Bilayer Hexagonal Boron Nitride Research Articles

Moiré flat bands and antiferroelectric domains in lattice relaxed twisted bilayer hexagonal boron nitride under perpendicular electric fields

Moiré flat bands and antiferroelectric domains in lattice relaxed twisted bilayer hexagonal boron nitride under perpendicular electric fields

Ultrafast Switching of Sliding Polarization and Dynamical Magnetic Field in van der Waals Bilayers Induced by Light.

Sliding ferroelectricity is a unique type of polarity recently observed in van der Waals bilayers with a suitable stacking. However, electric-field control of sliding ferroelectricity is hard and could induce large coercive electric fields and serious leakage currents that corrode the ferroelectricity and electronic properties, which are essential for modern two-dimensional electronics and optoelectronics. Here, we proposed laser-pulse deterministic control of sliding polarization in bilayer hexagonal boron nitride by first principles and molecular dynamics simulation with machine-learned force fields. The laser pulses excite shear modes that exhibit certain directional movements of lateral sliding between bilayers. The vibration of excited modes under laser pulses is predicted to overcome the energy barrier and achieve the switching of sliding polarization. Furthermore, it is found that three possible sliding transitions-between AB (BA) and BA (AB) stacking-can lead to the occurrence of dynamical magnetic fields along three different directions. Remarkably, the magnetic fields are generated by the simple linear motion of nonmagnetic species, without any need for more exotic (circular, spiral) pathways. Such predictions of deterministic control of sliding polarization and multistates of dynamical magnetic field thus expand the potential applications of sliding ferroelectricity in memory and electronic devices.

Flatbands in a bilayer surface plasmon crystal at a large twist angle due to interlayer strong coupling.

The twisted bilayer system provides an excellent platform for the study of flatbands. In this work, we propose a bilayer hexagonal boron nitride (h-BN)-like surface plasmon crystal at a large twist angle of 38.213° due to the interlayer strong coupling, in which the adjacent pillars are in different radii. We numerically and theoretically calculate the band structure while tuning the pillar radius ratio (PRR) and the interlayer separation distance. As a result, both increasing the PRR and decreasing the separation distance contribute to the transition from weak coupling to strong coupling, leading to the flatbands with slow velocity and large density of state. Consequently, the in-layer geometry as well as the separation distance offers the degree of freedom to achieve flatbands in the bilayer surface plasmon crystal. Our work provides a fundamental understanding of the band structure of the twisted bilayer photonic system, which enriches the methods to obtain flatbands at a large twist angle.

Mechanical and vibrational behaviors of bilayer hexagonal boron nitride in different stacking modes

Hexagonal boron nitride (h-BN) is a semiconductor material with a wide band gap, which has great potential to serve as a nanoresonators in microelectronics and mass and force sensing fields. This paper investigates the mechanical properties and natural frequencies of bilayer h-BN nanosheets under five different stacking modes, which have been rarely studied, using molecular dynamics simulations. The mechanical properties, including Young’s modulus, the ultimate stress, ultimate strain, Poisson’s ratio and shear modulus, are studied for all five stacking modes. And the effects of strain rate, crystal orientation and temperature to bilayer h-BN nanosheets’ tensile properties have also been studied. Our findings suggest that bilayer h-BN nanosheets are basically an anisotropic material whose tensile properties vary substantially with stacking modes and temperature. Moreover, the natural frequencies are proposed in an explicit form based on the nonlocal theory. The differences of the fundamental natural frequencies among different stacking modes are affected by the constraint condition of bilayer h-BN sheet. The theory results match well with the simulation results. These findings establish elementary understandings of the mechanical behavior and vibration character of bilayer h-BN nanosheets under five different stacking modes, which could benefit its application in advanced nanodevices.

High-Mobility Compensated Semimetals, Orbital Magnetization, and Umklapp Scattering in Bilayer Graphene Moiré Superlattices.

Twist-controlled moiré superlattices (MSs) have emerged as a versatile platform for realizing artificial systems with complex electronic spectra. The combination of Bernal-stacked bilayer graphene (BLG) and hexagonal boron nitride (hBN) can give rise to an interesting MS, which has recently featured a set of unexpected behaviors, such as unconventional ferroelectricity and the electronic ratchet effect. Yet, the understanding of the electronic properties of BLG/hBN MS has, at present, remained fairly limited. Here, we combine magneto-transport and low-energy sub-THz excitation to gain insights into the properties of this MS. We demonstrate that the alignment between BLG and hBN crystal lattices results in the emergence of compensated semimetals at some integer fillings of the moiré bands, separated by van Hove singularities where the Lifshitz transition occurs. A particularly pronounced semimetal develops when eight holes reside in the moiré unit cell, where coexisting high-mobility electron and hole systems feature strong magnetoresistance reaching 2350% already at B = 0.25 T. Next, by measuring the THz-driven Nernst effect in remote bands, we observe valley splitting, indicating an orbital magnetization characterized by a strongly enhanced effective gv-factor of 340. Finally, using THz photoresistance measurements, we show that the high-temperature conductivity of the BLG/hBN MS is limited by electron-electron umklapp processes. Our multifaceted analysis introduces THz-driven magnetotransport as a convenient tool to probe the band structure and interaction effects in van der Waals materials and provides a comprehensive understanding of the BLG/hBN MS.

Stacking effects on dynamic mechanical behavior of bilayer hexagonal boron nitride under impact

Hexagonal boron nitride (h-BN) is a promising material for ballistic armor due to its excellent mechanical properties, enriched by different bilayer stacking arrangements. Molecular dynamics methods are used to study the stacking effects on the static and dynamic mechanical properties of bilayer h-BN. The AB (nitrogen) stacked bilayer structure attracts our attention because of its superior interlayer synergistic ability to resist projectile indentation up to a maximum force of 152.89 nN, which is about 22.9 % higher than the average value of other stacked bilayers. The impact response of bilayer h-BN with AB (nitrogen) stacking arrangement is then investigated at velocities of 2–4 km/s, which has the highest critical perforation velocity of 3.075 km/s, increased by 36.7 % compared to monolayer h-BN. At a low impact velocity of 2.5 km/s, the AB (nitrogen) stacked h-BN bilayer spends the shortest time to dissipate the impact energy of projectile and remains intact, while the top layers of other stacked bilayers are penetrated. At high impact velocities, a perforation event occurs, accompanied by multiple deflections of crack tips from zigzag to armchair to zigzag again, which intrinsically enhances the toughness of material. This study provides more understanding of the dynamic mechanical behavior of bilayer h-BN, as well as the design of armor structures based on stacking arrangements of 2D materials.

Manipulating the Stacking in Two-Dimensional Hexagonal Boron Nitride Bilayers: Implications for Defect-Based Single Photon Emitters

Manipulating the Stacking in Two-Dimensional Hexagonal Boron Nitride Bilayers: Implications for Defect-Based Single Photon Emitters

Functionalized hexagonal boron nitride bilayers: desirable electro-optical properties for optoelectronic applications.

Structural, electronic, and optical properties of functionalized hexagonal boron nitride (h-BN) bilayer were deeply explored by carrying out the PBE + G0W0 + BSE calculations. Hydrogenation/hydrofluorination/fluorination can cause the planar h-BN bilayer to form a novel diamane-like monolayer by interfacial sp3 atom bonding. These functionalized h-BN bilayers are estimated to be stable dynamically due to their phonon dispersions. The functionalization on h-BN bilayer can induce its electronic nature to be transformed from an indirect wide-gap insulator to direct narrow-gap semiconductor, which is desirable for its application in optoelectronics. In particular, hydrogenated and hydrofluorinated h-BN bilayers have strong absorbance coefficients for the near-infrared and visible part of the incident sunlight (larger than 105 cm-1). More interestingly, the binding energy of the observed first bright exciton can achieve a value beyond 1 eV, which can effectively reduce the recombination of photogenerated electron-hole pairs. These results are potentially important for extending the applications of the h-BN bilayer in optoelectronic devices.

Substrate Ferroelectric Proximity Effects Have a Strong Influence on Charge Carrier Lifetime in Black Phosphorus.

By stacking monolayer black phosphorus (MBP) with nonpolarized and ferroelectric polarized bilayer hexagonal boron nitride (h-BN), we demonstrate that ferroelectric proximity effects have a strong influence on the charge carrier lifetime of MBP using nonadiabatic (NA) molecular dynamics simulations. Through enhancing the motion of phosphorus atoms, ferroelectric polarization enhances the overlap of electron-hole wave functions that improves NA coupling and decreases the bandgap, resulting in a rapid electron-hole recombination completing within a quarter of nanoseconds, which is two times shorter than that in nonpolarized stackings. In addition to the dominant in-plane Ag2 mode in free-standing MBP, the out-of-plane high-frequency Ag1 and low-frequency interlayer breathing modes presented in the heterojunctions drive the recombination. Notably, the resonance between the breathing mode within bilayer h-BN and the B1u mode of MBP provides an additional nonradiative channel in ferroelectric stackings, further accelerating charge recombination. These findings are crucial for charge dynamics manipulation in two-dimensional materials via substrate ferroelectric proximity effects.

Effect of stacking configuration on high harmonic generation from bilayer hexagonal boron nitride.

High harmonic generation from bilayer h-BN materials with different stacking configurations is theoretically investigated by solving the extended multiband semiconductor Bloch equations in strong laser fields. We find that the harmonic intensity of AA'-stacking bilayer h-BN is one order of magnitude higher than that of AA-stacking bilayer h-BN in high energy region. The theoretical analysis shows that with broken mirror symmetry in AA'-stacking, electrons have much more opportunities to transit between each layer. The enhancement in harmonic efficiency originates from additional transition channels of the carriers. Moreover, the harmonic emission can be dynamically manipulated by controlling the carrier envelope phase of the driving laser and the enhanced harmonics can be utilized to achieve single intense attosecond pulse.

Computational study on the impact of Nb doping on electronic structure, magnetic and optical properties of hexagonal bilayer BN

We investigate the impact of Niobium (Nb) doping on the electronic structure, and magnetic and optical properties of the bilayer hexagonal boron nitride (BL hBN) using spin-polarized density functional theory (DFT). The calculated values of formation energy reveal the structural stability of Nb-doped BL hBN. The structural parameter analysis indicates the bond length and lattices constant of BL hBN increase due to Nb doping. In addition, it is found that the energy band gap of BL hBN is reduced from 5.1 eV to 3.9 eV due to 5.5% of Nb doping. Moreover, the obtained magnetic moment of 2 μ B and 4 μ B for Nb concentrations of 5.55% and 11.11% respectively, indicate the turning of the paramagnetic behavior of pure BL hBN to ferromagnetic. Besides, we have also found that the first and second nearest neighboring (NN) magnetic interaction between two dopants (Nb atoms) is ferromagnetic. Whereas, the third nearest neighbor interaction is antiferromagnetic. More interestingly, using mean field theory together with spin-polarized DFT ferromagnetic transition temperature (T c ) of 367 K is obtained for 11.11% of Nb-doped BL hBN. Furthermore, a significant enhancement of the absorption coefficient due to Nb doping in both the visible and mid-to-far-infrared regions was observed. Based on those results, we suggest that Nb-doped BL hBN is a good candidate material for nanoelectronics, spintronics, and optoelectronics applications.

The encapsulation of atomically-thin MgB2-based superconductors in two-dimensional material bilayers

Two-dimensional (2D) superconductors are a class of materials with unique properties that can potentially exhibit novel superconductivity at a reduced dimensionality, as well as pave the way for miniaturizing superconducting devices at the atomic limit. However, such materials are highly sensitive to interaction with their substrates and the environment, and therefore it is necessary to find potential methods for chemically isolating them. We address this problem by examining the possibility of isolating the medium-temperature 2D MgB2-based superconductors. We examine two possible structures: the monolayer stoichiometric MgB2 and the B-caged Mg3B8 structure. By solving the anisotropic Eliashberg equations, we predict that the latter possesses K upon application of a small lateral (3% tensile) strain, with an electron–phonon coupling of 0.88. To investigate protecting the superconductivity of these two layers, we apply density functional theory calculations to examine their encapsulation in a graphene bilayer or a hexagonal boron nitride bilayer. We find that both have high potential as encapsulation systems to protect the superconductivity of the 2D MgB2-based superconductors, in particular B-caged (B–Mg) n systems.

Moiré and non-twisted sp3-hybridized structures based on hexagonal boron nitride bilayers: Ab initio insight into infrared and Raman spectra, bands structures and mechanical properties

We investigated hydrogenated twisted (21.8°) and non-twisted bilayer structures consisting of two hexagonal boron nitride (hBN) monolayers with interlayer covalent bonds. These structures, named bornitranes, are boron nitride analogues of well-known carbon diamanes. We found that the binding energy of twisted structures was about 0.5 eV/BN higher than that of non-twisted AA’- and AB-stacked hBN layers. According to our calculations, the fully hydrogenated Moiré bornitrane with the 21.8° twisted angle has a flattened valence band and an indirect band gap of about 2.8 eV. This value is almost twice wider than that for their non-twisted counterparts. The computed Young’s modulus of bornitranes is higher than that for the hBN monolayer. The infrared and Raman spectra of the considered systems were also defined. Spectral fingerprints of the Moiré bornitrane possess many peaks due to the presence of distorted interlayer bonds and are radically different from the spectra of non-twisted systems. Calculated peaks can facilitate experimental detection of the Moiré bornitranes. Investigated structures are novel 2D semiconductors suitable for nanoelectronics and optoelectronics applications.

Localized interlayer excitons in MoSe2–WSe2 heterostructures without a moiré potential

Interlayer excitons (IXs) in MoSe2–WSe2 heterobilayers have generated interest as highly tunable light emitters in transition metal dichalcogenide (TMD) heterostructures. Previous reports of spectrally narrow (<1 meV) photoluminescence (PL) emission lines at low temperature have been attributed to IXs localized by the moiré potential between the TMD layers. We show that spectrally narrow IX PL lines are present even when the moiré potential is suppressed by inserting a bilayer hexagonal boron nitride (hBN) spacer between the TMD layers. We compare the doping, electric field, magnetic field, and temperature dependence of IXs in a directly contacted MoSe2–WSe2 region to those in a region separated by bilayer hBN. The doping, electric field, and temperature dependence of the narrow IX lines are similar for both regions, but their excitonic g-factors have opposite signs, indicating that the origin of narrow IX PL is not the moiré potential.

Anomalous ferroelectricity and double-negative effects in bilayer hexagonal boron nitride

Recently, the presence of an out-of-plane ferroelectric polarization was experimentally confirmed in bilayer two-dimensional (2D) hexagonal boron nitride (h-BN). In this work, we employ first-principles computations to reveal that (i) such slidetronic ferroelectricity is electronic in nature and arises from in-plane interlayer translation, which is distinctive among 2D slidetronic ferroelectric materials; and (ii) there is a coexistence of a negative longitudinal piezoelectric effect and an out-of-plane negative Poisson's ratio in the ferroelectric state of bilayer h-BN, which we refer to as anomalous double-negative effects.

Effect of Interlayer Coupling and Symmetry on High-Order Harmonic Generation from Monolayer and Bilayer Hexagonal Boron Nitride

High-order harmonic generation (HHG) is a fundamental process which can be simplified as the production of high energetic photons from a material subjected to a strong driving laser field. This highly nonlinear optical process contains rich information concerning the electron structure and dynamics of matter, for instance, gases, solids and liquids. Moreover, the HHG from solids has recently attracted the attention of both attosecond science and condensed matter physicists, since the HHG spectra can carry information of electron-hole dynamics in bands and inter- and intra-band current dynamics. In this paper, we study the effect of interlayer coupling and symmetry in two-dimensional (2D) material by analyzing high-order harmonic generation from monolayer and two differently stacked bilayer hexagonal boron nitrides (hBNs). These simulations reveal that high-order harmonic emission patterns strongly depend on crystal inversion symmetry (IS), rotation symmetry and interlayer coupling.

Nucleation and growth of stacking-dependent nanopores in bilayer h-BN.

The nucleation and growth of well-defined nanopores are presented under electron irradiation in h-BN bilayers with various stacking angles. The pores are initiated by the formation of boron vacancies in each basal layer, and then evolve into either triangular or hexagonal pores, which is dependent on the relative rotation between BN layers. The result may shed light on the rational design and fabrication of nanopores.

Moiré and Non-Twisted Sp3-Hybridized Structures Based on Hexagonal Boron Nitride Bilayers: Ab Initio Insight into Infrared and Raman Spectra, Bands Structures and Mechanical Properties

Moiré and Non-Twisted Sp3-Hybridized Structures Based on Hexagonal Boron Nitride Bilayers: Ab Initio Insight into Infrared and Raman Spectra, Bands Structures and Mechanical Properties

Giant tunnelling electroresistance through 2D sliding ferroelectric materials.

Very recently, ferroelectric polarization in staggered bilayer hexagonal boron nitride (BBN) and its novel sliding inversion mechanism were reported experimentally (Science2021, 372, 1458; 2021, 372, 1462), which paved a new way to realizing van der Waals (vdW) ferroelectric devices with new functionalities. Here, we develop vdW sliding ferroelectric tunnel junctions (FTJs) using the sliding ferroelectric BBN unit as an ultrathin barrier and explore their transport properties with different ferroelectric states and metal contacts via first principles. It is found that the electrode/BBN contact electric field quenches the ferroelectricity in the staggered BBN, resulting in a very small tunnelling electroresistance (TER). Inserting high-mobility 2D materials between Au and BN can restore the BBN ferroelectricity, reaching a giant TER of ∼10 000% in sliding FTJs. We finally investigate the metal-contact and thickness effect on the tunnelling property of sliding FTJs. The giant TER and multiple non-volatile resistance states in vdW sliding FTJs show promising applications in voltage-controlled nano-memories with ultrahigh storage density.

Tunable enhanced spatial shifts of reflective beam on the surface of a twisted bilayer of hBN

We investigated Goos–Hänchen (GH) and Imbert–Fedorov (IF) shifts of a reflective beam on a twisted bilayer of hexagonal boron nitride (hBN), where a left circularly polarized beam was incident on the surface. Our results demonstrate that the twist angle between the two optical axes plays an important role in obtaining large shifts with a high reflectivity. The GH shift with 10λ 0 is achieved, while the reflectivity is near 100% by tuning the twist angle. The maximum of the IF shift is found in the certain condition satisfied by the reflective coefficients, and the shift strongly depends on the twist angle between the optical axes of the two slabs. The spatial shifts obtained directly from the GH and IF shift definitions were provided, which indicate that the theoretical results from the stationary phase method are believable. These results may open up a new way for developing the nano-optical devices.