Abstract: The frequent oil spill accidents during oil exploration and transportation have caused large economic loss and catastrophic environmental disasters. Due to low cost and simplicity, adsorption and filtration materials are often chosen to deal with oil spills, but the outcomes are not satisfactory mainly because of the awfully high viscosity of crude oil. Herein a photothermal ultra-high molecular weight polyethylene/MXene composite aerogel with a high light absorption (99.97%) and water repellency (water contact angle >148°) is developed by thermally induced phase separation method. The composite aerogel endows durable hydrophobicity with which the water contact angle is more than 142° in acidic/alkaline environments, and the maximum absorption capacity of 81 g g−1. In addition, it exhibits an excellent photothermal performance, rising surface temperature to 70 °C within 60 s under 1 sun irradiation, that can drastically reduce the crude oil absorption time from 60 min to 60 s, saving 98% of absorption time and reaching a crude oil absorption capacity of 21 g g−1. More interestingly, the designed solar evaporation device with the obtained composite aerogel can achieve an evaporation rate of 1.15 kg m−2h−1 and evaporation efficiency of 74%. The designed composite aerogel opens a possible pathway for solar-powered crude oil adsorption applications.

Abstract: In this work, a novel Ti3C2T x MXene/chitosan/lignosulfonate adsorbent (MCL), was prepared via a facile decoration of Ti3C2T x MXene sheets with chitosan/lignosulfonate nanospheres as a renewable and biodegradable additive that can improve the biocompatibility and aqueous stability of MXenes. Chitosan/lignosulfonate nanospheres were stabilized on the surface of MXne sheets, endowing them with a variety of surface functionalities, high specific surface area, and antioxidant characteristics. The competitive adsorption of multi-metal systems revealed that MCL had a preferential adsorption affinity toward various heavy metal ions; the MCL removal efficiency for the quinary-metal ions adsorption followed a trend of Pb(II) > Cr(VI) ≈ Cu(II) > Ni(II) ≈ Co(II) in neutral pH conditions. A moderate reduction was observed for Cu(II) and Cr(VI) ions. For all metals, the kinetics data fitted well with the pseudo-second-order model, and the adsorption equilibrium was best described by the Langmuir model. The adsorption mechanism is suggested to be a synergic combination of electrostatic interaction, surface complexation, and ion exchange. The findings of this study provide a new approach for eco-friendly MXene surface modification and give a general pattern of metal pollutants interactions during adsorption.

Abstract: As one of two-dimensional (2D) semiconductor materials, transition metal dichalcogenides (TMDs) have sparked enormous potential in next-generation optoelectronics due to their unique and excellent physical, electronic and optical properties. Controllable growth of wafer-scale 2D TMDs is essential to realize various high-end applications, while it remains challenging. Herein, 2-inch 2D WS2 films were successfully synthesized by ambient pressure chemical vapor deposition based on substrate engineering and space-confined strategies. WS2 nucleation density can be effectively modulated depending on the annealing conditions of sapphire substrate. 2D WS2 films with controllable thickness can be fabricated by adjusting the space-confined height. Moreover, our strategies are demonstrated to be universal for the growth of other 2D TMD semiconductors. WS2-based photodetectors with different thicknesses were systematically investigated. Monolayer WS2 photodetector displays large responsivity of 0.355 A/W and high specific detectivity of 1.48 × 1011 Jones. Multilayer WS2 device exhibits negative self-powered photoresponse. Our work provides a new route for the synthesis of wafer-scale 2D TMD materials, paving the way for high performance integrated optoelectronic devices.

Abstract: Recent advancements in the field of two-dimensional (2D) materials have led to the discovery of a wide range of 2D materials with intriguing properties. Atomistic-scale simulation methods have played a key role in these discoveries. In this review, we provide an overview of the recent progress in ReaxFF force field developments and applications in modeling the following layered and nonlayered 2D materials: graphene, transition metal dichalcogenides, MXenes, hexagonal boron nitrides, groups III-, IV- and V-elemental materials, as well as the mixed dimensional van der Waals heterostructures. We further discuss knowledge gaps and challenges associated with synthesis and characterization of 2D materials. We close this review with an outlook addressing the challenges as well as plans regarding ReaxFF development and possible large-scale simulations, which should be helpful to guide experimental studies in a discovery of new materials and devices.

Abstract: Layered materials (LMs) produced by liquid phase exfoliation (LPE) can be used as building blocks for optoelectronic applications. However, when compared with mechanically exfoliated flakes, or films prepared by chemical vapor deposition (CVD), LPE-based printed optoelectronic devices are limited by mobility, defects and trap states. Here, we present a scalable fabrication technique combining CVD with LPE LMs to overcome such limitations. We use black phosphorus inks, inkjet-printed on graphene on Si/SiO2, patterned by inkjet printing based lithography, and source and drain electrodes printed with an Ag ink, to prepare photodetectors (PDs). These have an external responsivity (R ext)∼337 A W−1 at 488 nm, and operate from visible (∼488 nm) to short-wave infrared (∼2.7 µm, R ext∼ 48 mA W−1). We also use this approach to fabricate flexible PDs on polyester fabric, one of the most common used in textiles, achieving R ext∼ 6 mA W−1 at 488 nm for an operating voltage of 1 V. Thus, our combination of scalable CVD and LPE techniques via inkjet printing is promising for wearable and flexible applications.

Abstract: Graphdiyne (GDY) is a new carbon allotrope with excellent properties due to its unique structure and highly conjugated system. In this work, GDY/CuMoO4 (CMO)/CuO tandem S-scheme heterojunction was constructed using the cross-coupling method. Among them, CuI is not only used as a coupling catalyst to obtain easily collected GDY, but also as a precursor for more active composite catalysts. 2D GDY provides a substrate for the loading of CMO and CuO, while the highly conjugated system and excellent electrical conductivity allow the composites to form a unique system with strong charge distribution and transport. The step-by-step progressive S-scheme heterojunctions constructed based on the one-step calcination strategy have stronger reducing activity and carrier transfer capability. The intrinsic charge transfer mechanism of the catalyst was investigated by photoelectrochemical characterization and in situ x-ray photoelectron spectroscopy analysis, and the mechanism of the photocatalytic hydrogen production reaction was proposed. This work provides a viable approach for the development of GDY in photocatalysis and the design of S-scheme heterojunctions.

Abstract: Abstract Manipulating the interlayer twist angle is a powerful tool to tailor the properties of layered two-dimensional crystals. The twist angle has a determinant impact on these systems’ atomistic structure and electronic properties. This includes the corrugation of individual layers, formation of stacking domains and other structural elements, and electronic structure changes due to the atomic reconstruction and superlattice effects. However, how these properties change with the twist angle, θ , is not yet well understood. Here, we monitor the change of twisted bilayer (tBL) MoS 2 characteristics as a function of θ . We identify distinct structural regimes, each with particular structural and electronic properties. We employ a hierarchical approach ranging from a reactive force field through the density-functional-based tight-binding approach and density-functional theory. To obtain a comprehensive overview, we analyzed a large number of tBLs with twist angles in the range of θ = 0.2 ∘ … 59.6 ∘ . Some systems include up to half a million atoms, making structure optimization and electronic property calculation challenging. For 13 ° ≲ θ ≲ 47 ° , the structure is well-described by a moiré regime composed of two rigidly twisted monolayers. At small twist angles ( θ ⩽ 3 ∘ and 57 ∘ ⩽ θ ), a domain-soliton regime evolves, where the structure contains large triangular stacking domains, separated by a network of strain solitons and short-ranged high-energy nodes. The corrugation of the layers and the emerging superlattice of solitons and stacking domains affects the electronic structure. Emerging predominant characteristic features are Dirac cones at K and kagome bands. These features flatten for θ approaching 0 ∘ and 60 ∘ . Our results show at which range of θ the characteristic features of the reconstruction, namely extended stacking domains, the soliton network, and superlattice, emerge and give rise to exciting electronics. We expect our findings also to be relevant for other tBL systems.

Abstract: Flexible broadband optoelectronic devices play a prominent role in the areas of daily life including wearable optoelectronic systems, health care, and bio-imaging systems. Two-dimensional (2D) narrow-bandgap materials with atomic thickness, adjustable bandgap, mechanical flexibility, as well as excellent optical and electrical properties exhibit great potential for applications in flexible optoelectronic devices. Here, we demonstrate a high-performance photodetector based on high-quality ternary Ta2NiSe5 nanosheets with a narrow bandgap of 0.25 eV. The photodetectors exhibit broadband photodetection capability in the visible-infrared (IR) spectrum (405–2200 nm) at room temperature. The maximum values of responsivity can reach up to 280 A W−1 at the wavelength of 405 nm. Meanwhile, the high responsivity of 63.9 A W−1 and detectivity of 3.8 × 109 Jones are achieved at the wavelength of 2200 nm, respectively. In addition, the obtained Ta2NiSe5-based photodetector shows excellent flexibility and the photodetection performance is almost insignificantly degraded after 1000 bending cycles. These results indicate that the 2D Ta2NiSe5 semiconductor has great potential in future wearable IR optoelectronic devices.

Abstract: The energy landscape of optical excitations in mono- and few-layer transition metal dichalcogenides (TMDs) is dominated by optically bright and dark excitons. These excitons can be fully localized within a single TMD layer, or the electron- and the hole-component of the exciton can be charge-separated over multiple TMD layers. Such intra- or interlayer excitons have been characterized in detail using all-optical spectroscopies, and, more recently, photoemission spectroscopy. In addition, there are so-called hybrid excitons whose electron- and/or hole-component are delocalized over two or more TMD layers, and therefore provide a promising pathway to mediate charge-transfer processes across the TMD interface. Hence, an in-situ characterization of their energy landscape and dynamics is of vital interest. In this work, using femtosecond momentum microscopy combined with many-particle modeling, we quantitatively compare the dynamics of momentum-indirect intralayer excitons in monolayer WSe2 with the dynamics of momentum-indirect hybrid excitons in heterobilayer WSe2/MoS2, and draw three key conclusions: First, we find that the energy of hybrid excitons is reduced when compared to excitons with pure intralayer character. Second, we show that the momentum-indirect intralayer and hybrid excitons are formed via exciton-phonon scattering from optically excited bright excitons. And third, we demonstrate that the efficiency for phonon absorption and emission processes in the mono- and the heterobilayer is strongly dependent on the energy alignment of the intralayer and hybrid excitons with respect to the optically excited bright exciton. Overall, our work provides microscopic insights into exciton dynamics in TMD mono- and bilayers.

Abstract: This work reports on the hardware implementation of analog dot-product operation on arrays of two-dimensional (2D) hexagonal boron nitride (h-BN) memristors. This extends beyond previous work that studied isolated device characteristics towards the application of analog neural network accelerators based on 2D memristor arrays. The wafer-level fabrication of the memristor arrays is enabled by large-area transfer of CVD-grown few-layer (8 layers) h-BN films. Individual devices achieve an on/off ratio of >10, low voltage operation (∼0.5 V set/V reset), good endurance (>6000 programming steps), and good retention (>104 s). The dot-product operation shows excellent linearity and repeatability, with low read energy consumption (∼200 aJ to 20 fJ per operation), with minimal error and deviation over various measurement cycles. Moreover, we present the implementation of a stochastic logistic regression algorithm in 2D h-BN memristor hardware for the classification of noisy images. The promising resistive switching characteristics, performance of dot-product computation, and successful demonstration of logistic regression in h-BN memristors signify an important step towards the integration of 2D materials for next-generation neuromorphic computing systems.

Abstract: Layered transition metal carbides or nitrides (MXenes), as a novel two-dimensional material, are widely used in the field of electromagnetic (EM) functions and devices due to their unique EM properties. However, the excessive conductivity of MXenes nanosheets often causes impedance mismatch, resulting in a single EM function. Moreover, original MXenes nanosheets are too small in size and needed to be dispersed in the matrix during application, resulting in inconvenience and unstable performance. Architecture strategy is an effective way to handle these problems. Assembling MXenes nanosheets into hierarchical structures, on the one hand, can effectively tailor conductivity, optimize impedance, and tune the EM response of MXenes, achieving multiple EM functions, on the other hand, can obtain directly usable macro assemblies. Herein, we systematically summarize various methods for fabricating MXenes hierarchical architectures, gaining deep insight into the EM response mechanism. Subsequently, the multiple EM functions including electromagnetic absorption (EMA) and electromagnetic interference (EMI) shielding were concluded. More importantly, rich progress has been made in EM functional devices based on MXene, but there is no review in this regard. We have provided a comprehensive summary of relevant excellent work in this review. Ultimately, we have provided insightful commentary on the challenges in this area and predicted the future direction.

Abstract: Two-dimensional (2D) materials have received extensive research attentions over the past two decades due to their intriguing physical properties (such as the ultrahigh mobility and strong light–matter interaction at atomic thickness) and a broad range of potential applications (especially in the fields of electronics and optoelectronics). The growth of single-crystal 2D materials is the prerequisite to realize 2D-based high-performance applications. In this review, we aim to provide an in-depth analysis of the state-of-the-art technology for the growth and applications of 2D materials, with particular emphasis on single crystals. We first summarize the major growth strategies for monolayer 2D single crystals. Following that, we discuss the growth of multilayer single crystals, including the control of thickness, stacking sequence, and heterostructure composition. Then we highlight the exploration of 2D single crystals in electronic and optoelectronic devices. Finally, a perspective is given to outline the research opportunities and the remaining challenges in this field.

Abstract: Abstract In recent years, much research has been undertaken to investigate the suitability of two-dimensional materials to act as single-photon sources with high optical and quantum optical quality. Amongst them, transition-metal dichalcogenides, especially WSe 2 , have been one of the subjects of intensive studies. Yet, their single-photon purity and photon indistinguishability remain the most significant challenges to compete with mature semiconducting systems such as self-assembled InGaAs quantum dots. In this work, we explore the emission properties of quantum emitters in a WSe 2 monolayer which are induced by metallic nanoparticles. Under quasi-resonant pulsed excitation, we verify clean single-photon emission with a g (2) (0) = 0.036 ± 0.004. Furthermore, we determine the temperature dependent coherence time via Michelson interferometry, where a value of (13.5 ± 1.0) ps is extracted for the zero-phonon line at 4 K, which reduces to (9 ± 2) ps at 8 K. Associated time-resolved photoluminescence experiments reveal a decrease of the decay time from (2.4 ± 0.1) ns to (0.42 ± 0.05) ns. This change in decay time is explained by a model which considers a Förster-type resonant energy transfer process which yields a strong temperature induced energy loss from the single-photon emitters to the nearby Ag nanoparticle.

Abstract: A polyol-assisted solvothermal route is used to synthesize Ni x Fe y nanoalloys supported on a highly electron conductive 2D transition metal Mo2CT x MXene. Structural, morphological and chemical characteristics of the materials are determined using several physicochemical techniques. The MXene support allows not only the formation of a nanostructured metallic Ni x Fe y nanoalloys, but also favors the interfacial charge transfer for the oxygen evolution reaction (OER). The Ni x Fe y @Mo2CT x material with a Ni/Fe ratio of 2.66 leads to the outstanding activity for the OER with an amazingly low Tafel slope value of 34 mV dec−1 and a current density of 10 mA.cm−2 at a potential of only 1.50 V vs. reversible hydrogen electrode (RHE). In situ Raman experiments show that β-NiOOH formed by oxidation of the nanoalloys under positive scan, likely containing a very small amount of Fe, is the active phase for the OER. This material exhibits also an excellent stability over 168 h in a 5 M KOH electrolyte. Transmission electron microscopy -electron energy-loss spectroscopy analyses after 100 voltammetric cycles between 0.2 and 1.55 V vs. RHE evidence for the first time that the MXene support is not fully oxidized in the first cycle. Also, oxyhydroxide layer formed in the OER potential region at the surface of the Ni x Fe y nanoparticles can be reversibly reduced.

Abstract: The capability to structure two-dimensional materials (2DMs) at the nanoscale with customizable patterns and over large areas is critical for a number of emerging applications, from nanoelectronics to 2D photonic metasurfaces. However, current technologies, such as photo- and electron-beam lithography, often employing masking layers, can significantly contaminate the materials. Large-area chemical vapour deposition-grown graphene is known to have non-ideal properties already due to surface contamination resulting from the transferring process. Additional contamination through the lithographic process might thus reduce the performance of any device based on the structured graphene. Here, we demonstrate a contactless chemical-free approach for simultaneous patterning and cleaning of self-supporting graphene membranes in a single step. Using energetic ions passing through a suspended mask with pre-defined nanopatterns, we deterministically structure graphene with demonstrated feature size of 15 nm, approaching the performance of small-area focused ion beam techniques and extreme ultraviolet lithography. Our approach, however, requires only a broad beam, no nanoscale beam positioning and enables large area patterning of 2DMs. Simultaneously, in regions surrounding the exposed areas, contaminations commonly observed on as-grown graphene targets, are effectively removed. This cleaning mechanism is attributed to coupling of surface diffusion and sputtering effects of adsorbed surface contaminants. For applications using 2DMs, this simultaneous patterning and cleaning mechanism may become essential for preparing the nanostructured materials with improved cleanliness and hence, quality.

Abstract: Quantifying and controlling the coherent dynamics and couplings of optically active excitations in solids is of paramount importance in fundamental research in condensed matter optics and for their prospective optoelectronic applications in quantum technologies. Here, we perform ultrafast coherent nonlinear spectroscopy of a charge-tunable MoSe2 monolayer. The experiments show that the homogeneous and inhomogeneous line width and the population decay of exciton complexes hosted by this material can be directly tuned by an applied gate bias, which governs the Fermi level and therefore the free carrier density. By performing two-dimensional spectroscopy, we also show that the same bias-tuning approach permits us to control the coherent coupling strength between charged and neutral exciton complexes.

Abstract: The fine structure of attractive Fermi polarons in van der Waals heterostructures based on monolayer transition metal dichalcogenides in the presence of elastic strain is studied theoretically. The charged excitons (trions), three particle bound states of two electrons and a hole or two holes and an electron, do not show any strain-induced fine structure splitting compared to neutral excitons whose radiative doublet is split by the strain into linearly polarized components. The correlation of the trions with Fermi sea holes gives rise to attractive Fermi polarons. We show that this results in a fine structure splitting of the polaron into states polarized along the main axes of the strain tensor. This effect is related to the bosonic statistics of Fermi polarons. We develop a microscopic theory of the effect and calculate the strain-induced splitting of Fermi polarons for both tungsten- and molybdenum-based monolayers, identifying the role of inter- and intravalley exciton–electron interactions. The fine structure splitting of the attractive Fermi polaron is proportional to both the excitonic splitting and the Fermi energy. The Fermi polaron fine structure in bilayers is briefly analyzed, and the role of electron and trion localization in moiré potentials is discussed.

Abstract: Abstract How to enhance the spin polarization, the Curie temperature and the perpendicular magnetic anisotropy (PMA) is crucial for the applications of 2D magnets in spintronic devices. In this work, based on the experimental FeCl 2 flakes and the predicted in-plane magnetic anisotropy (IMA) and lower Curie temperature of FeCl 2 monolayer, we use first-principles and Monte Carlo simulation to explore the strain and carrier-doping effects on the electronic and magnetic properties of Janus FeClF monolayer. The structure is stable within −10% to 2% biaxial strain. Janus FeClF monolayer can experience transitions from a half-semiconductor to a spin gapless semiconductor (SGS) around the −6% compressive strain, and from the IMA to the PMA at the −7% compressive strain. The super-exchange Fe–F/Cl–Fe interaction induces the ferromagnetic coupling, and the Curie temperature can be considerably enhanced from 56 K to 281 K at the −10% compressive strain. The half-metallicity can be achieved whether under electron doping or hole doping. The Fe- d orbitals and the spin–orbit coupling interaction between occupied and unoccupied intraorbital states are responsible for the electronic phase transition and the magnetic anisotropy, respectively. Remarkably, the compressive −10% strain and the 0.02 e doping collectively increase the Curie temperature to near room temperature (286 K). The high spin polarization (exhibiting SGS and half-metal), the PMA and the near-room-temperature ferromagnetism induced by strain and doping make Janus FeClF a promising candidate for 2D spintronic applications, which will stimulate experimental and theoretical broad studies on this class of Janus monolayers FeXY (X,Y = F, Cl, Br, and X ≠ Y).

Abstract: A significant challenge for graphene nanoplatelet (GNP) suppliers is the characterisation of platelet morphology in industrial environments. This challenge is further exacerbated to platelet surface chemistry when scalable functionalisation processes, such as plasma treatment, are used to modify the GNPs to improve the filler-matrix interphase in nanocomposites. The costly and complex suite of analytical equipment necessary for a complete material description makes quality control and process optimisation difficult. Raman spectroscopy is a facile and accessible characterisation technique, with recent advancements unlocking fast mapping for rapid data collection. In this study, we develop novel techniques to better characterise GNP morphology and changes in surface chemistry using Raman maps of bulk powders. Providing a bespoke algorithmic framework for the analysis of these advanced materials. An unsupervised peak fitting and processing algorithm was used to extract crystallinity data and correlate it with laser-diffraction-derived lateral size values for a commercial set of GNPs rapidly and accurately. Classical machine learning was used to identify the most informative Raman features for classifying the plasma-functionalised GNPs. The initial material properties were found to affect the peak features that were the most useful for classification. In low defect density and low specific surface area GNPs, the D peak full width at half maximum is found to be the most useful, whereas the I2D/IG ratio is the most useful in the opposite case. Finally, a convolutional neural network was trained to discern between different GNP grades with 86% accuracy. This work demonstrates how computer vision could be deployed for rapid and accurate quality control on the factory floor.

Abstract: The effect of degeneracy and the impact of free-carrier screening on a low-field mobility and a high-field drift velocity in MoS2 and WS2 are explored using an in-house ensemble Monte Carlo simulator. Electron low field mobility increases to 8400cm2V−1s−1 for MoS2 and to 12040cm2V−1s−1 for WS2 when temperature decreases to 77K and carrier concentration is around 5×1012cm−2 . In the case of holes, best mobility values were 9320cm2V−1s−1 and 13290cm2V−1s−1 , reached at similar temperature and carrier concentration conditions while at room temperature these fall to 80cm2V−1s−1 and 150cm2V−1s−1 for MoS2 and WS2, respectively. The carrier screening effect plays a major role at low fields, and low and intermediate temperatures, where a combination of large occupancy of primary valleys and carrier–phonon interactions dominated by relatively low energy exchange processes results in an enhanced screening of intrinsic scattering. For electrons, degeneracy yields to transport in secondary valleys, which plays an important role in the decrease of the low field mobility at high concentrations and/or at room temperature. The high-field drift velocity is not much affected by carrier screening because of an increased carrier scattering with surface optical polar phonons, favouring larger phonon wavevector interactions with small dielectric function values.

Abstract: Abstract Moiré interference effects influence profoundly the optoelectronic properties of vertical van der Waals structures. Here we systematically establish secondary electron imaging in a scanning electron microscope as a powerful technique for visualizing reconstruction of moiré lattices into registry-contrasting domains in vertical homobilayers and heteorbilayers of transition metal dichalcogenides (TMDs) with parallel and antiparallel alignment. With optimal parameters for contrast-maximizing imaging of high-symmetry registries, we identify distinct crystal realizations of WSe 2 homobilayers and MoSe 2 –WSe 2 heterostructures synthesized by chemical vapor deposition. In particular, we find evidence for a mutually exclusive competition between R h X and R h M registries, manifesting in complete reconstruction of bilayer crystals into one distinct registry or alternating large-area domains in R h X and R h M stacking. Our results have immediate implications for the optical properties of registry-specific excitons in layered stacks of TMDs, and demonstrate the general potential of secondary electron imaging for van der Waals twistronics.

Abstract: Integration of graphene and hexagonal boron nitride (hBN) in lateral heterostructures has provided a route to broadly engineer the material properties by quantum confinement of electrons or introduction of novel electronic and magnetic states at the interface. In this work we demonstrate lateral heteroepitaxial growth of graphene nanoribbons (GNRs) passivated by hBN using high-temperature molecular beam epitaxy (HT-MBE) to grow graphene in oriented hBN trenches formed ex-situ by catalytic nanoparticle etching. High-resolution atomic force microscopy (AFM) reveals that GNRs grow epitaxially from the etched hBN edges, and merge to form a GNR network passivated by hBN. Using conductive AFM we probe the nanoscale electrical properties of the nanoribbons and observe quasiparticle interference patterns caused by intervalley scattering at the graphene/hBN interface, which carries implications for the potential transport characteristics of hBN passivated GNR devices.

Abstract: Nanomechanical spectroscopy (NMS) is a recently developed approach to determine optical absorption spectra of nanoscale materials via mechanical measurements. It is based on measuring changes in the resonance frequency of a membrane resonator vs. the photon energy of incoming light. This method is a direct measurement of absorption, which has practical advantages compared to common optical spectroscopy approaches. In the case of two-dimensional (2D) materials, NMS overcomes limitations inherent to conventional optical methods, such as the complications associated with measurements at high magnetic fields and low temperatures. In this work, we develop a protocol for NMS of 2D materials that yields two orders of magnitude improved sensitivity compared to previous approaches, while being simpler to use. To this end, we use mechanical sample actuation, which simplifies the experiment and provides a reliable calibration for greater accuracy. Additionally, the use of low-stress silicon nitride membranes as our substrate reduces the noise-equivalent power to NEP=890 fW Hz−1 , comparable to commercial semiconductor photodetectors. We use our approach to spectroscopically characterize a 2D transition metal dichalcogenide (WS2), a layered magnetic semiconductor (CrPS4), and a plasmonic super-crystal consisting of gold nanoparticles.

Abstract: Abstract Epitaxial growth has become a promising route to achieve highly crystalline continuous two-dimensional layers. However, high-quality layer production with expected electrical properties is still challenging due to the defects induced by the coalescence between imperfectly aligned domains. In order to control their intrinsic properties at the device scale, the synthesized materials should be described as a patchwork of coalesced domains. Here, we report multi-scale and multi-structural analysis on highly oriented epitaxial WS 2 and WSe 2 monolayers using scanning transmission electron microscopy (STEM) techniques. Characteristic domain junctions are first identified and classified based on the detailed atomic structure analysis using aberration corrected STEM imaging. Mapping orientation, polar direction and phase at the micrometer scale using four-dimensional STEM enabled to access the density and the distribution of the specific domain junctions. Our results validate a readily applicable process for the study of highly oriented epitaxial transition metal dichalcogenides, providing an overview of synthesized materials from large scale down to atomic scale with multiple structural information.

Abstract: Graphene oxide (GO) sheet structures are highly variable and depend on preparation conditions. The use of molecular simulation is a complementary strategy to explore how this complexity influences the ion transport properties of GO membranes. However, despite recent advances, computational models of GO typically lack the required complexity as suggested by experiment. The labor required to create such an ensemble of such structural models with the required complexity is impractical without recourse to automated approaches, but no such code currently can meet this challenge. Here, a modular tiling concept is introduced, along with the HierGO suite of code; an automated approach to producing highly complex hierarchically-structured models of GO with a high degree of control in terms of holes and topological defects, and oxygen-group placement, that can produce simulation-ready input files. The benefits of the code are exemplified by modeling and contrasting the properties of three types of GO membrane stack; the widely-modeled Lerf–Klinowski structure, and two types of highly heterogeneous GO sheet reflecting differing processing conditions. The outcomes of this work clearly demonstrate how the introduction of the complexity modeled here leads to new insights into the structure/property relationships of GO with respect to permeation pathways of water, ions and molecular agents that are inaccessible using previously-considered models.

Abstract: Herein, we established a synthetic route towards MXene/poly(ionic liquid) (PIL) composite porous membranes as a new platform of solar-thermal conversion materials. These membranes were made by a base-triggered ionic crosslinking process between a cationic PIL and a weak polyacid in solution in the presence of dispersed MXene nanosheets. A three-dimensionally interconnected porous architecture was formed with MXene nanosheets uniformly distributed within it. The unique characteristics of the as-produced composite membranes displays significant light-to-heat conversion and excellent performance for solar-driven water vapor generation. This facile synthetic strategy opens a new avenue for developing composite porous membranes as solar absorbers for the solar-driven water production from natural resources.

Abstract: High-performance photodetectors in the near-infrared (NIR) regime are essential for many advanced applications, such as optical communication, intelligent driving, and imaging system. However, conventional photoconductive infrared detectors commonly suffer from slow response speed and narrow spectral response. Here, we demonstrate a high performance NIR photodetector based on plasmonic sub-stoichiometry molybdenum oxide (MoO3−x) nanostructures/graphene heterostructure. Empowered by surface plasmon resonance induced near-field enhancement in MoO3−x and the subsequent hot-electron injection (HEI), a fast response time (rise time ∼6.7 μs, decay time ∼12.5 μs), high responsivity (3.3 A/W), low noise equivalent power (∼4.9 pW/Hz1/2), as well as wide response range from visible light to NIR is obtained at room temperature. The weak carrier–phonon interaction in graphene prevents the relaxation of injected hot electrons and enables efficient electron extraction. The response speed is nearly four orders of magnitude improved compared with other graphene-based hybrid devices with similar device structures. Moreover, the interfacial HEI breaks the bandgap limits of molybdenum oxide and further extends the response spectrum of the device to conventional band (C-band) of optical communication. Our proposed device architecture offers new strategy for developing high-performance infrared photodetectors.

Abstract: Point defects in hexagonal boron nitride (hBN) are promising candidates as single-photon emitters (SPEs) in nanophotonics and quantum information applications. The precise control of SPEs requires in-depth understanding of their optoelectronic properties. However, how the surrounding environment of host materials, including the number of layers, substrates, and strain, influences SPEs has not been fully understood. In this work, we study the dielectric screening effect due to the number of layers and substrates, and the strain effect on the optical properties of carbon dimer and nitrogen vacancy defects in hBN from first-principles many-body perturbation theory. We report that environmental screening causes a lowering of the quasiparticle gap and exciton binding energy, leading to nearly constant optical excitation energy and exciton radiative lifetime. We explain the results with an analytical model starting from the Bethe–Salpeter equation Hamiltonian with Wannier basis. We also show that optical properties of quantum defects are largely tunable by strain with highly anisotropic response, in good agreement with experimental measurements. Our work clarifies the effect of environmental screening and strain on optoelectronic properties of quantum defects in two-dimensional insulators, facilitating future applications of SPEs and spin qubits in low-dimensional systems.

Abstract: Abstract Cathodoluminescence spectroscopy in conjunction with second-order auto-correlation measurements of g 2 ( τ ) allows to extensively study the synchronization of photon emitters in low-dimensional structures. Co-existing excitons in two-dimensional transition metal dichalcogenide monolayers provide a great source of identical photon emitters which can be simultaneously excited by an electron. Here, we demonstrate large photon bunching with g 2 ( 0 ) up to 156 ± 16 of a tungsten disulfide monolayer (WS 2 ), exhibiting a strong dependence on the electron-beam current. To further improve the excitation synchronization and the electron-emitter interaction, we show exemplary that the careful selection of a simple and compact geometry—a thin, monocrystalline gold nanodisk—can be used to realize a record-high bunching g 2 ( 0 ) of up to 2152 ± 236 . This approach to control the electron excitation of excitons in a WS 2 monolayer allows for the synchronization of photon emitters in an ensemble, which is important to further advance light information and computing technologies.