Twisted Layers Research Articles

Bright excitons in black phosphorus.

Twisted layers of atoms provide a tunable playground for quantum optoelectronics.

Twisted perovskite layers come together.

Twisted perovskite layers come together.

Amplification of interlayer exciton emission in twisted WSe2/WSe2/MoSe2 heterotrilayers

Van der Waals heterostructures based on transition metal dichalcogenides exhibit physical properties that depend on their monolayer constituents’ twisting angle and stacking order. Particularly in type-II heterostructures, low-energy photoluminescence is dominated by interlayer excitons, resulting in low emission yields, which drastically hampers their optoelectronic applicability. This study reports on the photoluminescence quantum yield of heterostructures consisting of WSe2/WSe2/MoSe2 twisted layers. Our findings show that the additional WSe2 monolayer in the trilayer system enhances the low-energy photoluminescence by more than an order of magnitude depending on the WSe2/WSe2 twist-angle in comparison to their WSe2/MoSe2 heterobilayer counterpart. Furthermore, combining density functional theory calculations and extracted degree of circular polarization, we identify excitonic signatures arising from hybridized states that originate from the additional WSe2 layer. In addition to providing an additional understanding of hybridization effects in 2D semiconducting heterostructures, our findings provide a viable method to enhance emission in van der Waals heterostructures, relevant for studying the fundamental properties of excitons and enabling optoelectronic applications with high luminescence yield.

Unraveling the Interactions between Lithium and Twisted Graphene.

Graphene is undoubtedly the carbon allotrope that has attracted the attention of a myriad of researchers in the last decades more than any other. The interaction of external or intercalated Li and Li+ with graphene layers has been the subject of particular attention for its importance in the applications of graphene layers in Lithium Batteries (LiBs). It is well known that lithium atoms and Li+ can be found inside and/or outside the double layer of graphene, and the graphene layers are often twisted around its parallel plane to obtain twisted graphene with tuneable properties. Thus, in this research, the interactions between Li and Li+ with bilayer graphene and twisted bilayer graphene were investigated by a first-principles density functional theory method, considering the lithium atom and the cation at different symmetry positions and with two different adsorption configurations. Binding energies and equilibrium interlayer distances of filled graphene layers were obtained from the computed potential energy profiles. This work shows that the twisting can regulate the interaction of bilayer graphene with Li and Li+. The binding energies of Li+ systematically increase from bilayer graphene to twisted graphene regardless of twisted angles, while for lithium atoms, the binding energies decrease or remain substantially unchanged depending on the twist angles. This suggests a higher adsorption capacity of twisted graphene towards Li+, which is important for designing twisted graphene-based material for LiB anode coating. Furthermore, when the Li or Li+ is intercalated between two graphene layers, the equilibrium interlayer distances in the twisted layers increase compared to the unrotated bilayer, and the relaxation is more significant for Li+ with respect to Li. This suggests that the twisted graphene can better accommodate the cation in agreement with the above result. The outcomes of this research pave the way for the study of the selective properties of twisted graphene.

Light-wave-controlled Haldane model in monolayer hexagonal boron nitride

In recent years, the stacking and twisting of atom-thin structures with matching crystal symmetry has provided a unique way to create new superlattice structures in which new properties emerge1,2. In parallel, control over the temporal characteristics of strong light fields has allowed researchers to manipulate coherent electron transport in such atom-thin structures on sublaser-cycle timescales3,4. Here we demonstrate a tailored light-wave-driven analogue to twisted layer stacking. Tailoring the spatial symmetry of the light waveform to that of the lattice of a hexagonal boron nitride monolayer and then twisting this waveform result in optical control of time-reversal symmetry breaking5 and the realization of the topological Haldane model6 in a laser-dressed two-dimensional insulating crystal. Further, the parameters of the effective Haldane-type Hamiltonian can be controlled by rotating the light waveform, thus enabling ultrafast switching between band structure configurations and allowing unprecedented control over the magnitude, location and curvature of the bandgap. This results in an asymmetric population between complementary quantum valleys that leads to a measurable valley Hall current7, which can be detected by optical harmonic polarimetry. The universality and robustness of our scheme paves the way to valley-selective bandgap engineering on the fly and unlocks the possibility of creating few-femtosecond switches with quantum degrees of freedom.

High-temperature Josephson diode.

Many superconducting systems with broken time-reversal and inversion symmetry show a superconducting diode effect, a non-reciprocal phenomenon analogous to semiconducting p-n-junction diodes. While the superconducting diode effect lays the foundation for realizing ultralow dissipative circuits, Josephson-phenomena-based diode effect (JDE) can enable the realization of protected qubits. The superconducting diode effect and JDE reported thus far are at low temperatures (~4 K), limiting their applications. Here we demonstrate JDE persisting up to 77 K using an artificial Josephson junction of twisted layers of Bi2Sr2CaCu2O8+δ. JDE manifests as an asymmetry in the magnitude and distributions of switching currents, attaining the maximum at 45° twist. The asymmetry is induced by and tunable with a very small magnetic field applied perpendicular to the junction and arises due to interaction between Josephson and Abrikosov vortices. We report a large asymmetry of 60% at 20 K. Our results provide a path towards realizing superconducting Josephson circuits at liquid-nitrogen temperature.

Unveiling The Unconventional Superconductivity Via Cuprates and Twisted Bilayer Graphene

Since the twentieth century, the exploration of superconducting material, a type of material that exhibits zero electrical resistance, has remained a paramount topic of inquiry within the scientific community seeing its excellent potential in bringing dramatical improvement to the material science and electric power and high-field magnet technology. However, earliest materials with superconducting aptitude requires extreme condition for critical temperature: It needs a temperature close to 0K, which is hard for application. This severe technical issue then led to an exploration to materials with higher temperature to reveal superconductivity. With decades of efforts, despite there are still arguments in working principle, new material like cooper oxide and iron-based material were found to have critical temperature higher than the limit predicted by Bardeen–Cooper–Schrieffer theory. However, recent experiment and accompanying working principle for the superconductivity of twisted layer graphene may suggest that it has greater potential in high temperature superconducting, due to its tunable property and relatively simpler working mechanism.

Twisted epitaxy of gold nanodisks grown between twisted substrate layers of molybdenum disulfide.

We expand the concept of epitaxy to a regime of "twisted epitaxy" with the epilayer crystal orientation between two substrates influenced by their relative orientation. We annealed nanometer-thick gold (Au) nanoparticles between two substrates of exfoliated hexagonal molybdenum disulfide (MoS2) with varying orientation of their basal planes with a mutual twist angle ranging from 0° to 60°. Transmission electron microscopy studies show that Au aligns midway between the top and bottom MoS2 when the twist angle of the bilayer is small (<~7°). For larger twist angles, Au has only a small misorientation with the bottom MoS2 that varies approximately sinusoidally with twist angle of the bilayer MoS2. Four-dimensional scanning transmission electron microscopy analysis further reveals a periodic strain variation (<|±0.5%|) in the Au nanodisks associated with the twisted epitaxy, consistent with the Moiré registry of the two MoS2 twisted layers.

A twisted carbonaceous nanotube as the air-electrode for flexible Zn-Air batteries.

Exploring electrocatalysts with high-efficiency oxygen reduction reaction (ORR) is significant for practical applications of fuel cells and metal-air batteries. In this work, a twisted core@shell material has been prepared with helical polypyrrole nanotubes (HPPys) as the core and coordination polymers (CPs) as the shell. After the pyrolysis process, a dense twisted carbon layer was formed by the reaction of CP and HPPy at its interface under Ar. The derived twisted carbonaceous nanotube exhibits good performance in both electrocatalytic ORR and OER. When used as the air-electrode in a flexible Zn-air battery, the battery shows good performance and stability.

Hydrogen Transport Between Layers of Transition Metal‐Dichalcogenides

AbstractHydrogen is a crucial source of green energy and is extensively studied for its potential usage in fuel cells. The advent of 2D crystals (2DCs) has taken hydrogen research to new heights, enabling it to tunnel through layers of 2DCs or be transported within voids between the layers, as demonstrated in recent experiments by Geim's group. In this study, it investigates how the composition and stacking of transition‐metal dichalcogenide (TMDC) layers influence the transport and self‐diffusion coefficients (D) of hydrogen atoms using well‐tempered metadynamics (WTMetaD) simulations. The findings show that modifying either the transition metal or the chalcogen atoms significantly affects the free energy barriers (ΔF) and, consequently, the self‐diffusion of hydrogen atoms between the 2DC layers. In the polytype (2H stacking), MoSe2 exhibits the lowest ΔF, while WS2 has the highest, resulting in the largest D for the former system. Additionally, hydrogen atoms inside the (or 3R) polytype encounter more than twice lower energy barriers and, thus, much higher diffusivity compared to those within the most stable stacking. These findings are particularly significant when investigating twisted layers or homo‐ or heterostructures, as different stacking areas may dominate over others, potentially leading to directional transport and interesting materials for ion or atom sieving.

Twist Phase Matching in Two-Dimensional Materials.

Optical phase matching involves establishing a proper phase relationship between the fundamental excitation and generated waves to enable efficient optical parametric processes. It is typically achieved through birefringence or periodic polarization. Here, we report that the interlayer twist angle in two-dimensional (2D) materials creates a nonlinear geometric phase that can compensate for the phase mismatch, and the vertical assembly of the 2D layers with a proper twist sequence generates a nontrivial "twist-phase-matching" (twist-PM) regime. The twist-PM model provides superior flexibility in the design of optical crystals, which can be applied for twisted layers with either periodic or random thickness distributions. The designed crystal from the twisted rhombohedral boron nitride films within a thickness of only 3.2 μm is capable of producing a second-harmonic generation with conversion efficiency of ∼8% and facile polarization controllability that is absent in conventional crystals. Our methodology establishes a platform for the rational design and atomic manufacturing of nonlinear optical crystals based on abundant 2D materials.

Moiré Superlattice Structure of Pleated Trilayer Graphene Imaged by 4D Scanning Transmission Electron Microscopy.

Moiré superlattices in graphene arise from rotational twists in stacked 2D layers, leading to specific band structures, charge density and interlayer electron and excitonic interactions. The periodicities in bilayer graphene moiré lattices are given by a simple moiré basis vector that describes periodic oscillations in atomic density. The addition of a third layer to form trilayer graphene generates a moiré lattice comprised of multiple harmonics that do not occur in bilayer systems, leading to nontrivial crystal symmetries. Here, we use atomic resolution 4D-scanning transmission electron microscopy to study atomic structure in bilayer and trilayer graphene moiré superlattices and use 4D-STEM to map the electric fields to show subtle variations in the long-range moiré patterns. We show that monolayer graphene folded into an S-bend graphene pleat produces trilayer moiré superlattices with both small (<2°) and larger twist angles (7-30°). Annular in-plane electric field concentrations are detected in high angle bilayers due to overlapping rotated graphene hexagons in each layer. The presence of a third low angle twisted layer in S-bend trilayer graphene, introduces a long-range modulation of the atomic structure so that no real space unit cell is detected. By directly imaging trilayer moiré harmonics that span from picoscale to nanoscale using 4D-STEM, we gain insights into the complex spatial distributions of atomic density and electric fields in trilayer twisted layered materials.

Visualizing moiré ferroelectricity via plasmons and nano-photocurrent in graphene/twisted-WSe2 structures

Ferroelectricity, a spontaneous and reversible electric polarization, is found in certain classes of van der Waals (vdW) materials. The discovery of ferroelectricity in twisted vdW layers provides new opportunities to engineer spatially dependent electric and optical properties associated with the configuration of moiré superlattice domains and the network of domain walls. Here, we employ near-field infrared nano-imaging and nano-photocurrent measurements to study ferroelectricity in minimally twisted WSe2. The ferroelectric domains are visualized through the imaging of the plasmonic response in a graphene monolayer adjacent to the moiré WSe2 bilayers. Specifically, we find that the ferroelectric polarization in moiré domains is imprinted on the plasmonic response of the graphene. Complementary nano-photocurrent measurements demonstrate that the optoelectronic properties of graphene are also modulated by the proximal ferroelectric domains. Our approach represents an alternative strategy for studying moiré ferroelectricity at native length scales and opens promising prospects for (opto)electronic devices.

Composite color filters for wide color gamut and high optical efficiency liquid crystal displays

We propose a composite color filter to achieve the wide color gamut and high optical efficiency of liquid crystal display (LCD). The composite color filter comprises a multi-layer polarization interference filter (ML-PIF) and a color filter. Specifically, two crossed polarizers and four twisted nematic liquid crystal layers with alternating opposite twisted directions form the ML-PIF. The Jones matrix method provides the transmittance formula of the ML-PIF. In the experiment, we successfully fabricate the blue and green ML-PIFs samples using the temperature birefringence effect of liquid crystal. When composite color filters (ML-PIF with certain color filters) are used in LCD, this can successfully achieve a color gamut of 122.3% NTSC and an absolute optical efficiency improvement of 1.4%. Alternatively, the composite color filter can attain a color gamut similar to that of a high-performance color filter and an absolute optical efficiency improvement of 3.8%. This composite color filter presents a tremendous opportunity for achieving a wide color gamut and high optical efficiency.

Conversion of chirality to twisting via sequential one-dimensional and two-dimensional growth of graphene spirals.

The properties of two-dimensional (2D) van der Waals materials can be tuned through nanostructuring or controlled layer stacking, where interlayer hybridization induces exotic electronic states and transport phenomena. Here we describe a viable approach and underlying mechanism for the assisted self-assembly of twisted layer graphene. The process, which can be implemented in standard chemical vapour deposition growth, is best described by analogy to origami and kirigami with paper. It involves the controlled induction of wrinkle formation in single-layer graphene with subsequent wrinkle folding, tearing and re-growth. Inherent to the process is the formation of intertwined graphene spirals and conversion of the chiral angle of 1D wrinkles into a 2D twist angle of a 3D superlattice. The approach can be extended to other foldable 2D materials and facilitates the production of miniaturized electronic components, including capacitors, resistors, inductors and superconductors.

Kinetic friction of structurally superlubric 2D material interfaces

The ultra-low kinetic friction Fk of 2D structurally superlubric interfaces, connected with the fast motion of the incommensurate moiré pattern, is often invoked for its linear increase with velocity v0 and area AS, but never seriously addressed and calculated so far. Here we do that, exemplifying with a twisted graphene layer sliding on top of bulk graphite – a demonstration case that could easily be generalized to other systems. Neglecting quantum effects and assuming a classical Langevin dynamics, we derive friction expressions valid in two temperature regimes. At low temperatures the nonzero sliding friction velocity derivative dFk/dv0 is shown by Adelman–Doll–Kantorovich type approximations to be equivalent to that of a bilayer whose substrate is affected by an analytically derived effective damping parameter, replacing the semi-infinite substrate. At high temperatures, friction grows proportional to temperature as analytically required by fluctuation–dissipation. The theory is validated by non-equilibrium molecular dynamics simulations with different contact areas, velocities, twist angles and temperatures. Using 6°-twisted graphene on Bernal graphite as a prototype we find a shear stress of measurable magnitude, from 25kPa at low temperature to 260kPa at room temperature, yet only at high sliding velocities such as 100m/s. However, it will linearly drop many orders of magnitude below measurable values at common experimental velocities such as 1μm/s, a factor 10−8 lower. The low but not ultra-low “engineering superlubric” friction measured in existing experiments should therefore be attributed to defects and/or edges, whose contribution surpasses by far the negligible moiré contribution.

Effect of Coulomb impurities on the electronic structure of magic angle twisted bilayer graphene

In graphene, charged defects break the electron-hole symmetry and can even give rise to exotic collapse states when the defect charge exceeds a critical value which is proportional to the Fermi velocity. In this work, we investigate the electronic properties of twisted bilayer graphene (tBLG) with charged defects using tight-binding calculations. Like monolayer graphene, tBLG exhibits linear bands near the Fermi level but with a dramatically reduced Fermi velocity near the magic angle (approximately 1.1°). This suggests that the critical value of the defect charge in magic-angle tBLG should also be very small. We find that charged defects give rise to significant changes in the low-energy electronic structure of tBLG. Depending on the defect position in the moiré unit cell, it is possible to open a band gap or to induce an additional flattening of the low-energy valence and conduction bands. Our calculations suggest that the collapse states of the two monolayers hybridize in the twisted bilayer. However, their in-plane localization remains largely unaffected by the presence of the additional twisted layer because of the different length scales of the moiré lattice and the monolayer collapse state wavefunctions. These predictions can be tested in scanning tunneling spectroscopy experiments.

Reflection of stepwise twisted stratified anisotropic optical media

Stratified optical films have fascinating optical properties and many important applications. Here we report a theoretical study of stepwise twisted stratified anisotropic optical media. We used Fourier transform to analyze the helical component of the dielectric tensor of the media. We then used the Berreman 4 × 4 method to calculate the reflection spectrum of the media. We discovered that right-handed and left-handed helices could coexist in stepwise twisted layers, which producing a simultaneous reflection of right-handed and left-handed circularly polarized light. This feature can be used to produce films with superior reflection properties, such as high reflectance, broad bandwidth reflection and short wavelength reflection.

Moiré Enhanced Potentials in Twisted Transition Metal Dichalcogenide Trilayers Homostructures.

The exploration of moiré superlatticesholds promising potential to uncovernovel quantum phenomena emerging from the interplay of atomic structure and electronic correlation . However, the impact of the moiré potential modulation on the number of twisted layers has yet to be experimentally explored. Here, this work synthesizes a twisted WSe2 homotrilayer using a dry-transfer method and investigates the enhancement of the moiré potential with increasing number of twisted layers. The results of the study reveal the presence of multiple exciton resonances with positive or negative circularly polarized emission in the WSe2 homostructure with small twist angles, which are attributed to the excitonic ground and excited states confined to the moiré potential. The distinct g-factor observed in the magneto-optical spectroscopy is also shown to be a result of the confinement of the exciton in the moiré potential. The moiré potential depths of the twisted bilayer and trilayer homostructures are found to be 111 and 212 meV, respectively, an increase of 91% from the bilayer structure. These findings demonstrate that the depth of the moiré potential can be manipulated by adjusting the number of stacked layers, providing a promising avenue for exploration into highly correlated quantum phenomena.

Thermal conductance of twisted-layer graphite nanofibers

We study the thermal transport properties of twisted-layer graphite nanofibers. We show that in the presence of a twisted layer, the phonon thermal conductance of a graphite nanofiber of rectangular cross-section varies remarkably with the twist angle and can reach minimum values either at two critical angles θ1 and θ2 that conform to the rule θ1+θ2=1800 or exactly at the angle θ= 900. A reduction of roughly 50% of the phonon thermal conductance can be achieved in some structures. We unveil that the twisting effect mainly influences the optical modes, more precisely, the breathing modes ZOꞌ, and leaving almost unaltered the acoustic ones. The effect is also visible in the higher and more numerous van Hove singularities of the phonon density of states. We also point out that the behavior of the thermal conductance with the twist angle is associated with and dominated by the alteration in the overlap area between the twisted and non-twisted layers. The finite-size effect is demonstrated to play an essential role in defining the critical angles at the local minima, where these angles are dependent on the size of the investigated nanofibers, in particular on the proportion between the widths of zigzag and armchair edges. We also analyze the behavior of circular nanofibers where the correlation between the overlap area and the thermal conductance is much smaller.