Strong Interlayer Research Articles

First-Principles Study of the Schottky Contact, Tunneling Probability, and Optical Properties of MX/TiB4 Heterojunctions (M = Ge, Sn; X = S, Se, Te): Strain Engineering Tunability.

Designing two-dimensional (2D) heterojunctions with rapid response and minimal energy consumption holds immense significance for the advancement of the next generation of electronic devices. Here, we construct a series of Schottky heterojunctions based on TiB4 monolayer and group-IV monochalcogenide monolayers MX (M = Ge, Sn; X = S, Se, Te). Using first-principles calculations, we investigate the structural stability, Schottky contact barrier, tunneling probability, and optical properties of MX/TiB4 heterojunctions. The calculated binding energies reveal that X-type MX/TiB4 heterojunctions exhibit more stable structures than M- and C-type stacking modes. Schottky barrier heights (SBHs) indicate that X-type GeSe/TiB4 and GeTe/TiB4 form n-type Schottky contacts with SBHs of 0.497 and 0.132 eV, respectively, while SnS/TiB4 and SnSe/TiB4 form p-type Schottky contacts with SBHs of 0.557 and 0.418 eV, respectively. Moreover, X-type MX/TiB4 heterojunctions exhibit high susceptibility to interlayer electron tunneling due to their large tunneling probability and strong interlayer interaction. Meanwhile, enhanced optical absorption capacity in MX/TiB4 heterojunctions is also observed compared with individual TiB4 and MX monolayers. By applying in-plane biaxial strain, the transformation of MX/TiB4 heterojunctions from a Schottky contact to an Ohmic contact can also be realized. Our findings could offer valuable candidate materials and guidance for the design of the next generation of nanodevices with high electronic and optical performances.

Excitons at the interface of 2D TMDs and molecular semiconductors.

Van der Waals heterostructures (vdWHs) of vertically stacked two-dimensional (2D) atomic crystals have been used to elicit intriguing phenomena stemming from strong electronic correlations, magnetic textures, and interlayer excitons spawned at the heterointerface. However, vdWHs comprised of heterointerfaces between these 2D atomic crystal lattices and molecular assemblies are emerging as equally intriguing platforms supporting properties to be harnessed for photovoltaic energy conversion, photodetection, spin-selective charge injection, and quantum emission. In this perspective, we summarize recent research examining exciton dynamics in heterostructures between semiconducting 2D transition metal dichalcogenides and molecular organic semiconductors. We discuss methods for assembly of these heterostructures, the nature of interlayer or charge-transfer excitons at transition-metal dichalcogenide (TMD)-molecule interfaces, explicit exciton transfer between organics and TMDs, and other interfacial phenomena driven by the merger of these two material classes. We also suggest key new research directions extending the remit of these 2D atomic-molecular lattice heterointerfaces into the domains of condensed matter physics, quantum sensing, and energy conversion.

An integrated, multi-functional intrinsic responsive foldable protective layer for space station solar panels

The functionalized foldable protective layer proficiently alleviates the potential detriment endured by space station solar panels due to prolonged and uninterrupted exposure to the environment. Soft actuators demonstrate significant value in foldable protective layers due to their intrinsic response characteristics and programmability. However, current soft actuators still struggle to meet the requirements of work stability and scene applicability in the space environment. A PMT (Polydimethylsiloxane (PDMS)/Multi-walled carbon nanotubes (MWCNTs)-Thermoplastic polyimides (TPI)) soft actuator was proposed to address this issue in this paper. The PMT soft actuators exhibit strong interlayer interfacial adhesion, stable physical and chemical performance, and excellent mechanical performance. Notably, the PMT soft actuators can sense thermal, electric fields, infrared light, and mechanical force simultaneously with only one active layer. Furthermore, analytical models were calibrated to provide predictions, and the thermal and photoelectric actuation processes of PMT soft actuators with different structures and application scenes were predicted accurately. The experimental results validated the application value of PMT actuators as foldable protective layers for space station solar panels. The preparation, testing, application, and model construction of the PMT system provide new research ideas and development opportunities for the practical application of functional polymers in intelligent sensing and actuation systems.

Neuromorphic Computing in Synthetic Antiferromagnets by Spin‐Orbit Torque Induced Magnetic‐Field‐Free Magnetization Switching

AbstractSynthetic antiferromagnet (SAF) with high thermal stability, ultra‐fast spin dynamics, and highly efficient spin‐orbit torque switching has great application potential in neuromorphic computing hardware. However, two challenges, the weakening of Hall signal in the remanent state and the need for a large auxiliary magnetic field for perpendicular magnetization switching, greatly limit the advantages of SAF in neuromorphic computing. In this work, both the enhanced anomalous Hall resistance and magnetic‐field‐free perpendicular magnetization switching are achieved by using oblique sputtering to fabricate the Pt/CoPt/Ru/CoTb SAF with strong interlayer exchange coupling and magnetic moment compensation. The fabricated SAF as synapse shows nearly linear, nonvolatile multistate plasticity, and as neuron exhibits a nonlinear sigmoid activation function, which are used to construct a fully connected neural network with a remarkable 97.0–98.1% recognition rate for the handwritten digits. Additionally, SAF serving as spike‐timing‐dependent plasticity synapse is used to construct an adaptive, unsupervised learning spiking neural network, and achieve an 87.0% accuracy in handwritten digit recognition. The findings exhibit the promise of SAFs as specialized hardware for high‐performance neuromorphic computing, offering high recognition rates and low power consumption.

Ligand‐Assisted Growth of 2D Perovskite Single Crystal for Highly Sensitive X‐Ray Detectors

AbstractThe emerging 2D layered perovskites have promising optoelectronic properties, good intrinsic stability and reduced ion migration, making them effective for detecting X‐ray radiation. However, their application is constrained by poor out‐of‐plane carrier transport. In this study, inch‐sized high‐quality CsPb2Br5 layered single crystals (SCs) are developed using an organic ligand‐assisted solution process. By modifying the surface energy, the anisotropy of crystal growth is conquered, resulting in CsPb2Br5 SCs with sufficient thickness for X‐ray detection. Importantly, this modification significantly enhanced the crystal quality as the grown CsPb2Br5 SCs exhibited longer photoluminescence lifetime and smaller trap density. Notably, the CsPb2Br5 SCs demonstrate unprecedented out‐of‐plane carrier transport, achieving a high carrier mobility‐lifetime product of 2.53 × 10−2 cm2V−1. This can be attributed to the small interlayer distance and the strong interlayer force of Cs─Br bonding. Furthermore, CsPb2Br5 SCs possess other intriguing attributes for X‐ray detection, including high bulk resistivity and outstanding thermal stability. These advantageous properties enable high‐performance vertical‐structure X‐ray detection with a superior sensitivity of up to 8865.6 µC Gyair−1cm−2 and a low detectable dose rate of 12.7 nGyairs−1. Additionally, CsPb2Br5 SCs exhibit high spatial resolution in X‐ray imaging and exceptional thermal stability, making them promising candidates for nondestructive determination.

Electric-field tunable Type-I to Type-II band alignment transition in MoSe2/WS2 heterobilayers

Semiconductor heterojunctions are ubiquitous components of modern electronics. Their properties depend crucially on the band alignment at the interface, which may exhibit straddling gap (type-I), staggered gap (type-II) or broken gap (type-III). The distinct characteristics and applications associated with each alignment make it highly desirable to switch between them within a single material. Here we demonstrate an electrically tunable transition between type-I and type-II band alignments in MoSe2/WS2 heterobilayers by investigating their luminescence and photocurrent characteristics. In their intrinsic state, these heterobilayers exhibit a type-I band alignment, resulting in the dominant intralayer exciton luminescence from MoSe2. However, the application of a strong interlayer electric field induces a transition to a type-II band alignment, leading to pronounced interlayer exciton luminescence. Furthermore, the formation of the interlayer exciton state traps free carriers at the interface, leading to the suppression of interlayer photocurrent and highly nonlinear photocurrent-voltage characteristics. This breakthrough in electrical band alignment control, interlayer exciton manipulation, and carrier trapping heralds a new era of versatile optical and (opto)electronic devices composed of van der Waals heterostructures.

Magnetization switching driven by spin current in a T-type ferromagnetic trilayer

The T-type CoFeB/spacer/CoFeB structure is a promising candidate for the development of perpendicular spin–orbit torque (SOT) magnetic random-access memory and other SOT devices. It consists of an in-plane magnetized layer, a perpendicularly magnetized layer, and a non-magnetic metal spacer that induces interlayer exchange coupling. By engineering the W spacer, this system achieves field-free SOT switching with a nearly 100% switching ratio. Furthermore, it realizes a high exchange coupling field of 255 Oe using a relatively thinner spacer thickness, enhancing the reliability and energy efficiency of SOT switching. Measurement of current switching probability suggests that this perpendicular magnetic anisotropy system may enable the implementation of probability-adjustable true random number generators in future applications. The T-type structures with strong interlayer coupling exhibit great potential for spintronic device applications.

Self-condensation-assisted chemical vapour deposition growth of atomically two-dimensional MOF single-crystals

Two-dimensional metal-organic frameworks (MOFs) have a wide variety of applications in molecular separation and other emerging technologies, including atomically thin electronics. However, due to the inherent fragility and strong interlayer interactions, high-quality MOF crystals of atomic thickness, especially isolated MOF crystal monolayers, have not been easy to prepare. Here, we report the self-condensation-assisted chemical vapour deposition growth of atomically thin MOF single-crystals, yielding monolayer single-crystals of poly[Fe(benzimidazole)2] up to 62 μm in grain sizes. By using transmission electron microscopy and high-resolution atomic force microscopy, high crystallinity and atomic-scale single-crystal structure are verified in the atomically MOF flakes. Moreover, integrating such MOFs with MoS2 to construct ultrathin van der Waals heterostructures is achieved by direct growth of atomically MOF single-crystals onto monolayer MoS2, and enables a highly selective ammonia sensing. These demonstrations signify the great potential of the method in facilitating the development of the fabrication and application of atomically thin MOF crystals.

Study on the tribological properties of MoB/Cu laminated composite materials fabricated by hot-pressing process

This work presents a novel method for fabricating MoB/Cu laminated composite materials which are distinguished by their strong interlayer bonding and unique microstructure. MoB ceramic layer can obviously improve the friction and wear properties of Cu matrix composites. The tribological properties on cross-sections of MoB/Cu laminated composite are studied with GCr15 (a typical high-carbon chromium bearing steel) ball as counterpart under dry friction conditions. When the friction angle is less than 30°, the wear rate (∼0.4974 × 10-4mm3/(N·m)) is reduced substantially by about 85 % compared to pure copper. The coefficient of friction of the composite ranges from 0.182 to 0.223 at a friction angle from 0° to 90°. A dense lubricating oxide film is formed during the friction process, effectively slowing down the adhesive wear and increasing the friction and wear resistance. After XPS (X-ray photoelectron spectroscopy) analysis, the main components of the lubricating film generated during the friction process are MoO3, B2O3, Al2O3, CuO, and Fe2O3.

Engineering van der Waals Contacts by Interlayer Dipoles.

Tuning the interfacial Schottky barrier with van der Waals (vdW) contacts is an important solution for two-dimensional (2D) electronics. Here we report that the interlayer dipoles of 2D vdW superlattices (vdWSLs) can be used to engineer vdW contacts to 2D semiconductors. A bipolar WSe2 with Ba6Ta11S28 (BTS) vdW contact was employed to exhibit this strategy. Strong interlayer dipoles can be formed due to charge transfer between the Ba3TaS5 and TaS2 layers. Mechanical exfoliation breaks the superlattice and produces two distinguished surfaces with TaS2 and Ba3TaS5 terminations. The surfaces thus have opposite surface dipoles and consequently different work functions. Therefore, all the devices fall into two categories in accordance with the rectifying direction, which were verified by electrical measurements and scanning photocurrent microscopy. The growing vdWSL family along with the addition surface dipoles enables prospective vdW contact designs and have practical application in nanoelectronics and nano optoelectronics.

Enhanced interlayer Dzyaloshinskii–Moriya interaction and field-free switching in magnetic trilayers with orthogonal magnetization

The indirect interlayer exchange coupling (IEC) between two magnetic layers holds significant importance in the field of spintronics and has been widely used in the construction of synthetic antiferromagnets. Recently, the interlayer Dzyaloshinskii–Moriya interaction (DMI), antisymmetric counterpart of IEC, has been discovered in magnetic trilayers with a heavy-metal spacer. In this study, we present an investigation on antisymmetric and symmetric counterparts of IEC in D022-Mn3Ga/Pt/Co trilayers with orthogonal magnetization. Due to the strong interlayer DMI across the entire multilayer, the symmetry of magnetic reversal process was broken, leading to an enhanced chiral exchange-bias field of 42.7 Oe in the Co layer. In addition, field-free spin–orbit torque (SOT) switching of D022-Mn3Ga layer has been realized in Hall bar devices. In-plane field dependence analysis of the SOT switching behavior reveals that the symmetric counterpart of IEC exhibits antiferromagnetic characteristics within the spacer thickness range of 2 nm ≤ tPt ≤5 nm. Moreover, the magnitude of both antisymmetric and symmetric counterparts of IEC exhibits an exponential decreasing trend with increasing tPt. These findings hold significant implications for the design and manipulation of three-dimensional chiral spin textures in the future spintronic devices.

Emergent quasi-two-dimensional ferromagnetic state with perpendicular magnetic anisotropy at La0.7Sr0.3MnO3/SrCuO2 interface

Due to the strong interlayer coupling between multiple degrees of freedom, oxide heterostructures usually produce distinct interfacial phases with unexpected functionalities. Here, we report on the realization of quasi-two-dimensional ferromagnetic state in ultrathin La0.7Sr0.3MnO3 (LSMO) layer down to two unit cells (u.c.), being sandwiched by the planar infinite-layer structured SrCuO2 layers (P-SCO). We find the LSMO/P-SCO interface coupling has greatly suppressed the magnetic dead layer of LSMO, resulting in an emergent interfacial ferromagnetic phase. Thus, robust ferromagnetic order can be maintained in the 2 u.c.-thick LSMO layer (∼7.7 Å), showing a Curie temperature of ∼260 K and remarkable perpendicular magnetic anisotropy. X-ray absorption spectra reveal notable charge transfer from Mn to Cu at the interface, and thus, resulted preferential d3z2−r2 orbital occupation for interfacial Mn ions plays an important role in the inducing of perpendicular magnetic anisotropy in quasi-two-dimensional LSMO layer. Our work demonstrates a unique approach for tuning the properties of oxides via an interface engineering of oxygen coordination in perovskite/infinite-layer heterostructures.

High Performance Nacre Fibers by Engineering Interfacial Entanglement.

Biological materials exhibit fascinating mechanical properties for intricate interactions at multiple interfaces to combine superb toughness with wondrous strength and stiffness. Recently, strong interlayer entanglement has emerged to replicate the powerful dissipation of natural proteins and alleviate the conflict between strength and toughness. However, designing intricate interactions in a strong entanglement network needs to be further explored. Here, we modulate interlayer entanglement by introducing multiple interactions, including hydrogen and ionic bonding, and achieve ultrahigh mechanical performance of graphene-based nacre fibers. Two essential modulating trends are directed. One is modulating dynamic hydrogen bonding to improve the strength and toughness up to 1.58 GPa and 52 MJ/m3, simultaneously. The other is tailoring ionic coordinating bonding to raise the strength and stiffness, reaching 2.3 and 253 GPa. Modulating various interactions within robust entanglement provides an effective approach to extend performance limits of bioinspired nacre and optimize multiscale interfaces in diverse composites.

Charge-Transfer-Induced Interfacial Ferromagnetism in Ferromagnet-Free Oxide Heterostructures.

Due to the strong interlayer coupling between multiple degrees of freedom, oxide heterostructures have demonstrated exotic properties that are not shown by their bulk counterparts. One of the most interesting properties is ferromagnetism at the interface formed between "nonferromagnetic" compounds. Here we report on the interfacial ferromagnetic phase induced in the superlattices consisting of the two paramagnetic oxides CaRuO3 (CRO) and LaNiO3 (LNO). By varying the sublayer thickness in the superlattice period, we demonstrate that the ferromagnetic order has been established in both CaRuO3 and LaNiO3 sublayers, exhibiting an identical Curie temperature of ∼75 K. The X-ray absorption spectra suggest a strong charge transfer from Ru to Ni at the interface, triggering superexchange interactions between Ru/Ni ions and giving rise to the emergent ferromagnetic phase. Moreover, the X-ray linear dichroism spectra reveal the preferential occupancy of the d3z2-r2 orbital for the Ru ions and the dx2-y2 orbital for the Ni ions in the heterostructure. This leads to different magnetic anisotropy of the superlattices when they are dominated by CRO or LNO sublayers. This work clearly demonstrates a charge-transfer-induced interfacial ferromagnetic phase in the whole ferromagnet-free oxide heterostructures, offering a feasible way to tailor oxide materials for desired functionalities.

2D/0D multiscale interfacial engineering of carbon fiber composites for simultaneous achieving high mechanical and electromagnetic interference shielding properties

AbstractIn the face of escalating electromagnetic pollution, it is urgently needed to expedite the development of innovative carbon fiber reinforced polymer (CFRP) composites that not only demonstrate superior mechanical properties as well as durability but also boast exceptional electromagnetic interference shielding (EMI) performance. However, given the absence of robust interface interactions and the lack of an outstanding nanostructured conductive network, there remains a need to further elevate the overall performance of CFRP composites. Herein, a highly continuous conductive network by integrating 2D MXene and 0D Ag nanoparticles with strong interlayer interactions was constructed through point‐to‐plane conductive modes, facilitated by polydopamine (PDA). Thanks to the excellent electromagnetic wave loss and the unique multi‐dimensional structure arising from the optimizing interfacial engineering, the EMI shielding effectiveness of the modified CF‐PDA‐M‐Ag/EP composite achieved a remarkable 45.9 dB, obtaining a 99.5% enhancement compared with the neat CF/EP. The synergistic effect resulting from the multi‐dimensional structure and strong interaction can improve the interfacial shear strength (IFSS), interlaminar shear strength (ILSS) and flexure strength of the composite up to 81.9, 85.8 and 864.6 MPa, respectively, far superior to the unmodified composite materials. This research provides a dependable and convenient approach for exploiting high‐performance CFRP composites with intriguing electromagnetic interference (EMI) shielding properties.Highlights An optimizing multifunctional 2D/0D interface for carbon fiber was designed. A highly conductive network via the point‐to‐plane conductive mode. The EMI shielding effectiveness of the composite reached up to 45.9 dB.

A Cu3BHT-Graphene van der Waals Heterostructure with Strong Interlayer Coupling for Highly Efficient Photoinduced Charge Separation.

Two-dimensional van der Waals heterostructures (2D vdWhs) are of significant interest due to their intriguing physical properties critically defined by the constituent monolayers and their interlayer coupling. Synthetic access to 2D vdWhs based on chemically tunable monolayer organic 2D materials remains challenging. Herein, the fabrication of a novel organic-inorganic bilayer vdWh by combining π-conjugated 2D coordination polymer (2DCP, i.e., Cu3BHT, BHT = benzenehexathiol) with graphene is reported. Monolayer Cu3BHT with detectable µm2-scale uniformity and atomic flatness is synthesized using on-water surface chemistry. A combination of diffraction and imaging techniques enables the determination of the crystal structure of monolayer Cu3BHT with atomic precision. Leveraging the strong interlayer coupling, Cu3BHT-graphene vdWh exhibits highly efficient photoinduced interlayer charge separation with a net electron transfer efficiency of up to 34% from Cu3BHT to graphene, superior to those of reported bilayer 2D vdWhs and molecular-graphene vdWhs. This study unveils the potential for developing novel 2DCP-based vdWhs with intriguing physical properties.

Strong Sliding Ferroelectricity and Interlayer Sliding Controllable Spintronic Effect in Two-Dimensional HgI2 Layers.

Exploration of two-dimensional (2D) sliding ferroelectric (FE) materials with experimentally detectable ferroelectricity and value-added novel functionalities is highly sought for the development of 2D "slidetronics". Herein, based on first-principles calculations, we identify the synthesizable van der Waals (vdW) layered crystals HgX2 (X = Br and I) as a new class of 2D sliding ferroelectrics. Both HgBr2 and HgI2 in 2D multilayered forms adopt the preferential stacking sequence, leading to room temperature stable out-of-plane (vertical) ferroelectricity that can be reversed via the sliding of adjacent monolayers. Owing to strong interlayer coupling and interfacial charge rearrangement, 2D HgI2 layers possess strong sliding ferroelectricity up to 0.16 μC/cm2, readily detectable in experiment. Moreover, robust sliding ferroelectricity and interlayer sliding controllable Rashba spin texture of FE-HgI2 layers enable potential applications as 2D spintronic devices such that the electric control of electron spin detection can be realized at the 2D regime.

Constructing 2D Phthalocyanine Covalent Organic Framework with Enhanced Stability and Conductivity via Interlayer Hydrogen Bonding as Electrocatalyst for CO2 Reduction.

Fabricating COFs-based electrocatalysts with high stability and conductivity still remains a great challenge. Herein, 2D polyimide-linked phthalocyanine COF (denoted as NiPc-OH-COF) is constructed via solvothermal reaction between tetraanhydrides of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(II) and 2,5-diamino-1,4-benzenediol (DB) with other two analogous 2D COFs (denoted as NiPc-OMe-COF and NiPc-H-COF) synthesized for reference. In comparison with NiPc-OMe-COF and NiPc-H-COF, NiPc-OH-COF exhibits enhanced stability, particularly in strong NaOH solvent and high conductivity of 1.5×10-3Sm-1 due to the incorporation of additional strong interlayer hydrogen bonding interaction between the O-H of DB and the hydroxy "O" atom of DB in adjacent layers. This in turn endows the NiPc-OH-COF electrode with ultrahigh CO2-to-CO faradaic efficiency (almost 100%) in a wide potential range from -0.7 to -1.1V versus reversible hydrogen electrode (RHE), a large partial CO current density of -39.2mAcm-2 at -1.1V versus RHE, and high turnover number as well as turnover frequency, amounting to 45000 and 0.76S-1 at -0.80V versus RHE during 12h lasting measurement.

Dual material fused filament fabrication of composite core‐shell structures with improved impact resistance and interfacial adhesion

AbstractThe mechanical performance of parts produced by fused filament fabrication (FFF) has been limited due to the presence of voids and poor interlayer welding. Recent advancements in FFF have enabled the fabrication of void‐free objects with strong interlayer welding through the use of semicrystalline polymer shells such as high‐density polyethylene (HDPE) along with a high viscosity core polymer like acrylonitrile‐butadiene‐styrene (ABS). The zero‐shear viscosity (η0) of ABS is three orders of magnitude higher than HDPE making the ABS‐HDPE core‐shell configuration preferable. ABS holds the shape by preventing bulk flow and part bending while HDPE promotes full surface contact across the layers. Most polymers, however, are immiscible which causes a weak weld line along the core‐shell interface. Herein, maleic anhydride (MAH) is grafted to the butadiene segment of the ABS core thereby compatibilizing the interface with HDPE, improving the interfacial adhesion. Attenuated total reflectance‐Fourier transform infrared spectroscopy was employed to confirm successful grafting. Using a custom‐made die affording the core‐shell structure, the ABS‐g‐MAH is shown to improve the impact resistance by 253% and 16% compared to neat HDPE and ABS specimens, respectively. Additionally, a 10% increase compared to the unmodified ABS‐HDPE core‐shell configuration is observed.

Novel Polytype of III-VI Metal Chalcogenides Nano Crystals Realized in Epitaxially Grown InTe.

III-VI metal chalcogenides have garnered considerable research attention as a novel group of layered van der Waals materials because of their exceptional physical properties and potential technological applications. Here, the epitaxial growth and stacking sequences of InTe is reported, an essential and intriguing material from III-VI metal chalcogenides. Aberration-corrected scanning transmission electron microscopy (STEM) is utilized to directly reveal the interlayer stacking modes and atomic structure, leading to a discussion of a new polytype. Furthermore, correlations between the stacking sequences and interlayer distances are substantiated by atomic-resolution STEM analysis, which offers evidence for strong interlayer coupling of the new polytype. It is proposed that layer-by-layer deposition is responsible for the formation of the unconventional stacking order, which is supported by ab initio density functional theory calculations. The results thus establish molecular beam epitaxy as a viable approach for synthesizing novel polytypes. The experimental validation of the InTe polytype here expands the family of materials in the III-VI metal chalcogenides while suggesting the possibility of new stacking sequences for known materials in this system.