Long range piezoelectricity effects in van der Waals heterobilayer systems beyond 1000 atoms.

Twist angle is a relevant design and control component for the piezoelectric coefficients of van der Waals (vdW) heterostructures. This theoretical work assesses in high detail the impact of the twist angle on the piezoelectricity of two-dimensional (2D) heterobilayer systems. We expand the density-functional based tight-binding method to predict the piezoelectric coefficients of twisted and corrugated 2D heterobilayer structures with more than 1000 atoms. We showcase the method on hexagonal III-V/transition metal dichalcogenide vdW heterosystems. Our calculations yield a periodic relationship between the in-plane piezoelectric coefficients and the corresponding twist angles, indicating the tunability of the in-plane piezoelectricity. In contrast, the out-of-plane piezoelectricity is not twist angle dependent, but nonlinearly changes with the average interlayer distance.

Twist-Angle Tuning of Electronic Structure in Two-Dimensional Dirac Nodal Line Semimetal Au2Ge on Au(111).

Topological semimetals have emerged as quantum materials including Dirac, Weyl, and nodal line semimetals, and so on. Dirac nodal line (DNL) semimetals possess topologically nontrivial bands crossing along a line or a loop and are considered precursor states for other types of semimetals. Here, we combine scanning tunneling microscopy/spectroscopy (STM/S) measurements and density functional theory (DFT) calculations to investigate a twist angle tuning of electronic structure in two-dimensional DNL semimetal Au2Ge. Theoretical calculations show that two bands of Au2Ge touch each other in Γ-M and Γ-K paths, forming a DNL. A significant transition of electronic structure occurs by tuning the twist angle from 30° to 24° between monolayer Au2Ge and Au(111), as confirmed by STS measurements and DFT calculations. The disappearing of DNL state is a direct consequence of symmetry breaking.

Twisted Integration of Complex Oxide Magnetoelectric Heterostructures via Water-Etching and Transfer Process.

HIGHLIGHTS: The (001)-oriented ferromagnetic La0.67Sr0.33MnO3 films are stuck onto the (011)-oriented ferroelectric single-crystal 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 substrate with 0° and 45° twist angle. By applying a 7.2 kV cm-1 electric field, the coexistence of uniaxial and fourfold in-plane magnetic anisotropy is observed in 45° Sample, while a typical uniaxial anisotropy is found in 0° Sample. Manipulating strain mode and degree that can be applied to epitaxial complex oxide thin films have been a cornerstone of strain engineering. In recent years, lift-off and transfer technology of the epitaxial oxide thin films have been developed that enabled the integration of heterostructures without the limitation of material types and crystal orientations. Moreover, twisted integration would provide a more interesting strategy in artificial magnetoelectric heterostructures. A specific twist angle between the ferroelectric and ferromagnetic oxide layers corresponds to the distinct strain regulation modes in the magnetoelectric coupling process, which could provide some insight in to the physical phenomena. In this work, the La0.67Sr0.33MnO3 (001)/0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (011) (LSMO/PMN-PT) heterostructures with 45º and 0º twist angles were assembled via water-etching and transfer process. The transferred LSMO films exhibit a fourfold magnetic anisotropy with easy axis along LSMO < 110 >. A coexistence of uniaxial and fourfold magnetic anisotropy with LSMO [110] easy axis is observed for the 45° Sample by applying a 7.2 kV cm-1 electrical field, significantly different from a uniaxial anisotropy with LSMO [100] easy axis for the 0° Sample. The fitting of the ferromagnetic resonance field reveals that the strain coupling generated by the 45° twist angle causes different lattice distortion of LSMO, thereby enhancing both the fourfold and uniaxial anisotropy. This work confirms the twisting degrees of freedom for magnetoelectric coupling and opens opportunities for fabricating artificial magnetoelectric heterostructures.

Twist-Angle-Dependent Electronic Properties of Exfoliated Single Layer MoS2 on Au(111).

Synthetic materials and heterostructures obtained by the controlled stacking of exfoliated monolayers are emerging as attractive functional materials owing to their highly tunable properties. We present a detailed scanning tunneling microscopy and spectroscopy study of single layer MoS2-on-gold heterostructures as a function of the twist angle. We find that their electronic properties are determined by the hybridization of the constituent layers and are modulated at the moiré period. The hybridization depends on the layer alignment, and the modulation amplitude vanishes with increasing twist angle. We explain our observations in terms of a hybridization between the nearest sulfur and gold atoms, which becomes spatially more homogeneous and weaker as the moiré periodicity decreases with increasing twist angle, unveiling the possibility of tunable hybridization of electronic states via twist angle engineering.

Effect of Twist Angle on Interfacial Thermal Transport in Two-Dimensional Bilayers.

Advances in two-dimensional (2D) devices require innovative approaches for manipulating transport properties. Analogous to the electrical and optical responses, it has been predicted that thermal transport across 2D materials can have a similar strong twist-angle dependence. Here, we report experimental evidence deviating from this understanding. In contrast to the large tunability in electrical transport, we measured an unexpected weak twist-angle dependence of interfacial thermal transport in MoS2 bilayers, which is consistent with theoretical calculations. More notably, we confirmed the existence of distinct regimes with weak and strong twist-angle dependencies for thermal transport, where, for example, a much stronger change with twist angles is expected for graphene bilayers. With atomic simulations, the distinct twist-angle effects on different 2D materials are explained by the suppression of long-wavelength phonons via the moiré superlattice. These findings elucidate the unique feature of 2D thermal transport and enable a new design space for engineering thermal devices.

Effects of Twisting and Surface Finish on the Mechanical Properties of Natural Gut Harp Strings.

Natural gut harp strings are made from twisted bundles of gut strips, which are dried, ground, and varnished. The effects of varying the twist angle and surface finishing on the mechanical properties of gut harp strings have been explored. Strings were tested over a range of twist angles from 23.5∘ to 58.3∘, and with all four combinations of ground or unground and varnished or unvarnished surface finishing. The principal effects of varying the degree of twisting were that the breaking strength and tensile Young's modulus both fell as the twist angle was increased. String makers must therefore make a compromise between sound quality and string strength and durability. Leaving the string unvarnished dramatically increased the sensitivity to changes in humidity, which, in turn, affected the thermal tuning sensitivity and creep behaviour. Grinding the string surface prior to varnishing had no significant effect on the behaviour, but did make some difference to the thermal tuning sensitivity if the string was left unvarnished. Increasing the humidity frequently triggered episodes of additional string creep. There appeared to be a threshold effect, with the additional creep triggered when the string linear density exceeded its previous maximum. When the string was not creeping, there appeared to be a strong coupling mechanism between changes in the linear density and complementary changes in the string tension, such that there was almost no net effect on the string frequency. This behaviour was independent of the twist angle and the surface finishing, suggesting that whatever the coupling mechanism was, it was not dependent on the twisted structure of the string.

Deformation Coupled Moiré Mapping of Superlubricity in Graphene.

The ultralow friction of two-dimensional (2D) materials, commonly referred to as superlubricity, has been associated with Moiré superlattices (MSLs). While MSLs have been shown to play a crucial role in achieving superlubricity, the long-standing challenge of achieving superlubricity in engineering has been attributed to surface roughness, which tends to destroy MSLs. Here, we show via molecular dynamics simulations that MSLs alone are not capable of capturing the friction behavior of a multilayer-graphene-coated substrate where similar MSLs persist in spite of significant changes in friction as the graphene coating thickness increases. To resolve this problem, a deformation coupled contact pattern is constructed to describe the spatial distribution of the atomic contact distance. It is shown that as the graphene thickness increases, the interfacial contact distance is determined by a competition between increased interfacial MSLs interactions and reduced out-of-plane deformation of the surface. A frictional Fourier transform model is further proposed to distinguish between intrinsic and extrinsic contributions to friction, with results showing that thicker graphene coatings exhibit lower intrinsic friction and higher sliding stability. These results shed light on the origin of interfacial superlubricity in 2D materials and may guide related applications in engineering.

Multiscale Study of the Effect of Fiber Twist Angle and Interface on the Viscoelasticity of 2D Woven Composites.

Time and temperature affect the viscoelasticity of woven composites, and thus affect their long-term mechanical properties. We develop a multiscale method considering fiber twist angle and interfaces to predict viscoelasticity. The multiscale approach is based on homogenization theory and the time-temperature superposition principle (TTSP). It is carried out in two steps. Firstly, the effective viscoelasticity properties of yarn are calculated using microscale homogenization; yarn comprises elastic fibers, interface, and a viscoelastic matrix. Subsequently, the effective viscoelasticity properties of woven composites are computed by mesoscale homogenization; it consists of homogenized viscoelastic yarns and matrix. Moreover, the multiscale method is verified using the Mechanics of Structure genome (MSG) consequence. Finally, the effect of temperature, fiber twist angle, fiber array, and coating on either the yarn's effective relaxation stiffness or the relaxation moduli of the woven composite is investigated. The results show that increased temperature shortens the relaxation time of viscoelastic woven composites, and fiber twist angle affects tensors in the relaxation stiffness matrix of the yarn; the coating affects the overall mechanical properties of woven composites as well.

Superior Thermoelectric Properties of Twist-Angle Superlattice Borophene Induced by Interlayer Electrons Transport.

In this paper, the energy bands, interlayer interactions and thermoelectric effects of twisted bilayer borophene (TBB) synthesized on Ag (111) are studied theoretically. The results manifest the advantages of twistronics, where the high electrical conductivity and the large Seebeck coefficient are regulated to the same range, which lead to the significantly increase of figure of merit ZT than that of bilayer borophene (BB) without twist, where the BB without twist is successfully synthesized on Ag (111) film is recently experimental report [Nat. Mater. 2022, 21, 35]. For the TBB synthesized of on Ag (111) film, theoretical analysis demonstrates that TBB and Ag are relatively strongly coupled, and TBB becomes a metallic 2D material, where the top and bottom borophene layers are semiconducting and metallic, respectively. TBB exhibits excellent thermoelectric efficiency due to the charge transfer bonding between the layers, less electron localization, and the regulation of Seebeck coefficient, electrical conductivity, and ZT at the same region of chemical potential and the same temperature by twistronics. The structure-property relationship offers the possibility of applying TBB in thermoelectric devices.

Robust Interlayer-Coherent Quantum Hall States in Twisted Bilayer Graphene.

We introduce a novel two-dimensional electronic system with ultrastrong interlayer interactions, namely, twisted bilayer graphene with a large twist angle, as an ideal ground for realizing interlayer-coherent excitonic condensates. In these systems, sub-nanometer atomic separation between the layers allows significant interlayer interactions, while interlayer electron tunneling is geometrically suppressed due to the large twist angle. By fully exploiting these two features we demonstrate that a sequence of odd-integer quantum Hall states with interlayer coherence appears at the second Landau level (N = 1). Notably the energy gaps for these states are of order 1 K, which is several orders of magnitude greater than those in GaAs. Furthermore, a variety of quantum Hall phase transitions are observed experimentally. All the experimental observations are largely consistent with our phenomenological model calculations. Hence, we establish that a large twist angle system is an excellent platform for high-temperature excitonic condensation.

One Dimensional Twisted Van der Waals Structures Constructed by Self-Assembling Graphene Nanoribbons on Carbon Nanotubes.

Twisted van der Waals heterostructures were recently found to possess unique physical properties, such as superconductivity in magic angle bilayer graphene. Owing to the nonhomogeneous stacking, the energy of twisted van der Waals heterostructures are often higher than their AA or AB stacking counterpart, therefore, fabricating such structures remains a great challenge in experiments. On the other hand, one dimensional (1D) coaxial van der Waals structures has less freedom to undergo phase transition, thus offer opportunity for fabricating the 1D cousin of twisted bilayer graphene. In this work, we show by molecular dynamic simulations that graphene nanoribbons can self-assemble onto the surface of carbon nanotubes driven by van der Waals interactions. By modifying the size of the carbon nanotubes or graphene nanoribbons, the resultant configurations can be controlled. Of particular interest is the formation of twisted double walled carbon nanotubes whose chiral angle difference can be tuned, including the 1.1° magic angle. Upon the longitudinal unzipping of such structures, twisted bilayer graphene nanoribbons can be obtained. As the longitudinal unzipping of carbon nanotubes is a mature technique, we expect the strategy proposed in this study to stimulate experimental efforts and promote the fast growing research in twistronics.

Twist Angle-Dependent Molecular Intercalation and Sheet Resistance in Bilayer Graphene.

Bilayer graphene (BLG) has a two-dimensional (2D) interlayer nanospace that can be used to intercalate molecules and ions, resulting in a significant change of its electronic and magnetic properties. Intercalation of BLG with different materials, such as FeCl3, MoCl5, Li ions, and Ca ions, has been demonstrated. However, little is known about how the twist angle of the BLG host affects intercalation. Here, by using artificially stacked BLG with controlled twist angles, we systematically investigated the twist angle dependence of intercalation of metal chlorides. We discovered that BLG with high twist angles of >15° is more favorable for intercalation than BLG with low twist angles. Density functional theory calculations suggested that the weaker interlayer coupling in high twist angle BLG is the key for effective intercalation. Scanning transmission electron microscope observations revealed that co-intercalation of AlCl3 and CuCl2 molecules into BLG gives various 2D structures in the confined interlayer nanospace. Moreover, before intercalation we observed a significantly lower sheet resistance in BLG with high twist angles (281 ± 98 Ω/□) than that in AB stacked BLG (580 ± 124 Ω/□). Intercalation further decreased the sheet resistance, reaching values as low as 48 Ω/□, which is the lowest value reported so far for BLG. This work provides a twist angle-dependent phenomenon, in which enhanced intercalation and drastic changes of the electrical properties can be realized by controlling the stacking angle of adjacent graphene layers.

Identification of twist-angle-dependent excitons in WS2/WSe2 heterobilayers.

Stacking atomically thin films enables artificial construction of van der Waals heterostructures with exotic functionalities such as superconductivity, the quantum Hall effect, and engineered light-matter interactions. In particular, heterobilayers composed of monolayer transition metal dichalcogenides have attracted significant interest due to their controllable interlayer coupling and trapped valley excitons in moiré superlattices. However, the identification of twist-angle-modulated optical transitions in heterobilayers is sometimes controversial since both momentum-direct (K-K) and -indirect excitons reside on the low energy side of the bright exciton in the monolayer constituents. Here, we attribute the optical transition at ∼1.35 eV in the WS2/WSe2 heterobilayer to an indirect Γ-K transition based on a systematic analysis and comparison of experimental photoluminescence spectra with theoretical calculations. The exciton wavefunction obtained by the state-of-the-art GW-Bethe-Salpeter equation approach indicates that both the electron and hole of the excitons are contributed by the WS2 layer. Polarization-resolved k-space imaging further confirms that the transition dipole moment of this optical transition is dominantly in-plane and is independent of the twist angle. The calculated absorption spectrum predicts that the so-called interlayer exciton peak coming from the K-K transition is located at 1.06 eV, but with a much weaker amplitude. Our work provides new insight into the steady-state and dynamic properties of twist-angle-dependent excitons in van der Waals heterostructures.

Electronically Weak Coupled Bilayer MoS2 at Various Twist Angles via Folding.

Constructing a bilayer system with defined twist angles is an effective way to engineer the physical properties of two-dimensional (2D) materials, opening up a new research area of twistronics. How to achieve high-quality bilayer 2D materials in a controlled and mass production way is of primary importance to this emerging area. In this work, we present a strategy for the large-scale fabrication of twisted bilayer molybdenum disulfide (MoS2) through photolithography patterning and folding of single-crystal monolayer MoS2. Atomic resolution transmission electron spectroscopy directly confirms that the as-achieved folded bilayer MoS2 is of high quality with targeted twist angles. Various twist angles result in tuning Raman mode frequencies and direct optical transition energies. Due to the weak interlayer coupling between the twisted layers, folded bilayers exhibit an extremely high photoluminescence with doubled intensity as compared to the unfolded monolayer, indicating a possible application in optoelectronic devices. Our work provides a new strategy to tailor the properties of MoS2, which will be beneficial to twistable electronics.

Stacking-Engineered Heterostructures in Transition Metal Dichalcogenides.

The layer-by-layer assembly of 2D transition metal dichalcogenide monolayer blocks to form a 3D stack, with a precisely chosen sequence/angle, is the newest development for these materials. In this way, one can create "van der Waals heterostructures (HSs)," opening up a new realm of materials engineering and novel devices with designed functionalities. Herein, a detailed systematic review of transition metal dichalcogenide stacking-engineered heterostructures, from controllable fabrication to typical characterization, and stacking-correlated physical behaviors is presented. Furthermore, recent advances in stacking design, such as stacking sequence, twist angles, and moiré superlattice heterojunctions, are also comprehensively summarized. Finally, the remaining challenges and possible strategies for using stacking engineering to tune the properties of 2D materials are also outlined.

Tunable Optical Properties of Thin Films Controlled by the Interface Twist Angle.

Control of materials properties has been the driving force of modern technologies. So far, materials properties have been modulated by their composition, structure, and size. Here, by using cathodoluminescence in a scanning transmission electron microscope, we show that the optical properties of stacked, >100 nm thick hexagonal boron nitride (hBN) films can be continuously tuned by their relative twist angles. Due to the formation of a moiré superlattice between the two interface layers of the twisted films, a new moiré sub-band gap is formed with continuously decreasing magnitude as a function of the twist angle, resulting in tunable luminescence wavelength and intensity increase of >40×. Our results demonstrate that moiré phenomena extend beyond monolayer-based systems and can be preserved in a technologically relevant, bulklike material at room temperature, dominating optical properties of hBN films for applications in medicine, environmental, or information technologies.

Chemical Route to Twisted Graphene, Graphene Oxide and Boron Nitride.

The recently discovered twisted graphene has attracted considerable interest. A simple chemical route was found to prepare twisted graphene by covalently linking layers of exfoliated graphene containing surface carboxyl groups with an amine-containing linker (trans-1,4-diaminocyclohexane). The twisted graphene shows the expected selected area electron diffraction pattern with sets of diffraction spots out with different angular spacings, unlike graphene, which shows a hexagonal pattern. Twisted multilayer graphene oxide could be prepared by the above procedure. Twisted boron nitride, prepared by cross-linking layers of boron nitride (BN) containing surface amino groups with oxalic acid linker, exhibited a diffraction pattern comparable to that of twisted graphene. First-principles DFT calculations threw light on the structures and the nature of interactions associated with twisted graphene/BN obtained by covalent linking of layers.

Understanding Interlayer Contact Conductance in Twisted Bilayer Graphene.

Bilayer or few-layer 2D materials showing novel electrical properties in electronic device applications have aroused increasing interest in recent years. Obtaining a comprehensive understanding of interlayer contact conductance still remains a challenge, but is significant for improving the performance of bilayer or few-layer 2D electronic devices. Here, conductive atomic force microscope (C-AFM) experiments are reported to explore the interlayer contact conductance between bilayer graphene (BLG) with various twisted stacking structures fabricated by the chemical vapor deposition (CVD) method. The current maps show that the interlayer contact conductance between BLG strongly depends on the twist angle. The interlayer contact conductance of 0° AB-stacking bilayer graphene (AB-BLG) is ≈4 times as large as that of 30° twisted bilayer graphene (t-BLG), which indicates that the twist angle-dependent interlayer contact conductance originates from the coupling-decoupling transitions. Moreover, the moiré superlattice-level current images of t-BLG show modulations of local interlayer contact conductance. Density functional theory calculations together with a theoretical model reproduce the C-AFM current map and show that the modulation is mainly attributed to the overall contribution of local interfacial carrier density and tunneling barrier.

Memory in the hippocampus.

To date, there is no clear evidence for memory formation. In this article, we provide a framework to understand how memory is formed. The information collected by sensory organs is converted to a digital current that enters the presynaptic neuron through axonal conductance. Digital waves are converted to analog waves in the synapses. The analog current of information flows into the postsynapse. The degree of Ca2+ influx in the postsynapse is proportional to the voltage of each wave of analog current. The activation (via dephosphorylation) of the phosphorylated phosphatase, Slingshot, is regulated by Ca2+ concentration in the spine. After dephosphorylation by Slingshot, activated cofilin binds the parallel actin bundle. The wide helical twist angle of an actin filament that has been decorated with cofilin confers high electric potential to the filament. Phosphorylation results in the deactivation of the actin filament bound to cofilin, which in turn results in the cleavage of cofilin and actin filament, followed by a decrease in the twist angle of the actin filament. Next, the electric potential energy is discharged by the actin filament as it returns to its non-cofilin bound state, resulting in the formation of additional analog waves in the postsynapse.

Twist-Angle-Dependent Optoelectronics in a Few-Layer Transition-Metal Dichalcogenide Heterostructure.

Lattice matching has been supposed to play an important role in the coupling between two materials in a vertical heterostructure (HS). To investigate this role, we fabricated a heterojunction device with a few layers of p-type WSe2 and n-type MoSe2 with different crystal orientation angles. The crystal orientations of WSe2 and MoSe2 were estimated using high-resolution X-ray diffraction. Heterojunction devices were fabricated with twist angles of 0, 15, and 30°. The I- V curve of the sample with the twist angle of 0° under the dark condition showed a diodelike behavior. The strong coupling due to lattice matching caused a well-established p-n junction. In cases of 15 and 30° samples, the van der Waals gap was built because of lattice mismatching, which resulted in the formation of a potential barrier. However, when the light-emitting diode light of 365 nm (3.4 eV) was illuminated, it was possible for excited electrons and holes to jump beyond the potential barrier and the current flowed well in both forward and reverse directions. The effects of the twist angle were analyzed by spectral responsivity and external quantum efficiency, where it was found that the untwisted HS exhibited higher sensitivity under IR illumination, whereas the twisting effect was not noticeable under UV illumination. From photoluminescence and Raman spectroscopy studies, it was confirmed that the twisted HS showed a weak coupling because of the lattice mismatch.