Observing and Modeling the Wear Process of Heterogeneous Interface.

Understanding and controlling the wear process of heterogeneous interfaces between soft and hard phases is crucial for designing and fabricating materials, such as improving the wear resistance of particle reinforced metal matrix composites and the accuracy and efficiency of chemical mechanical polishing. However, the wear process can be hardly observed, as interfaces are buried under the surface. Here, we proposed a nanowear test method by combining focused ion beam cutting to expose interfaces, atomic force microscopy to rub against interfaces, and scanning electron microscope to characterize the interface damage. Using this method, three typical wear forms had been observed in Al/SiC composite, i.e., merely matrix wear, particle fracture, and particle pullout. A theoretical model was proposed that revealed that the increasing interfacial friction would induce particle fracture or pullout, depending on the particle edge angle and tip edge angle. This work sheds light on wear control in composites and nanofabrication.

Ultralow-Friction at Cryogenic Temperature Induced by Hydrogen Correlated Quantum Effect.

Temperature is one of the governing factors affecting friction of solids. Undesired high friction state has been generally reported at cryogenic temperatures due to the prohibition of thermally activated processes, following conventional Arrhenius equation. This has brought huge difficulties to lubrication at extremely low temperatures in industry. Here, the study uncovers a hydrogen-correlated sub-Arrhenius friction behavior in hydrogenated amorphous carbon (a-C:H) film at cryogenic temperatures, and a stable ultralow-friction over a wide temperature range (103-348 K) is achieved. This is attributed to hydrogen-transfer-induced mild structural ordering transformation, confirmed by machine-learning-based molecular dynamics simulations. The anomalous sub-Arrhenius temperature dependence of structural ordering transformation rate is well-described by a quantum mechanical tunneling (QMT) modified Arrhenius model, which is correlated with quantum delocalization of hydrogen in tribochemical reactions. This work reveals a hydrogen-correlated friction mechanism overcoming the Arrhenius temperature dependence and provides a new pathway for achieving ultralow friction under cryogenic conditions.

Domino-like stacking order switching in twisted monolayer-multilayer graphene.

Atomic reconstruction has been widely observed in two-dimensional van der Waals structures with small twist angles1-7. This unusual behaviour leads to many novel phenomena, including strong electronic correlation, spontaneous ferromagnetism and topologically protected states1,5,8-14. Nevertheless, atomic reconstruction typically occurs spontaneously, exhibiting only one single stable state. Using conductive atomic force microscopy, here we show that, for small-angle twisted monolayer-multilayer graphene, there exist two metastable reconstruction states with distinct stacking orders and strain soliton structures. More importantly, we demonstrate that these two reconstruction states can be reversibly switched, and the switching can propagate spontaneously in an unusual domino-like fashion. Assisted by lattice-resolved conductive atomic force microscopy imaging and atomistic simulations, the detailed structure of the strain soliton networks has been identified and the associated propagation mechanism is attributed to the strong mechanical coupling among solitons. The fine structure of the bistable states is critical for understanding the unique properties of van der Waals structures with tiny twists, and the switching mechanism offers a viable means for manipulating their stacking states.

Fluctuation of Interfacial Electronic Properties Induces Friction Tuning under an Electric Field.

Mysteries about the origin of friction have remained for centuries. Especially, how friction is tuned by an electric field is still unclear. Present tuning mechanisms mainly focus on the atomic configurations and electrostatic force, yet the role of interfacial electronic properties is not fully understood. Here, we investigate a unique friction tuning effect induced by an electric current in a conductive atomic force microscopy experiment and uncover two main tuning mechanisms of friction by the fluctuation of electronic properties during sliding: (1) electric-field-induced electron density redistribution and (2) current-induced electron transfer. We put forward an electronic level friction model unraveling the relationship between the friction tuning and the electronic property fluctuation (EPF) under electric field/current, which is applicable to tribosystems ranging from conductors to semiconductors and insulators, including two-dimensional material interfaces. This model provides theoretical guidance for tribosystem design and friction control, proposing a new perspective in understanding the origin of friction.

Unraveling the Friction Evolution Mechanism of Diamond-Like Carbon Film during Nanoscale Running-In Process toward Superlubricity.

Diamond-like carbon (DLC) films are capable of achieving superlubricity at sliding interfaces by a rapid running-in process. However, fundamental mechanisms governing the friction evolution during this running-in processes remain elusive especially at the nanoscale, which hinders strategic tailoring of tribosystems for minimizing friction and wear. Here, it is revealed that the running-in governing superlubricity of DLC demonstrates two sub-stages in single-asperity nanocontacts. The first stage, mechanical removal of a thin oxide layer, is described quantitatively by a stress-activated Arrhenius model. In the second stage, a large friction decrease occurs due to a structural ordering transformation, with the kinetics well described by the Johnson-Mehl-Avrami-Kolmogorov model with a modified load dependence of the activation energy. The direct observation of a graphitic-layered transfer film formation together with the measured Avrami exponent reveal the primary mechanism of the ordering transformation. The findings provide fundamental insights into friction evolution mechanisms, and design criteria for superlubricity.

Abnormal conductivity in low-angle twisted bilayer graphene.

Controlling the interlayer twist angle offers a powerful means for tuning the electronic properties of two-dimensional (2D) van der Waals materials. Typically, the electrical conductivity would increase monotonically with decreasing twist angle owing to the enhanced coupling between adjacent layers. Here, we report a nonmonotonic angle-dependent vertical conductivity across the interface of bilayer graphene with low twist angles. More specifically, the vertical conductivity enhances gradually with decreasing twist angle up to a crossover angle at θc ≈ 5°, and then it drops notably upon further decrease in the twist angle. Revealed by density functional theory calculations and scanning tunneling microscopy, the abnormal behavior is attributed to the unusual reduction in average carrier density originating from local atomic reconstruction. The impact of atomic reconstruction on vertical conductivity is unique for low-angle twisted 2D van der Waals materials and provides a strategy for designing and optimizing their electronic performance.

Surface Physical and Chemical Modification of Pure Iron by Using Atmospheric Pressure Plasma Treatment.

To investigate the mechanism of surface modification of pure iron by atmospheric pressure plasma treatment (APPT), the surface wettability of pure iron was characterized by using a contact-angle measuring instrument, and the mechanical properties of pure iron were measured by a tensile testing machine and nanoindentation instrument. Molecular dynamics simulations were used to explain the modification mechanism of the surface wettability and the mechanical behavior of pure iron by APPT. The experimental results show that pure iron treated by APPT is superhydrophilic, with reduced tensile strength and surface hardness. This result agrees with the molecular dynamics simulation, which shows that the pure iron material hydrophilicity improved after APPT. The behavior was attributed to the formation of hydrogen bonds on the surface of the pure iron after APPT. The surface binding energy of the pure iron material increased between the water molecule and the residual N atom that was induced by APPT. The N atom that was introduced by the APPT led to Fe bond fracture, and the N atom reduced the Fe bond strength, which resulted in a reduction of material yield strength and microhardness.

Achieving a superlubricating ohmic sliding electrical contact via a 2D heterointerface: a computational investigation.

Simultaneously achieving low friction and fine electrical conductance of sliding electrical contacts is a crucial factor but a great challenge for designing high-performance microscale and nanoscale functional devices. Through atomistic simulations, we propose an effective design strategy to obtain both low friction and high conductivity in sliding electrical contacts. By constructing graphene(Gr)/MoS2 two-dimensional (2D) heterojunctions between sliding Cu surfaces, superlubricity can be achieved with a remarkably lowered sliding energy barrier as compared to that of the homogeneous MoS2 lubricated Cu contact. Moreover, by introducing vacancy defects into MoS2 and substituting Cu with active metal Ti, the Schottky and tunneling barriers can be substantially suppressed without losing the superlubricious properties of the tribointerface. Consequently, a high conductivity ohmic contact with low sliding friction could be realized in our proposed Ti-MoS1.5-Gr-Ti system, which provides a potential strategy for tackling the well-known dilemma for high performance sliding electrical contacts.

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.

Modeling Atomic-Scale Electrical Contact Quality Across Two-Dimensional Interfaces.

Contacting interfaces with physical isolation and weak interactions usually act as barriers for electrical conduction. The electrical contact conductance across interfaces has long been correlated with the true contact area or the "contact quantity". Much of the physical understanding of the interfacial electrical contact quality was primarily based on Landauer's theory or Richardson formulation. However, a quantitative model directly connecting contact conductance to interfacial atomistic structures still remains absent. Here, we measure the atomic-scale local electrical contact conductance instead of local electronic surface states in graphene/Ru(0001) superstructure, via atomically resolved conductive atomic force microscopy. By defining the "quality" of individual atom-atom contact as the carrier tunneling probability along the interatomic electron transport pathways, we establish a relationship between the atomic-scale contact quality and local interfacial atomistic structure. This real-space model unravels the atomic-level spatial modulation of contact conductance, and the twist angle-dependent interlayer conductance between misoriented graphene layers.

Enhancing charge transfer with foreign molecules through femtosecond laser induced MoS2 defect sites for photoluminescence control and SERS enhancement.

Defect/active site control is crucial for tuning the chemical, optical, and electronic properties of MoS2, which can adjust the performance of MoS2 in application areas such as electronics, optics, catalysis, and molecular sensing. This study presents an effective method of inducing defect/active sites, including micro/nanofractured structures and S atomic vacancies, on monolayer MoS2 flakes by using femtosecond laser pulses, through which physical-chemical adsorption and charge transfer between foreign molecules (O2 or R6G molecules) and MoS2 are enhanced. The enhanced charge transfer between foreign molecules (O2 or R6G) and femtosecond laser-treated MoS2 can enhance the electronic doping effect between them, hence resulting in a photoluminescence photon energy shift (reaching 0.05 eV) of MoS2 and Raman enhancement (reaching 6.4 times) on MoS2 flakes for R6G molecule detection. Finally, photoluminescence control and micropatterns on MoS2 and surface-enhanced-Raman-scattering (SERS) enhancement of MoS2 for organic molecule detection are achieved. The proposed method, which can control the photoluminescence properties and arbitrary micropatterns on MoS2 and enhance its chemicobiological sensing performance for organic/biological molecules, has advantages of simplicity, maskless processing, strong controllability, high precision, and high flexibility, highlighting the superior ability of femtosecond laser pulses to achieve the property control and functionalization of two-dimensional materials.

Tuning Local Electrical Conductivity via Fine Atomic Scale Structures of Two-Dimensional Interfaces.

Two-dimensional (2D) materials have seen a broad range of applications in electronic and optoelectronic applications; however, full realization of this potential hitherto largely hinges on the quality and performance of the electrical contacts formed between 2D materials and their surrounding metals/semiconductors. Despite the progress in revealing the charge injecting mechanisms and enhancing electrical conductance using various interfacial treatments, how the microstructure of contact interfaces affects local electrical conductivity is still very limited. Here, using conductive atomic force microscopy (c-AFM), for the first time, we directly confirm the conjecture that the electrical conductivity of physisorbed 2D material-metal/semiconductor interfaces is determined by the local electronic charge transfer. Using lattice-resolved conductivity mapping and first-principles calculations, we demonstrate that the electronic charge transfer, thereby electrical conductivity, can be fine-tuned by the topological defects of 2D materials and the atomic stacking with respect to the substrate. Our finding provides a novel route to engineer the electrical contact properties by exploiting fine atomic interactions; in the meantime, it also suggests a convenient and nondestructive means of probing subtle interactions along 2D heterogeneous interfaces.

Interlayer Friction and Superlubricity in Single-Crystalline Contact Enabled by Two-Dimensional Flake-Wrapped Atomic Force Microscope Tips.

Interlayer friction between the atomic planes of 2D materials and heterostructures is a promising probe of the physics in their interlayer couplings and superlubricity. However, it is still challenging to measure the interlayer friction between well-defined 2D layers. We propose an approach of thermally assisted mechanical exfoliation and transfer to fabricate various 2D flake-wrapped atomic force microscopy (AFM) tips and to directly measure the interlayer friction between 2D flakes in single-crystalline contact. First, superlubricity between different 2D flakes and layered bulk materials is achieved with a friction coefficient as low as 10-4. The rotation angle dependence of superlubricity is observed for friction between graphite layers, whereas it is not observed between graphite and h-BN because of the incommensurate contact of the mismatched lattices. Second, the interlayer lateral force map between ReS2 layers is measured with atomic resolution, showing hexagonal patterns, as further verified by theoretical simulations. The tribological system constructed here offers an experimental platform to study interlayer couplings and friction between 2D flakes and layered bulk materials.