Interlayer Coupling Research Articles

Highly Tunable Interlayer Coupling and Electronic Structures of Few-Layer Graphene with Pressure.

The interlayer electronic coupling is responsible for the electronic structure evolution from monolayer graphene to graphite and for the moiré potential in twisted bilayer graphene. Here we demonstrate that the interlayer transfer integral (hopping parameter) increases nearly 40% with a quite moderate pressure of ∼3.5 GPa, manifested by the resonance peak shift in the infrared spectra of all 2-10 L graphene. A simple model based on the Morse potential enabled us to establish the relationship between the transfer integral and pressure. Our work provides fundamental insights into the dependence of the electronic coupling on the interlayer distance.

Ultrafast Decay of Interlayer Exciton in WS2/MoSe2 Heterostructure Under Pressure

AbstractAtomically thin transition metal dichalcogenides (TMDs) heterostructures provide a rich platform for exploring fascinating physics and engineering strategies. A pressure strategy is developed to effectively manipulate the physical properties in such heterostructures. However, there is still a lack of studies on the corresponding pressure‐modulated evolution of carrier dynamics, which is crucial to the performance of electronic and optoelectronic devices. Here, utilizing the diamond anvil cell, the interlayer exciton dynamics of WS2/MoSe2 heterostructure are subtly manipulated by pressure. Intriguingly, with pressure modulation, the enhanced interlayer coupling accelerates the recombination of spatially separated electron and hole, which significantly shortens the interlayer exciton lifetime from 37.10 ps at 0.0 Gpa to 3.03 ps at 2.2 Gpa. For comparison, the intralayer exciton lifetime of monolayer MoSe2 is increased due to the transition of direct to indirect bandgap under pressure. Furthermore, the pressure‐regulated band structure and interlayer coupling are confirmed by photoluminescence and Raman spectroscopy. The results demonstrate that pressure provides a powerful tuning knob for interlayer exciton relaxation of TMDs heterostructure, which is attractive to various electronic and optoelectronic applications based on such heterostructure.

Van der Waals Transition Metal Carbo-Chalcogenides: Theoretical Screening and Charge Storage.

High-rate lithium/sodium ion batteries or capacitors are the most promising functional units to achieve fast energy storage that highly depends on charge host materials. Host materials with lamellar structures are a good choice for hybrid charge storage hosts (capacitor or redox type). Emerging layered transition metal carbo-chalcogenides (TMCC) with homogeneous sulfur termination are especially attractive for charge storage. Using density functional theory calculations, six of 30 potential TMCC are screened to be stable, metallic, anisotropic in electronic conduction and mechanical properties due to the lamellar structures. Raman, infrared active modes and frequencies of the six TMCC are well assigned. Interlayer coupling, especially binding energies predict that the bulk layered materials can be easily exfoliated into 2D monolayers. Moreover, Ti2S2C, Zr2S2C are identified as the most gifted Li+/Na+ anode materials with relatively high capacities, moderate volume expansion, relatively low Li+/Na+ migration barriers for batteries or ion-hybrid capacitors. This work provides a foundation for rational materials design, synthesis, and identification of the emerging 2D family of TMCC.

Engineered moiré photonic and phononic superlattices.

Recent discoveries of Mott insulating and unconventional superconducting states in twisted bilayer graphene with moiré superlattices have not only reshaped the landscape of 'twistronics' but also sparked the rapidly growing fields of moiré photonic and phononic structures. These innovative moiré structures have opened new routes of exploration for classical wave physics, leading to intriguing phenomena and robust control of electromagnetic and mechanical waves. Drawing inspiration from the success of twisted bilayer graphene, this Perspective describes an overarching framework of the emerging moiré photonic and phononic structures that promise novel classical wave devices. We begin with the fundamentals of moiré superlattices, before highlighting recent studies that exploit twist angle and interlayer coupling as new ingredients with which to engineer and tailor the band structures and effective material properties of photonic and phononic structures. Finally, we discuss the future directions and prospects of this emerging area in materials science and wave physics.

Van Hove Singularity-Enhanced Raman Scattering and Photocurrent Generation in Twisted Monolayer-Bilayer Graphene.

Twisted monolayer-bilayer graphene (TMBG) has recently emerged as an exciting platform for exploring correlated physics and topological states with rich tunability. Strong light-matter interaction was realized in twisted bilayer graphene, boosting the development of broadband graphene photodetectors from the visible to infrared spectrum with high responsivity. Extending this approach to the case of TMBG will help design advanced quantum nano-optoelectronic devices because of the reduced symmetry of the system. Here, we observe the formation of van Hove singularities (VHSs) in TMBG by monitoring the significant enhancement of the Raman intensity of the G peak and the intensity ratio of G and 2D peaks. The strong interlayer coupling also leads to the appearance of twist-angle-dependent Raman R and R' peaks in TMBG. Furthermore, the constructed graphene photodetectors from 13.5°-TMBG show significantly enhanced photoresponsivity (∼31 folds of monolayer graphene and ∼15 folds of trilayer graphene) when the energy of incident photons matches the interval energy between the two VHSs in the conduction and valence bands. Our findings establish TMBG as a tunable platform for investigating the light-matter interaction and designing high-performance graphene photodetectors with combined high responsivity and high selectivity.

Emergence of Superconductivity in Indium Triphosphate via Pressure‐Tuned Interlayer Bond Formation

Tuning interlayer interactions offer an alternative approach to access novel electronic structure and intriguing physical properties in layered materials. Here, the emergence of a new form of superconductivity in two‐dimensional (2D) binary phosphides by strengthening the interlayer coupling with lattice compression is reported. Electrical transport measurements show strong evidence of superconductivity in InP3 with the highest critical temperature (Tc) of 9.5 K at 45.1 GPa. Raman and X‐ray diffraction (XRD) measurements indicate that the interlayer interactions are dramatically modulated under compression, along with the deformation of local In–P bipyramid structure and reduction of the interlayer distances, which eventually results in the formation of In–P bonds between neighboring In–P bipyramids and a Rm to Cmcm structural transition. First‐principles density functional theory (DFT) calculations reveal that pressure enhances the interlayer interactions, which increases the density of states (DOS) near the Fermi surface (N(EF)) and strengthens the electron–phonon coupling. Consequently, this favors the occurrence of superconductivity in compressed InP3. This study not only introduces a new superconductivity phase with enhanced electron–phonon coupling in binary phosphides, but also provides a platform for exploring the pressure effect on interlayer interactions in material systems with corrugated layered structure.

Strain-tunable electronic and optical absorption in the MXenes nanolayers: A DFT approach

Computational simulations using density functional theory (DFT) were performed to show that biaxial strain engineering within the range of −8% to +8% is an effective method for modifying the fundamental properties of two-dimensional (2D) transition metal carbides (MXenes). In this work, we computationally explored the effect of both compressive (0 to −8%) and tensile (0 to +8%) strain on the structural, electronic, and optical properties of M2CO2 MXenes (M = Ti, Zr, Sc and Hf) nanolayers. When compressive strains are applied, the charge transfer between layers increases because of decreased interlayer coupling. Conversely, tensile strains result in the opposite behavior. The strain-tunable band gap effect in Mo2CO2 nanolayers is revealed by investigating the valence band maximum (VBM) and conduction band minimum (CBM) in the band structure under biaxial strain. It is observed that the indirect-to-direct band gap transition occurs when the tensile strain is applied to Sc2CO2 and Ti2CO2 nanolayers. In most samples, the energy gap increases with an increase in tensile strain and decreases with an increase in compressive strain. The optical absorption coefficient indicates considerable absorption in the visible to ultraviolet (UV) region. Additionally, the absorption can be influenced by biaxial strains. In particular, under compressive strains (−8%) and Z-polarized light, the UV absorption peak in Hf2CO2, Ti2CO2, and Zr2CO2 reaches 68 %, 78 %, and 113 % respectively. The results indicate that these M2CO2 MXenes nanolayers will have significant potential for applications in tunable optoelectronic devices.

Terahertz Meta-Mirror with Scalable Reflective Passband by Decoupling of Cascaded Metasurfaces

Electromagnetic metasurfaces have been playing exotic roles in the construction of ultracompact and versatile metadevices for wave–matter interactions. So far, multiple metasurfaces cascaded with intercouplings have been intensively investigated for extraordinary wavefront control and broadband spectral regulations. However, most cases face high structural complexity and little attention is paid to cascaded metasurfaces without interlayer couplings. In this paper, we demonstrate one type of terahertz Bragg mirror with ideally high reflectivity and ultra-broad bandwidth by simply resorting to decoupled metasurfaces. Cascaded metasurfaces with decoupled mode control prove practically straightforward for analytical design and easy to fabricate for engineering purpose in our scheme. Essentially, by flexibly tuning the decoupled metasurface mode, the middle Fabry–Perot mode that behaves like a defect mode inside the reflective passband can be eliminated for substantial band expanding. Fundamental analyses and rigorous calculations are performed to confirm the feasibility of our metasurface-based THz Bragg mirror with scalable bandgap. In comparison, our meta-mirror provides superior spectral performance of a larger bandgap and higher in-band reflectivity over that composed by ten layers of alternate dielectrics (Rogers 3003 and 3005). Finally, our analytical methodology and numerical results provide a promising way for the rapid design and fabrication of a Bragg mirror in the optical regime.

The interlayer twist effectively regulates interlayer excitons in InSe/Sb van der Waals heterostructure

The interlayer twist angle endows a new degree of freedom to manipulate the spatially separated interlayer excitons in van der Waals (vdWs) heterostructures. Herein, we find that the band-edge Γ-Γ interlayer excitation directly forms interlayer exciton in InSe/Sb heterostructure, different from that of transition metal dichalcogenides (TMDs) heterostructures in two-step processes by intralayer excitation and transfer. By tuning the interlayer coupling and breathing vibrational modes associated with the Γ-Γ photoexcitation, the interlayer twist can significantly adjust the excitation peak position and lifetime of recombination. The interlayer excitation peak in InSe/Sb heterostructure can shift ~400 meV, and the interlayer exciton lifetime varies in hundreds of nanoseconds as a periodic function of the twist angle (0°–60°). This work enriches the understanding of interlayer exciton formation and facilitates the artificial excitonic engineering of vdWs heterostructures.

Hybrid-order Weyl semimetal and its acoustic realizations

Abstract Hybrid-order topological insulators combine first- and higher-order topological properties and host topological boundary states with codimension one and more than one in different bandgaps. A Weyl semimetal (WSM) can possess two types of Weyl points: one class of Weyl points terminates the Fermi arc surface states, while another class of Weyl points not only launch Fermi arc surface states but also hinge arc states, exhibiting the hybrid-order topology. Here, we propose a hybrid-order WSM by stacking two-dimensional rhomboid lattices based on chiral nearest-neighbor and double-helix next-nearest interlayer couplings. The first type of Weyl point that only truncates the Fermi arc surface states exists at the crossing of any two-fold degeneracy of two adjacent bands, and the second type of Weyl point that connects the hinge arc states only appears at the crossing of the two middle bands. Our findings enrich the classification of topological semimetals in condensed matter physics.

Stacking-dependent Van Hove singularity shifts in three-dimensional charge density waves of kagome metals AV3Sb5 (A = K, Rb, Cs)

Vanadium-based kagomé systems AV3Sb5 (A = K, Rb, Cs) have emerged as paradigmatic examples exhibiting unconventional charge density waves (CDWs) and superconductivity linked to van Hove singularities (VHSs). Despite extensive studies, the three-dimensional (3D) nature of CDW states in these systems remains elusive. This study employs first-principles density functional theory and a tight-binding model to investigate the stacking-dependent electronic structures of 3D CDWs in AV3Sb5, emphasizing the significant role of interlayer coupling in behaviors of the VHSs associated with diverse 3D CDW orders. We develop a minimal 3D tight-binding model and present a detailed analysis of band structures and density of states for various 3D CDW stacking configurations, including those with and without a π-phase shift stacking of the inverse star of David, as well as alternating stacking of the inverse star of David and the star of David. We find that VHSs exist below the Fermi level even in 3D CDWs without π-phase shift stackings, and that these VHSs shift downward in the π-phase shift stacking CDW structure, stabilizing the 2×2×2π-shifted inverse star of David distortions in alternating vanadium layers as the ground state 3D CDW order of AV3Sb5. Our work provides the electronic origin of 3D CDW orders, paving the way for a deeper understanding of CDWs and superconductivity in AV3Sb5 kagomé metals.

Twist Angle-Dependent Phonon Hybridization in WSe2/WSe2 Homobilayer.

The emerging moiré superstructure of twisted transition metal dichalcogenides (TMDs) leads to various correlated electronic and optical properties compared to those of twisted bilayer graphene. In such a versatile architecture, phonons can also be renormalized and evolve due to atomic reconstruction, which, in turn, depends on the twist angle. However, observing this reconstruction and its relationship to phonon behavior with conventional, cost-effective imaging methods remains challenging. Here, we used noninvasive Raman spectroscopy on twisted WSe2/WSe2 (t-WSe2) homobilayers to examine the evolution of phonon modes due to interlayer coupling and atomic reconstruction. Unlike in the natural bilayer (NB), ∼0° as well as ∼60° t-WSe2 samples, the nearly degenerate A1g/E2g mode in the twisted samples (1-7°) split into a doublet in addition to the nondegenerate B2g mode, and the maximum splitting is observed around 2-3°. Our detailed theoretical calculations qualitatively capture the splitting and its dependence as a function of the twist angle and highlight the role of the moiré potential in phonon hybridization. Additionally, we found that around the 2° twist angle, the anharmonic phonon-phonon interaction is higher than the natural bilayer and decreases for larger twist angles. Interestingly, we observed anomalous Raman frequency softening and line-width increase with the decreasing temperature below 50 K, pointing to the combined effect of enhanced electron-phonon coupling and cubic anharmonic interactions in moiré superlattice.

Gauge field dynamics in multilayer Kitaev spin liquids

The Kitaev spin liquid realizes an emergent static Z2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\\mathbb{Z}}}_{2}$$\\end{document} gauge field with vison excitations coupled to Majorana fermions. We consider Kitaev models stacked on top of each other, weakly coupled by Heisenberg interaction ∝ J⊥. This inter-layer coupling breaks the integrability of the model and makes the gauge fields dynamic. Conservation laws and topology keep single visons immobile. However, an inter-layer vison pairs can hop with a hopping amplitude linear in J⊥ confined to the layer, but their motion is strongly influenced by the type of stacking. For AA stacking, an interlayer pair has a two-dimensional motion but for AB or ABC stacking, sheet conservation laws restrict its motion to a one-dimensional channel within the plane. For all stacking types, an intra-layer vison-pair is constrained to move out-of-plane only. Depending on the anisotropy of the Kitaev couplings Kx, Ky, Kz, the intra-layer vison pairs can display either coherent tunnelling or purely incoherent hopping. When a magnetic field opens a gap for Majorana fermions, there exist two types of intra-layer vison pairs - a bosonic and a fermionic one. Only the bosonic pair obtains a hopping rate linear in J⊥. We use our results to identify the leading instabilities of the spin liquid phase induced by the inter-layer coupling.

Room-Temperature CrI3 Magnets through Lithiation.

The pursuit of two-dimensional (2D) magnetism is promising for energy-efficient electronic devices, including magnetoelectric random access memory and radio frequency/microwave magnonics, and it is gaining fundamental insights into quantum sensing technology. The key challenge resides in overseeing magnetic exchange interactions through a precise chemical reduction process, wherein manipulation of the arrangement of atoms and electrons is essential for achieving room-temperature 2D magnetism tailoring in a manner compatible with device architectures. Here, we report an electrochemically crafted CrI3 layered magnet─a van der Waals material─with precisely tailored lithiation and delithiation degrees. The crystalline and packing structure within the intralayer are preserved during the lithium intercalation within the interlayer, owing to weak interlayer coupling. Intrinsic ferromagnetism featuring a Curie temperature reaching 420 K has been unequivocally demonstrated, showcasing a coercivity of 1120 Oe at room temperature. The degree of lithiation through the reduction from Cr3+ to Cr2+ plays a crucial role in determining a 28.5% change in magnetization and a 0.29 eV shift in the bandgap. Room temperature ferromagnetism and magnetoelectricity are critical for noncontact, specifically photon-driven, dynamic magnetism control of 2D magnet-based magnonics devices.

Mo4/3B2T2/Co3O4 vdW heterostructure as saturable absorber for ultrafast pulse generation

VdW heterostructure have garnered significant interest in ultrafast laser generation because of their attractive saturable absorption properties, holding promise for applications in optics, medicine, and optoelectronics. In this study, the saturable absorption of Mo4/3B2T2/Co3O4 vdW is investigated for the first time. Mo4/3B2T2/Co3O4 vdW SA is successfully applied to passively mode-locked Er-doped fiber lasers. Due to the excellent saturable absorption properties of Mo4/3B2T2/Co3O4 vdW SA, stable mode-locked fiber lasers can be realized in the same cavity, including fundamentally conventional soliton, bound soliton, and harmonic soliton. Among them, the conventional soliton operates at a repetition rate of 11.16 MHz with a high SNR of 56.26 dB. Bound soliton is observed with a soliton pulse separation of 5.26 ps. Furthermore, 3rd-, 5th-, 8th-, 10th-, 12th-, 15th-, and 17th-order harmonic solitons are observed, corresponding to repetition rates of 33.48 MHz, 55.8 MHz, 89.28 MHz, 111.6 MHz, 133.92 MHz, 167.4 MHz and 189.72 MHz, respectively. For vdW heterostructure, the saturable absorption properties are strongly modulated by the interlayer coupling, which may be introduced by the Fermi level recombination and photogenerated carrier migration between the heterostructure. We established a model to understand the saturable absorption properties of the Mo4/3B2T2/Co3O4, which suggests the enhancements of the saturable absorption are attributed to the carrier migration between Mo4/3B2T2 and Co3O4. The results indicate that Mo4/3B2T2/Co3O4 vdW heterostructure can be used as an excellent nonlinear optical material, which can be used as SA in ultrafast pulse generation.

Synchronizability of multi-layer small-world dynamical networks

This paper investigates the synchronizability of multi-layer small-world dynamical networks and discusses the significant factors affecting the synchronizability. First, we introduce the network model of multi-layer small-world dynamical networks with one-to-one connections in the inter-layer connections and each layer has the same topology. Second, we consider the topological parameters including adding probability, intra-layer coupling strength, inter-layer coupling strength, number of nodes per layer, initial node degree, and number of network layers which will influence the network’s synchronizability. Third, we adopt the master stability function method and numerical simulations to analyze the synchronizability of the network. We also examine how the topological parameters influence the synchronizability of multi-layer small-world dynamical networks and the relationships among these parameters. Finally, synchronization control experiments are conducted to verify our results. As a result, we find that only increasing the number of nodes per layer will weaken the synchronizability of multi-layer small-world dynamical networks, while increasing other topological parameters will enhance the synchronizability. The current findings enable us to gain a deeper understanding of the synchronization behavior and characteristics of multi-layer small-world dynamical networks.

The Rise of Xene Hybrids.

Xenes, mono-elemental atomic sheets, exhibit Dirac/Dirac-like quantum behavior. When interfaced with other 2D materials such as boron nitride, transition metal dichalcogenides, and metal carbides/nitrides/carbonitrides, it enables them with unique physicochemical properties, including structural stability, desirable bandgap, efficient charge carrier injection, flexibility/breaking stress, thermal conductivity, chemical reactivity, catalytic efficiency, molecular adsorption, and wettability. For example, BN acts as an anti-oxidative shield, MoS2 injects electrons upon laser excitation, and MXene provides mechanical flexibility. Beyond precise compositional modulations, stacking sequences, and inter-layer coupling controlled by parameters, achieving scalability and reproducibility in hybridization is crucial for implementing these quantum materials in consumer applications. However, realizing the full potential of these hybrid materials faces challenges such as air gaps, uneven interfaces, and the formation of defects and functional groups. Advanced synthesis techniques, a deep understanding of quantum behaviors, precise control over interfacial interactions, and awareness of cross-correlations among these factors are essential. Xene-based hybrids show immense promise for groundbreaking applications in quantum computing, flexible electronics, energy storage, and catalysis. In this timely perspective, recent discoveries of novel Xenes and their hybrids are highlighted, emphasizing correlations among synthetic parameters, structure, properties, and applications. It is anticipated that these insights will revolutionize diverse industries and technologies.

Constructing Slip Stacking Diversity in Van der Waals Homobilayers.

The van der Waals (vdW) interface provides two important degrees of freedom-twist and slip-to tune interlayer structures and inspire unique physics. However, constructing diversified high-quality slip stackings (i.e., lattice orientations between layers are parallel with only interlayer sliding) is more challenging than twisted stackings due to angstrom-scale structural discrepancies between different slip stackings, sparsity of thermodynamically stable candidates and insufficient mechanism understanding. Here, using transition metal dichalcogenide (TMD) homobilayers as a model system, this work theoretically elucidates that vdW materials with low lattice symmetry and weak interlayer coupling allow the creation of multifarious thermodynamically advantageous slip stackings, and experimentally achieves13 and 9 slip stackings in 1T″-ReS2 and 1T″-ReSe2 bilayers via direct growth, which are systematically revealed by atomic-resolution scanning transmission electron microscopy (STEM), angle-resolved polarization Raman spectroscopy, and second harmonic generation (SHG) measurements. This work also develops modulation strategies to switch the stacking via grain boundaries (GBs) and to expand the slip stacking library from thermodynamic to kinetically favored structures via in situ thermal treatment. Finally, density functional theory (DFT) calculations suggest a prominent dependence of the pressure-induced electronic band structure transition on stacking configurations. These studies unveil a unique vdW epitaxy and offer a viable means for manipulating interlayer atomic registries.

Thickness-modulated electronic band structures and exciton behavior of non-van-der-waals 2D Bi2O2Se films

Bi2O2Se, as a non-van-der-waals (non-vdW) interlayer coupling two-dimensional material, its electronic band structures and exciton behavior still merit further in-depth studies, especially in the consideration of thickness tuning degrees of freedom. Here, we reveal the broadband excitonic performance and critical point properties of Bi2O2Se films with different thicknesses (3.54–16.33 nm). Five critical points are determined and assigned to specific optical transitions. Moreover, we observe that electronic bandstructures in the Γ valley are stable with variable thicknesses, while the deeper electron levels received more pronounced thickness modulation. And we first report four excitons in wide spectral range (1.24–6.20 eV) through absorption coefficient fitting. Significantly, due to the strong localization of electrons and holes induced by the intralayer built-in electric field, the exciton binding energy (Eb) value of 3.54 nm-Bi2O2Se (234 meV at Γ position) is apparently larger than typical multi-layer TMDCs, which offering unprecedented opportunities in applications in optoelectronic devices. Furthermore, Eb of two excitons at low energy region (Eb1, Eb2) red-shift with increasing thickness, while Eb of higher-energy excitons (Eb3, Eb4) blue-shift, owing to the dispersion characteristic of the effect dielectric screening effects. Our results are vital to wide-ranging applications of Bi2O2Se from fundamental science to optoelectronic devices.

Direct synthesis of controllable ultrathin heteroatoms-intercalated 2D layered materials

Two-dimensional (2D) layered materials have been studied in depth during the past two decades due to their unique structure and properties. Transition metal (TM) intercalation of layered materials have been proven as an effective way to introduce new physical properties, such as tunable 2D magnetism, but the direct growth of atomically thin heteroatoms-intercalated layered materials remains untapped. Herein, we directly synthesize various ultrathin heteroatoms-intercalated 2D layered materials (UHI-2DMs) through flux-assisted growth (FAG) approach. Eight UHI-2DMs (V1/3NbS2, Cr1/3NbS2, Mn1/3NbS2, Fe1/3NbS2, Co1/3NbS2, Co1/3NbSe2, Fe1/3TaS2, Fe1/4TaS2) were successfully synthesized. Their thickness can be reduced to the thinnest limit (bilayer 2D material with monolayer intercalated TM), and magnetic ordering can be induced in the synthesized structures. Interestingly, due to the possible anisotropy-stabilized long-range ferromagnetism in Fe1/3TaS2 with weak interlayer coupling, the layer-independent magnetic ordering temperature of Fe1/3TaS2 was revealed by magneto-transport properties. This work establishes a general method for direct synthesis of heteroatom-intercalated ultrathin 2D materials with tunable chemical and physical properties.