hexagonal boron nitride (hBN) has a property similar to that of graphene, and it has become one of the most popular materials due to its flexible physical and chemical properties for a variety of applications, especially in nanoelectronics. Enhanced properties of hBN-based heterostructures are crucial for future electronic devices. In this work, a sheet-like hBN crystal was synthesized and transferred onto SiO2/Si substrate and reduced graphene oxide (RGO)/SiO2/Si substrate. Accordingly, the hBN and hBN/RGO films are investigated by optical microscopy, X-ray diffraction, high-resolution transmission electron microscopy, Raman spectroscopy, and atomic force microscopy. The thickness of a single hBN layer is approximately 0.4 nm. A few layers of hBN stacked in large areas are mostly observed in both hBN and the hBN/RGO films. By using Kelvin probe force microscopy, it was found that the hBN/RGO heterostructure has a contact surface potential higher than that of the hBN layer. The large-scale synthesis and fabrication of hBN/RGO films could be extended to fabricate other van der Waals heterostructures.

Highly efficient spin field-effect transistor based on nanographene and hBN heterostructures: spintronic and quantum transport properties

Intense efforts are being undertaken to design atomic-scale nanodevices in response to the demand for novel electronic/spintronic devices to address the problems facing the current devices. In this work, we construct new spintronic nanodevices based on 2D heterostructures from graphene and hBN quantum dots. The heterostructures are ferromagnetic spin-ordered semiconductors with nonzero spin originating from the unpaired edge electrons of the graphene quantum dots. The net spin and its distribution on different layers of the heterostructures are controllable. For instance, doping the hBN layer in the lateral graphene-hBN-graphene structure with C-atoms can boost the net spin and facilitate its distribution on the three layers. The electronic properties are also affected where half metallicity has been achieved in this system. The I-V characteristics of the lateral G-hBN heterostructure show an oscillating spin-up current that is significantly higher than the regular spin-down current. Doping G-hBN with C-atoms significantly enhances the current magnitude and removes the oscillation due to the decreased net spin by the dopants. We demonstrate a field effect transistor from the lateral G-hBN-G heterostructure that operates based on quantum tunneling from the G-layer through the hBN-layer. The device works as a spin filter at zero gate voltage. A significant enhancement of the drain current is achieved by applying a positive gate voltage. This device shows an ON/OFF ratio of up to 1010 making it an ideal applicant for future spintronic nanodevices.

Reduced interface effect of proton beam irradiation on the electrical properties of WSe2/hBN field effect transistors

Two-dimensional transition metal dichalcogenide (TMDC) semiconductors are emerging as strong contenders for electronic devices that can be used in highly radioactive environments such as outer space where conventional silicon-based devices exhibit nonideal characteristics for such applications. To address the radiation-induced interface effects of TMDC-based electronic devices, we studied high-energy proton beam irradiation effects on the electrical properties of field-effect transistors (FETs) made with tungsten diselenide (WSe2) channels and hexagonal boron-nitride (hBN)/SiO2 gate dielectrics. The electrical characteristics of WSe2 FETs were measured before and after the irradiation at various proton beam doses of 1013, 1014, and 1015 cm−2. In particular, we demonstrated the dependence of proton irradiation-induced effects on hBN layer thickness in WSe2 FETs. We observed that the hBN layer reduces the WSe2/dielectric interface effect which would shift the transfer curve of the FET toward the positive direction of the gate voltage. Also, this interface effect was significantly suppressed when a thicker hBN layer was used. This phenomenon can be explained by the fact that the physical separation of the WSe2 channel and SiO2 dielectric by the hBN interlayer prevents the interface effects originating from the irradiation-induced positive trapped charges in SiO2 reaching the interface. This work will help improve our understanding of the interface effect of high-energy irradiation on TMDC-based nanoelectronic devices.

Polarization-insensitive perfect absorption in van der waals hyper-structure

Infrared perfect absorption has been widely investigated due to its potential applications in photodetectors, photovoltaics and medical diagnostics. In this report, we demonstrate that at particular infrared frequencies, a simple planar structure made up of graphene-hexagonal Boron Nitride (hBN) hyper-structure is able to nearly perfectly absorb incident light irrespective of its polarization (Transverse-Magnetic TM, or Transverse-Electric TE). By using this interferenceless technique, the hyper-structure achieves nearly zero reflectance at a wide range of angles in a narrow frequency band. We analytically predict the condition of achieving such an important feature of perfect absorption for both TM and TE polarizations. Interestingly, the infrared perfect absorption can be redshifted by increasing the thickness of the hBN layers and blueshifted by increasing the graphene’s chemical potential. Such flexible control of infrared perfect absorption offers a new tool for controlling electromagnetic waves and has potential applications in photodetection and other light control applications.

Highly Thermally Conductive Flexible Biomimetic APTES-BNNS/BC Nanocomposite Paper by Sol-Gel-Film Technology.

Owing to the evolution of 5G technology, new energy vehicles, flexible electronics, miniaturization and integration of microelectronic devices, high-frequency and high-power devices, and thermal management of materials must consider additional limitations such as electrical insulation, excellent transverse heat transfer, flexibility, and weight. Boron nitride nanosheets (BNNSs) are ideal insulating materials with high thermal conductivity. However, the problem of the 3D thermal conductivity pathway and toughness strength of nanocomposite paper loaded with inorganic thermal conductivity fillers remains a huge challenge. In this study, we propose a new method for preparing ultrathin, large, and uniformly thick BNNS for quantitative production. Bulk hexagonal boron nitride (hBN) layers were exfoliated using a simple and low-cost hydrothermal reaction, and large-scale fewer-layered BNNSs were efficiently prepared by ball milling with a high yield (up to 80%). Based on the aforementioned step, a flexible insulating composite film with high thermal conductivity and a natural "brick-mud" shell structure was constructed via the sol-gel-film conversion method. After prestretching and hot-pressing treatment, the hydrogels became denser, and the modified BNNS formed a three-dimensional (3D) network structure with an ordered orientation and interconnections in the bacterial cellulose (BC) matrix. After 100 folding cycles, the tensile strength of the nanofiber composite film reached 53 MPa, and the strength retention rate exceeded 42%. By optimizing the modified BNNS content, the thermal conductivity reached 24 W/(m·K). This simple approach has wide application potential in the next-generation electronic devices, providing options for designing thermal interface materials with excellent electrical insulation, high thermal stability, and flexibility.

Hybrid graphene anti-resonant fiber with tunable light absorption.

Controlling the output light-intensity and realizing the light-switch function in hollow-core anti-resonant fibers (HC-ARFs) is crucial for their applications in polarizers, lasers, and sensor systems. Here, we theoretically propose a hybrid light-intensity-tunable HC-ARF deposited with the sandwiched graphene/hexagonal boron nitride/graphene based on the typical six-circular-tube and the nested structures. Changing the external drive voltage from 12.3 to 31.8 V, the hybrid HC-ARF experiences a high-low alterative attenuation coefficient with a modulation depth 3.87 and 1.91 dB/cm for the six-circular-tube and nested structures respectively, serving as a well-performance light-switch at the optical communication wavelength of 1.55 µm. This response is attributed to the variation of the Fermi level of graphene and is obviously influenced by the core size, fiber length, and the number of graphene and hBN layers. Moreover, one attenuation dip of the modulation depth was found because of the epsilon-near-zero effect in graphene. Our design provides a feasible paradigm for integrating graphene with anti-resonant fibers and high-performance electro-optic modulators.

Graphene nanoribbons grown in hBN stacks for high-performance electronics.

Van der Waals encapsulation of two-dimensional materials in hexagonal boron nitride (hBN) stacks is a promising way to create ultrahigh-performance electronic devices1-4. However, contemporary approaches for achieving van der Waals encapsulation, which involve artificial layer stacking using mechanical transfer techniques, are difficult to control, prone to contamination and unscalable. Here we report the transfer-free direct growth of high-quality graphene nanoribbons (GNRs) in hBN stacks. The as-grown embedded GNRs exhibit highly desirable features being ultralong (up to 0.25 mm), ultranarrow (<5 nm) and homochiral with zigzag edges. Our atomistic simulations show that the mechanism underlying the embedded growth involves ultralow GNR friction when sliding between AA'-stacked hBN layers. Using the grown structures, we demonstrate the transfer-free fabrication of embedded GNR field-effect devices that exhibit excellent performance at room temperature with mobilities of up to 4,600 cm2 V-1 s-1 and on-off ratios of up to 106. This paves the way for the bottom-up fabrication of high-performance electronic devices based on embedded layered materials.

Spatiotemporal beating and vortices of van der Waals hyperbolic polaritons

In conventional thin materials, the diffraction limit of light constrains the number of waveguide modes that can exist at a given frequency. However, layered van der Waals (vdW) materials, such as hexagonal boron nitride (hBN), can surpass this limitation due to their dielectric anisotropy, exhibiting positive permittivity along one optic axis and negativity along the other. This enables the propagation of hyperbolic rays within the material bulk and an unlimited number of subdiffractional modes characterized by hyperbolic dispersion. By employing time-domain near-field interferometry to analyze ultrafast hyperbolic ray pulses in thin hBN, we showed that their zigzag reflection trajectories bound within the hBN layer create an illusion of backward-moving and leaping behavior of pulse fringes. These rays result from the coherent beating of hyperbolic waveguide modes but could be mistakenly interpreted as negative group velocities and backward energy flow. Moreover, the zigzag reflections produce nanoscale (60 nm) and ultrafast (40 fs) spatiotemporal optical vortices along the trajectory, presenting opportunities to chiral spatiotemporal control of light-matter interactions. Supported by experimental evidence, our simulations highlight the potential of hyperbolic ray reflections for molecular vibrational absorption nanospectroscopy. The results pave the way for miniaturized, on-chip optical spectrometers, and ultrafast optical manipulation.

HBN‐Encapsulated Graphene Coupled to a Plasmonic Metasurface via 1D Electrodes for Photodetection Applications

It is shown here how encapsulated graphene devices can be laterally coupled to plasmonic metasurfaces via 1D edge contacts, preserving the high mobility of encapsulated graphene while enhancing optical coupling. The device is used for photodetection applications where high responsivities in the range of 100 A W−1 for most of the visible spectrum are reported. The device exhibits a photogating effect which is attributed to defect states in the encapsulating hBN layers. The results highlight a new configuration to couple graphene with plasmonic structures and points to a new type of device based on defect states and graphene's excellent transport properties to achieve photodetectors with ultrahigh responsivities.