Twist angle-dependent interlayer hybridized exciton lifetimes in van der Waals heterostructures.

The interlayer twist angle has a direct effect on exciton lifetimes in van der Waals heterostructures. At small angles, the interlayer and intralayer excitons in MoSe2/WS2 heterostructures are hybridized, resulting in hybridized excitons with long lifetimes and strong resonance. However, the study of twist-angle modulation of hybridized exciton lifetimes is still insufficient, leading to an unclear understanding of the mechanism through which the twist angle between layers influences the lifetime of hybridized excitons. Here, we observed the formation of hybridized excitons by constructing MoSe2/WS2 heterostructures with different twist angles. The exciton lifetime is found to increase from 0.5 ns to 3.3 ns when the twist angle is reduced from 12° to 1°. This work provides a new perspective on the modulation of the exciton lifetime, enabling further exploration in improving the efficiency of optoelectronic devices.

Control of Hybrid Exciton Lifetime in MoSe2/WS2 Moiré Heterostructures.

Hybrid excitons, characterized by their strong oscillation strength and long lifetimes, hold great potential as information carriers in semiconductors. They offer promising applications in exciton-based devices and circuits. MoSe2/WS2 heterostructures represent an ideal platform for studying hybrid excitons, but how to regulate the exciton lifetime has not yet been explored. In this study, layer hybridization is modulated by applying electric fields parallel or antiparallel to the dipole moment, enabling us to regulate the exciton lifetime from 1.36 to 4.60 ns. Furthermore, the time-resolved photoluminescence decay traces are measured at different excitation power. A hybrid exciton annihilation rate of 8.9 × 10-4 cm2 s-1 is obtained by fitting. This work reveals the effects of electric fields and excitation power on the lifetime of hybrid excitons in MoSe2/WS2 1.5° moiré heterostructures, which play important roles in high photoluminescence quantum yield optoelectronic devices based on transition-metal dichalcogenides heterostructures.

Out-of-Plane Ferroelectricity in Two-Dimensional 1T‴-MoS2 Above Room Temperature.

Two-dimensional (2D) molybdenum disulfide (MoS2), one of the most extensively studied van der Waals (vdW) materials, is a significant candidate for electronic materials in the post-Moore era. MoS2 exhibits various phases, among which the 1T‴ phase possesses noncentrosymmetry. 1T‴-MoS2 was theoretically predicted to be ferroelectric a decade ago, but this has not been experimentally confirmed until now. Here, we have prepared high-purity 2D 1T‴-MoS2 crystals and experimentally confirmed the room-temperature out-of-plane ferroelectricity. The noncentrosymmetric crystal structure in 2D 1T‴-MoS2 was convinced by atomically resolved transmission electron microscopic imaging and second harmonic generation (SHG) measurements. Further, the ferroelectric polarization states in 2D 1T‴-MoS2 can be switched using piezoresponse force microscopy (PFM) and electrical gating in field-effect transistors (FETs). The ferroelectric-to-paraelectric transition temperature is measured to be about 350 K. Theoretical calculations have revealed that the ferroelectricity of 2D 1T‴-MoS2 originates from the intralayer charge transfer of S atoms within the layer. The discovery of intrinsic ferroelectricity in the 1T‴ phase of MoS2 further enriches the properties of this important vdW material, providing more possibilities for its application in the field of next-generation electronic devices.

Direct Visualization of Dark Interlayer Exciton Transport in Moiré Superlattices.

Moiré superlattices have emerged as an unprecedented manipulation tool for engineering correlated quantum phenomena in van der Waals heterostructures. With moiré potentials as a naturally configurable solid-state that sustains high exciton density, interlayer excitons in transition metal dichalcogenide heterostructures are expected to achieve high-temperature exciton condensation. However, the exciton degeneracy state is usually optically inactive due to the finite momentum of interlayer excitons. Experimental observation of dark interlayer excitons in moiré potentials remains challenging. Here we directly visualize the dark interlayer exciton transport in WS2/h-BN/WSe2 heterostructures using femtosecond transient absorption microscopy. We observe a transition from classical free exciton gas to quantum degeneracy by imaging temperature-dependent exciton transport. Below a critical degeneracy temperature, exciton diffusion rates exhibit an accelerating downward trend, which can be explained well by a nonlinear quantum diffusion model. These results open the door to quantum information processing and high-precision metrology in moiré superlattices.

Enhanced double resonance Raman scattering in multilayer graphene with broadband coherent anti-Stokes Raman spectroscopy.

Graphene's unique gapless band structure and remarkably large third-order optical susceptibility have drawn significant attention to its nonlinear optical response, particularly in the context of coherent anti-Stokes Raman scattering (CARS). Under the combined influence of phononic and electronic resonances, the CARS response of graphene has been observed to exhibit a distinctive feature of time-resolved dip-to-peak evolution. Here, we report a greatly enhanced double resonance Raman mode beyond the G mode of multi-layer graphene with broadband CARS measurements. The significant difference in the intensity ratio between CARS and SR for this mode may be attributed to the preferential activation of low-frequency phonons in the impulsive stimulated Raman scattering process (ISRS) and a lower dephasing rate. Our results build on a foundation towards a deeper exploration of the coherent Raman response of two-dimensional materials.

Effects of polyacrylic acid molecular weights on V2C-MXene nanocoatings for obtaining ultralow friction and ultralow wear in an ambient working environment.

Two modified V2C-MXene nanocoatings are prepared through different molecular weights of polyacrylic acid (polyacrylic acid with ∼4 50 000 is marked as LPAA, and polyacrylic acid with ∼4 000 000 is marked as HPAA) and two-dimensional V2C-MXene. Their properties are characterized using a ball-on-disc tribometer, three-dimensional white-light interferometry topography images, optical microscope, Raman spectrometer, focused ion beam/scanning electron microscope and high-resolution transmission electron microscope/energy dispersive X-ray spectrometer (HRTEM/EDS). As a result, an ultralow friction (µ ≈ 0.073 ± 0.024) and an ultralow wear (3.41 × 10-7 mm3 N-1 m-1 for ball scar, and 7.49 × 10-8 mm3 N-1 m-1 for disc track) are achieved for the LPAA@V2C vs. steel ball system tested under 4 N in the air through tribo-physicochemical interactions. During the rubbing process, the LPAA@V2C nanocoating is transferred onto counter-bodies to form mixed-phase lubricative tribofilms. Monitoring via a HRTEM/EDS, the mixed-phase lubricative tribofilms are found to be mainly composed of amorphous carbon phases containing O and V and layered nano-debris along the sliding surface. The tribofilm's stable structure is the key to realizing ultralow friction and ultralow wear through the LPAA modification. These findings disclose that MXene-based nanomaterials can be applied for material engineering and mechanical engineering under common working conditions.

Study on the Electrical Control Mechanism of Gas Occurrence in a Microscale Coal Matrix.

The study of the gas occurrence mechanism in a microscale coal matrix is the basis of coalbed methane (CBM) reservoir formation mechanism analysis and its exploration and development scheme design, which has important scientific and engineering significance. Currently, many researchers are focusing on a specific coal type to explore the macroscopic adsorption characteristics of gas occurrence. However, the research on the microscale gas-solid coupling mechanism is relatively rare and the electrical control mechanism of gas occurrence is not reported in detail. This study focuses on the electrical mechanism of microscale gas occurrence using physical simulation experiments and molecular dynamics analysis. This study clarifies the "gas adsorption-electrical properties-functional group" linkage mechanism and explores the macroscopic performance of the microscale gas occurrence mechanism using electrical properties. The study reveals the following: (1) the coal reservoirs exhibit a weak negative potential at the nanoscale, and the trends of surface potential (SP) and surface electrical charging density (SECD) are fluctuated with the degree of coal rank increases; (2) there is a good correlation between the SP, SECD values, and the relative content of functional groups; and (3) the charge density on the coal's microscopic surface influences their gas molecule attraction capacity, affecting the gas adsorption capacity of coal reservoirs at the macroscale. This study presents a theoretical foundation for establishing the molecular force field superposition mechanism of gas occurrence in microscale coal matrix and has broad application prospects in the macroscale numerical simulation of CBM development.

Non-contact friction energy dissipation via hysteretic behavior on a graphite surface.

For non-contact friction, energy is usually dissipated through phonon excitation, Joule dissipation and van der Waals friction. Although some new dissipation mechanisms related to the quantum phenomenon have been discovered, the contribution of hysteretic behavior to non-contact friction energy dissipation is lacking in research. In this paper, the distance dependence of non-contact friction on the graphite surface is studied by using a quartz tuning fork with lateral vibration in the atmosphere. It is found that energy dissipation begins to increase when the distance is less than 2 nm, showing the form of phonon dissipation. However, when the distance is further decreased, the dissipation deviates from phonon dissipation and presents a huge friction energy dissipation peak, which is caused by the hysteretic behavior between the vibration of the surface atoms and the oscillation of the tip. This work expands the understanding of the energy dissipation mechanism of non-contact friction.

Friction-Induced Clustered Rearrangement at a PbS Quantum Dot Nanocoating via Long-Term Lubrication under an Atmosphere Environment.

We report a long-term lubrication for a PbS QD nanocoating sliding against bearing steel balls in the air. Through tribo-physchemical interactions, ultralow friction (µ ≈ 0.078 ± 0.0026) is achieved for the system tested under 1 N for 60 min. During the rubbing process, the tribo-film of the counterfacing ball is covered by a degraded PbS QD layer and amorphous mixed phase. Meanwhile, the disc track surface is composed of degraded PbS QD layers, clustered rearranged PbS QD districts, induced decomposed Pb-enriched multilayers, and an amorphous mixed phase via friction-induced structural transformation. The PbS QDs are transferred onto the sliding contacts to form a robust tribo-film, which is the key to realizing ultralow friction. Consequently, a long-term lubrication mechanism is attributed to the synergetic tribo-physchemical interaction along sliding interfaces upon shift, redirection, and decomposition of nanoparticles. These discoveries reveal QD-based nanolubricants in common working conditions for mechanical engineering.

Visualizing Ultrafast Defect-Controlled Interlayer Electron-Phonon Coupling in Van der Waals Heterostructures.

Engineering ultrafast interlayer coupling provides access to new quantum phenomena and novel device functionalities in atomically thin van der Waals heterostructures. However, due to all the atoms of a monolayer material being exposed at the interfaces, the interlayer coupling is extremely susceptible to defects, resulting in high energy dissipation through heat and low device performance. The study of how defects affect the interlayer coupling at ultrafast and atomic scales remains a challenge. Here, using femtosecond transient absorption microscopy, a new defect-induced ultrafast interlayer electron-phonon coupling pathway is identified in a WS2 /graphene heterostructure, involving a three-body collision between electrons in WS2 and both acoustic phonons and defects in graphene. This interaction manifests as the reduced defect-related Raman resonant activity and the accelerated electron-phonon scattering time from 7.1 to 2.4 ps. Furthermore, the ultrafast interlayer coupling process is directly imaged. These insights will advance the fundamental knowledge of heat dissipation in nanoscale devices, and enable new ways to dynamically manipulate electrons and phonons via defects in van der Waals heterostructures.

Twist-angle-controlled neutral exciton annihilation in WS2 homostructures.

Exciton-exciton annihilation (EEA), as typical nonradiative recombination, plays an unpopular role in semiconductors. The nonradiative process significantly reduces the quantum yield of photoluminescence, which substantially inhibits the maximum efficiency of optoelectronic devices. Recently, laser irradiation, introducing defects and applying strain have become effective means to restrain EEA in two-dimensional (2D) transition metal dichalcogenides (TMDCs). However, these methods destroy the atomic structure of 2D materials and limit their practical applications. Fortunately, twisted structures are expected to validly suppress EEA through excellent interface quality. Here, we develop a non-destructive way to control EEA in WS2 homostructures by changing the interlayer twist angle, and systematically study the effect of interlayer twist angle on EEA, using fluorescence lifetime imaging measurement (FLIM) technology. Due to the large moiré potential at a small interlayer twist angle, the diffusion of excitons is hindered, and the EEA rate decreases from 1.01 × 10-1 cm2 s-1 in a 9° twisted WS2 homostructure to 4.26 × 10-2 cm2 s-1 in a 1° twisted WS2 homostructure. The results reveal the important role of the interlayer twist angle and EEA interaction in high photoluminescence quantum yield optoelectronic devices based on TMDC homostructures.

Inspection of Line Defects in Transition Metal Dichalcogenides Using a Microscopic Hyperspectral Imaging Technique.

The line defects of two-dimensional (2D) transition metal dichalcogenides (TMDs) play a vital role in determining their device performance. In this work, a microscopic hyperspectral imaging technique based on differential reflectance was introduced for the online inspection of line defects in TMDs. Upon comparison of the measurement results of imaging and spectra, the relationship between optical contrast and differential reflectance spectra was established. A light selection method was proposed to optimize the optical contrast of line defects. Via application of an image processing algorithm, an automatic detection of the line defects with a classification accuracy of 95% was achieved for WS2, MoS2, and MoSe2. This work not only provides a microscopic hyperspectral imaging technique for detecting 2D material defects but also introduces a versatile design strategy for developing an advanced machine vision spectroscopic system.

High-Precision Intelligent Cancer Diagnosis Method: 2D Raman Figures Combined with Deep Learning.

Raman spectroscopy, as a label-free detection technology, has been widely used in tumor diagnosis. However, most tumor diagnosis procedures utilize multivariate statistical analysis methods for classification, which poses a major bottleneck toward achieving high accuracy. Here, we propose a concept called the two-dimensional (2D) Raman figure combined with convolutional neural network (CNN) to improve the accuracy. Two-dimensional Raman figures can be obtained from four transformation methods: spectral recurrence plot (SRP), spectral Gramian angular field (SGAF), spectral short-time Fourier transform (SSTFT), and spectral Markov transition field (SMTF). Two-dimensional CNN models all yield more than 95% accuracy, which is higher than the PCA-LDA method and the Raman-spectrum-CNN method, indicating that 2D Raman figure inputs combined with CNN may be one reason for gaining excellent performances. Among 2D-CNN models, the main difference is the conversion, where SRP is based on the structure of wavenumber series with the best performances (98.9% accuracy, 99.5% sensitivity, 98.3% specificity), followed by SGAF on the wavenumber series, SSTFT on wavenumber and intensity information, and SMTF on wavenumber position information. The inclusion of external information in the conversion may be another reason for improvement in the accuracy. The excellent capability shows huge potential for tumor diagnosis via 2D Raman figures and may be applied in other spectroscopy analytical fields.

Imaging of Defect-Accelerated Energy Transfer in MoS2/hBN/WS2 Heterostructures.

Engineering energy transfer (ET) plays an important role in the exploration of novel optoelectronic devices. The efficient ET has been reasonably regulated using different strategies, such as dielectric properties, distance, and stacking angle. However, these strategies show limited degrees of freedom in regulation. Defects can provide more degrees of freedom, such as the type and density of defects. Herein, atomic-scale defect-accelerated ET is directly observed in MoS2/hBN/WS2 heterostructures by fluorescence lifetime imaging microscopy. Sulfur vacancies with different densities are introduced by controlling the oxygen plasma irradiation time. Our study shows that the ET rate can be increased from 1.25 to 6.58 ns-1 by accurately controlling the defect density. Also, the corresponding ET time is shortened from 0.80 to 0.15 ns, attributing to the participation of more neutral excitons in the ET process. These neutral excitons are transformed from trion excitons in MoS2, assisted by oxygen substitution at sulfur vacancies. Our insights not only help us better understand the role of defects in the ET process but also provide a new approach to engineer ET for further exploration of novel optoelectronic devices in van der Waals heterostructures.

Highly accurate diagnosis of lung adenocarcinoma and squamous cell carcinoma tissues by deep learning.

Intraoperative detection of the marginal tissues is the last and most important step to complete the resection of adenocarcinoma and squamous cell carcinoma. However, the current intraoperative diagnosis is time-consuming and requires numerous steps including staining. In this paper, we present the use of Raman spectroscopy with deep learning to achieve accurate diagnosis with stain-free process. To make the spectrum more suitable for deep learning, we utilize an unusual way of thinking which regards Raman spectral signal as a sequence and then converts it into two-dimensional Raman spectrogram by short-time Fourier transform as input. The normal-adenocarcinoma deep learning model and normal-squamous carcinoma deep learning model both achieve more than 96% accuracy, 95% sensitivity and 98% specificity when test, which higher than the conventional principal components analysis-linear discriminant analysis method with normal-adenocarcinoma model (0.896 accuracy, 0.867 sensitivity, 0.926 specificity) and normal-squamous carcinoma model (0.821 accuracy, 0.776 sensitivity, 1.000 specificity). The high performance of deep learning models provides a reliable way for intraoperative detection of marginal tissue, and is expected to reduce the detection time and save human lives.

A new opportunity for the emerging tellurium semiconductor: making resistive switching devices.

The development of the resistive switching cross-point array as the next-generation platform for high-density storage, in-memory computing and neuromorphic computing heavily relies on the improvement of the two component devices, volatile selector and nonvolatile memory, which have distinct operating current requirements. The perennial current-volatility dilemma that has been widely faced in various device implementations remains a major bottleneck. Here, we show that the device based on electrochemically active, low-thermal conductivity and low-melting temperature semiconducting tellurium filament can solve this dilemma, being able to function as either selector or memory in respective desired current ranges. Furthermore, we demonstrate one-selector-one-resistor behavior in a tandem of two identical Te-based devices, indicating the potential of Te-based device as a universal array building block. These nonconventional phenomena can be understood from a combination of unique electrical-thermal properties in Te. Preliminary device optimization efforts also indicate large and unique design space for Te-based resistive switching devices.

Accurate diagnosis of lung tissues for 2D Raman spectrogram by deep learning based on short-time Fourier transform.

Multivariate statistical analysis methods have an important role in spectrochemical analyses to rapidly identify and diagnose cancer and the subtype. However, utilizing these methods to analyze lager amount spectral data is challenging, and poses a major bottleneck toward achieving high accuracy. Here, a new convolutional neural networks (CNN) method based on short-time Fourier transform (STFT) to diagnose lung tissues via Raman spectra readily is proposed. The models yield that the accuracies of the new method are higher than the conventional methods (principal components analysis -linear discriminant analysis and support vector machine) for validation group (95.2% vs 85.5%, 94.4%) and test group (96.5% vs 90.4%, 93.9%) after cross-validation. The results illustrate that the new method which converts one-dimensional Raman data into two-dimensional Raman spectrograms improve the discriminatory ability of lung tissues and can achieve automatically accurate diagnosis of lung tissues.

Mineral Characteristics of Low-Rank Coal and the Effects on the Micro- and Nanoscale Pore-Fractures: A Case Study from the Zhundong Coalfield, Northwest China.

The mineral characteristics (occurrence, type, and content) of low-rank coal and their influence on coalbed methane (CBM) reservoirs are investigated at the micro- and nanoscales. Six coal samples of three representative coalmines were used to demonstrate the uniform tectonization from the Zhundong coalfield, NW China. Based on optical microscopy and scanning electron microscopyenergy dispersive spectrum (SEM-EDS) analysis, the mineral composition and occurrence characteristics were discussed. The micro- and nanoscale reservoir characteristics in low-rank coal (pore size distribution and adsorption capability) were studied by diverse methods, including lowtemperature N2 adsorption/desorption, mercury intrusion porosimetry and CH4 isotherm adsorption analysis. The coal reservoir nuclear magnetic T2 spectra of porosity and movable fluid were obtained by combining low-field nuclear magnetic resonance (NMR) analysis, which has an advantage of determining pore fluid technology. The mineral content is highly variable (4˜16 vol.%) in the Xi Heishan prospecting area of the Qitai region. Kaolinite, goyazite, ankerite and anorthosite were microscopically observed to be filling in coal pores and microfractures, and the minerals are given priority to silicate minerals. There is a greater content of mesopores (100-1000 nm) and transition pores (10-100 nm), and they are well connected. The micropores (0-10 nm) are dominated by parallel plate, closed or wedge-shaped pores. Furthermore, the microfractures are mainly observed for types B (width ≥ 5 µm and length≤ 10 mm) and D (width<5 µm and length<300 µm). The results show that microfractures B and C (width< 5 µm and length ≥ 300 µm) are better connected, but the orientation and connectivity of type D are worse. The Langmuir volume and mesopore content decreased with increasing mineral content, which shows that the low-rank coal minerals filled some adsorption space; the reduced CBM adsorption capacity and cellular pore and intergranular pore filled with minerals affect the mesopore content. Therefore, mineral characterization significantly influences methane adsorption capacity and pore structure.

Influence of elastic property on the friction between atomic force microscope tips and 2D materials.

The relationship between the elastic property of solid materials and friction has been discussed and studied by theoretical calculation and analysis. In the present work, we perform an experimental study concerning this relationship. Atomic force microscope (AFM) scanning of four different transition metal dichalcogenides is conducted under different experimental conditions. It is found that materials with smaller vertical interlayer force constant, which also means smaller elasticity modulus, have larger friction. We attribute this phenomenon to larger elastic deformation in softer materials, which results in a larger obstacle to the motion of AFM tips.

Ultrasensitive SERS detection of rhodamine 6G and p-nitrophenol based on electrochemically roughened nano-Au film.

Quantitative analysis of organic pollutants in environmental water is an important issue for ecological environment and human health. In this paper, the quantitative analysis of rhodamine 6G (R6G) and p-nitrophenol (PNP) is performed by the surface enhanced Raman scattering (SERS) technology. The enhancement of Raman signals is achieved on the surface of an electrochemically roughened nano-Au film. The SERS performance depends on the microstructure of roughened nano-Au films, which is affected by the thickness of Au films and electrochemical roughening parameters. The structure-dependence of SERS performance is validated by finite element simulation of local electromagnetic field distribution. An obvious SERS effect of R6G with an enhancement factor of 108 is obtained on the roughened nano-Au film. A sensitive SERS detection of R6G with a linear range of 10-9-10-5 M and a detection limit of 10-11 M is realized. Moreover, a wide linear range of 10-9-10-3 M is obtained for the detection of PNP. The roughened nano-Au film is an effective substrate for the SERS detection of organic pollutants with high reproducibility and good stability. Therefore, the electrochemical technology in this study is expected to be a very promising method for the fabrication of high-performance SERS substrate.