Correlating Nanocrystalline Structure with Electronic Properties in 2D Platinum Diselenide

Platinum diselenide (PtSe₂) is a 2D material with outstanding electronic and piezoresistive properties. The material can be grown at low temperatures in a scalable manner, which makes it extremely appealing for many potential electronics, photonics, and sensing applications. Here, the nanocrystalline structure of different PtSe₂ thin films grown by thermally assisted conversion (TAC) is investigated and is correlated with their electronic and piezoresistive properties. Scanning transmission electron microscopy for structural analysis, X-ray photoelectron spectroscopy (XPS) for chemical analysis, and Raman spectroscopy for phase identification are used. Electronic devices are fabricated using transferred PtSe₂ films for electrical characterization and piezoresistive gauge factor measurements. The variations of crystallite size and their orientations are found to have a strong correlation with the electronic and piezoresistive properties of the films, especially the sheet resistivity and the effective charge carrier mobility. The findings may pave the way for tuning and optimizing the properties of TAC-grown PtSe₂ toward numerous applications.     

Large-Scale,Controllable Synthesis of Ultrathin Platinum Diselenide Ribbons for Efficient Electrocatalytic Hydrogen Evolution

2D platinum diselenide (PtSe₂) exhibits exceptional layer-dependent electrical properties and high catalytic activity for hydrogen evolution reactions, making it an ideal system for studying structure–activity correlations. However, the synthesis of high-quality atomically thin PtSe₂ materials has proven challenging. This study presents a simple chemical vapor deposition method for synthesizing high-quality ultrathin 1T-PtSe₂ ribbons on Au foils, making it easily applicable. Theoretical and experimental results confirm that these atomically thin 1T-PtSe₂ ribbons possess abundant catalytic sites and can serve as ideal electrocatalysts. This study advances the large-scale synthesis and potential application of ultrathin transition metal disulfides and presents a novel method for designing and synthesizing highly active ultrathin catalysts.     

Fast,Self‐Driven,Air‐Stable,and Broadband Photodetector Based on Vertically Aligned PtSe2/GaAs Heterojunction

Group‐10 layered transitional metal dichalcogenides including PtS₂, PtSe₂, and PtTe₂ are excellent potential candidates for optoelectronic devices due to their unique properties such as high carrier mobility, tunable bandgap, stability, and flexibility. Large‐area platinum diselenide (PtSe₂) with semiconducting characteristics is far scarcely investigated. Here, the development of a high‐performance photodetector based on vertically aligned PtSe₂‐GaAs heterojunction which exhibits a broadband sensitivity from deep ultraviolet to near‐infrared light, with peak sensitivity from 650 to 810 nm, is reported. The I_light/I_dark ratio and responsivity of photodetector are 3 × 10⁴ and 262 mA W^?1 measured at 808 nm under zero bias voltage. The response speed of τ_r/τ_f is 5.5/6.5 µs, which represents the best result achieved for Group‐10 TMDs based optoelectronic device thus far. According to first‐principle density functional theory, the broad photoresponse ranging from visible to near‐infrared region is associated with the semiconducting characteristics of PtSe₂ which has interstitial Se atoms within the PtSe₂ layers. It is also revealed that the PtSe₂/GaAs photodetector does not exhibit performance degradation after six weeks in air. The generality of the above good results suggests that the vertically aligned PtSe₂ is an ideal material for high‐performance optoelectronic systems in the future.     

Few‐Layered PtS2 Phototransistor on h‐BN with High Gain

The very recently rediscovered group‐10 transition metal dichalcogenides (TMDs) such as PtS₂ and PtSe₂, have joined the 2D material family as potentially promising candidates for electronic and optoeletronic applications due to their theoretically high carrier mobility, widely tunable bandgap, and ultrastability. Here, the first exploration of optoelectronic application based on few‐layered PtS₂ using h‐BN as substrate is presented. The phototransistor exhibits high responsivity up to 1.56 × 10³ A W^?1 and detectivity of 2.9 × 10¹¹ Jones. Additionally, an ultrahigh photogain ≈2 × 10⁶ is obtained at a gate voltage V _g = 30 V, one of the highest gain among 2D photodetectors, which is attributed to the existence of trap states. More interestingly, the few‐layered PtS₂ phototransistor shows a back gate modulated photocurrent generation mechanism, that is, from the photoconductive effect dominant to photogating effect dominant via tuning the gate voltage from the OFF state to the ON state. Such good properties combined with gate‐controlled photoresponse of PtS₂ make it a competitive candidate for future 2D optoelectronic applications.     

Atomic and Molecular Layer Deposition of Hybrid Mo–Thiolate Thin Films with Enhanced Catalytic Activity

A synthetic route toward hybrid MoS₂‐based materials that combines the 2D bonding of MoS₂ with 3D networking of aliphatic carbon chains is devised, leading to a film with enhanced electrocatalytic activity. The hybrid inorganic–organic thin films are synthesized by combining atomic layer deposition (ALD) with molecular layer deposition (MLD) using the precursors molybdenum hexacarbonyl and 1,2‐ethanedithiol and characterized by in situ Fourier transform infrared spectroscopy, and the resultant material properties are probed by X‐ray photoelectron spectroscopy, Raman spectroscopy, and grazing incidence X‐ray diffraction. The process exhibits a growth rate of 1.3 Å per cycle, with an ALD/MLD temperature window of 155–175 °C. The hybrid films are moderately stable for about a week in ambient conditions, smooth (σ_RMS ≈ 5 Å for films 60 Å thick) and uniform, with densities ranging from 2.2–2.5 g cm^?3. The material is both optically transparent and catalytically active for the hydrogen evolution reaction (HER), with an overpotential (294 mV at ?10 mA cm^?2) superior to that of planar MoS₂. The enhancement in catalytic activity is attributed to the incorporation of organic chains into MoS₂, which induces a morphological change during electrochemical testing that increases surface area and yields high activity HER catalysts without the need for deliberate nanostructuring.     

Seed‐Induced Vertical Growth of 2D Bi2O2Se Nanoplates by Chemical Vapor Transport

As two‐dimensional (2D) layered materials attract more attention owing to their unique optical, electrical, and thermal properties, there are persistent efforts to grow high‐quality 2D layered materials for fundamental research and device applications. While large‐area 2D layered materials with high crystal quality can be obtained through chemical vapor transport, the strong binding between 2D layered materials and substrates poses a significant challenge for attempts to reveal their intrinsic properties and to use these 2D building blocks for constructing advanced heterostructured devices. Therefore, it would be ideal to grow high‐quality 2D materials with minimized contact and binding with substrate. Through both calculation and experiment, it is demonstrated that by introducing a seed layer at the nucleation stage, the crystallographic disregistry and the corresponding adhesion energy between 2D materials and substrate can be altered, resulting in a change of crystal surface in contact with the substrate, and therefore vertical growth of 2D materials on substrates. As an example, it is demonstrated that with Bi₂O₃ serving as a seed layer, vertical growth of 2D plates of Bi₂O₂Se on mica substrates can be realized. These vertically grown 2D nanoplates of Bi₂O₂Se can be conveniently transferred with their thermal properties investigated for the first time.     

Towards van der Waals Epitaxial Growth of GaAs on Si using a Graphene Buffer Layer

Van der Waals growth of GaAs on silicon using a two‐dimensional layered material, graphene, as a lattice mismatch/thermal expansion coefficient mismatch relieving buffer layer is presented. Two‐dimensional growth of GaAs thin films on graphene is a potential route towards heteroepitaxial integration of GaAs on silicon in the developing field of silicon photonics. Hetero‐layered GaAs is deposited by molecular beam epitaxy on graphene/silicon at growth temperatures ranging from 350 °C to 600 °C under a constant arsenic flux. Samples are characterized by plan‐view scanning electron microscopy, atomic force microscopy, Raman microscopy, and X‐ray diffraction. The low energy of the graphene surface and the GaAs/graphene interface is overcome through an optimized growth technique to obtain an atomically smooth low­ temperature GaAs nucleation layer. However, the low adsorption and migration energies of gallium and arsenic atoms on graphene result in cluster‐growth mode during crystallization of GaAs films at an elevated temperature. In this paper, we present the first example of an ultrasmooth morphology for GaAs films with a strong (111) oriented fiber‐texture on graphene/silicon using quasi van der Waals epitaxy, making it a remarkable step towards an eventual demonstration of the epitaxial growth of GaAs by this approach for heterogeneous integration.     

Synthesis,properties, and applications of large-scale two-dimensional materials by polymer-assisted deposition

Two-dimensional(2D) materials have attracted considerable attention because of their novel and tunable electronic,optical, ferromagnetic, and chemical properties. Compared to mechanical exfoliation and chemical vapor deposition, polymer-assisted deposition(PAD) is more suitable for mass production of 2D materials owing to its good reproducibility and reliability. In this review, we summarize the recent development of PAD on syntheses of 2D materials. First, we introduce principles and processing steps of PAD. Second, 2D materials, including graphene, MoS2, and MoS2/glassy-graphene heterostructures, are presented to illustrate the power of PAD and provide readers with the opportunity to assess the method. Last, we discuss the future prospects and challenges in this research field. This review provides a novel technique for preparing 2D layered materials and may inspire new applications of 2D layered materials.     

Inkjet Printing of MoS2

A simple and efficient inkjet printing technology is developed for molybdenum disulfide (MoS₂), one of the most attractive two‐dimensional layered materials. The technology effectively addresses critical issues associated with normal MoS₂ liquid dispersions (such as incompatible rheology, low concentration, and solvent toxicity), and hence can directly and reliably write uniform patterns of high‐quality (5–7 nm thick) MoS₂ nanosheets at a resolution of tens of micrometers. The technology efficiency facilitates the integration of printed MoS₂ patterns with other components (such as electrodes), and hence allows fabricating various functional devices, including thin film transistors, photoluminescence patterns, and photodetectors, in a simple, massive and cost‐effective manner while retains the unique properties of MoS₂. The technology has great potential in a variety of applications, such as photonics, optoelectronics, sensors, and energy storage.     

High-K dielectric deposition in 3D architectures: The case of Ta2O5 deposited with metal–organic precursor TBTDET

New applications in microelectronics need the integration of high capacitance devices. One way of this development is the integration of capacitors with 3D architecture such as trench fields. The challenge is then to deposit the dielectric material in a highly conformal way within trenches showing high aspects ratios. We have studied and modeled the conformality and the loading effect of Ta₂O₅ deposited by MOCVD in an analytical way.     

Coexistence of Negative and Positive Photoconductivity in Few-Layer PtSe2 Field-Effect Transistors

Platinum diselenide (PtSe₂) field-effect transistors with ultrathin channel regions exhibit p-type electrical conductivity that is sensitive to temperature and environmental pressure. Exposure to a supercontinuum white light source reveals that positive and negative photoconductivity coexists in the same device. The dominance of one type of photoconductivity over the other is controlled by environmental pressure. Indeed, positive photoconductivity observed in high vacuum converts to negative photoconductivity when the pressure is raised. Density functional theory calculations confirm that physisorbed oxygen molecules on the PtSe₂ surface act as acceptors. The desorption of oxygen molecules from the surface, caused by light irradiation, leads to decreased carrier concentration in the channel conductivity. The understanding of the charge transfer occurring between the physisorbed oxygen molecules and the PtSe₂ film provides an effective route for modulating the density of carriers and the optical properties of the material.     

Mixed‐Dimensional 1D ZnO–2D WSe2 van der Waals Heterojunction Device for Photosensors

2D layered van der Waals (vdW) atomic crystals are an emerging class of new materials that are receiving increasing attention owing to their unique properties. In particular, the dangling‐bond‐free surface of 2D materials enables integration of differently dimensioned materials into mixed‐dimensional vdW heterostructures. Such mixed‐dimensional heterostructures herald new opportunities for conducting fundamental nanoscience studies and developing nanoscale electronic/optoelectronic applications. This study presents a 1D ZnO nanowire (n‐type)–2D WSe₂ nanosheet (p‐type) vdW heterojunction diode for photodetection and imaging process. After amorphous fluoropolymer passivation, the ZnO–WSe₂ diode shows superior performance with a much‐enhanced rectification (ON/OFF) ratio of over 10⁶ and an ideality factor of 3.4–3.6 due to the carbon–fluorine (C? F) dipole effect. This heterojunction device exhibits spectral photoresponses from ultraviolet (400 nm) to near infrared (950 nm). Furthermore, a prototype visible imager is demonstrated using the ZnO–WSe₂ heterojunction diode as an imaging pixel. To the best of our knowledge, this is the first demonstration of an optoelectronic device based on a 1D–2D hybrid vdW heterojunction. This approach using a 1D ZnO–2D WSe₂ heterojunction paves the way for the further development of electronic/optoelectronic applications using mixed‐dimensional vdW heterostructures.     

Controlled Doping of Wafer‐Scale PtSe2 Films for Device Application

Semiconductive transition metal dichalcogenides (TMDs) have been considered as next generation semiconductors, but to date most device investigations are still based on microscale exfoliation with a low yield. Wafer scale growth of TMDs has been reported but effective doping approaches remain challenging due to their atomically thick nature. This work reports the synthesis of wafer‐scale continuous few‐layer PtSe₂ films with effective doping in a controllable manner. Chemical component analyses confirm that both n‐doping and p‐doping can be effectively modulated through a controlled selenization process. The electrical properties of PtSe₂ films have been systematically studied by fabricating top‐gated field effect transistors (FETs). The device current on/off ratio is optimized in two‐layer PtSe₂ FETs, and four‐terminal configuration displays a reasonably high effective field effect mobility (14 and 15 cm² V^?1 s^?1 for p‐type and n‐type FETs, respectively) with a nearly symmetric p‐type and n‐type performance. Temperature dependent measurement reveals that the variable range hopping is dominant at low temperatures. To further establish feasible application based on controllable doping of PtSe₂, a logic inverter and vertically stacked p–n junction arrays are demonstrated. These results validate that PtSe₂ is a promising candidate among the family of TMDs for future functional electronic applications.     

2D or Not 2D: Strain Tuning in Weakly Coupled Heterostructures

A route to realize strain engineering in weakly bonded heterostructures is presented. Such heterostructures, consisting of layered materials with a pronounced bond hierarchy of strong and weak bonds within and across their building blocks respectively, are anticipated to grow decoupled from each other. Hence, they are expected to be unsuitable for strain engineering as utilized for conventional materials which are strongly bonded isotropically. Here, it is shown for the first time that superlattices of layered chalcogenides (Sb₂Te₃/GeTe) behave neither as fully decoupled two‐dimensional (2D) materials nor as covalently bonded three‐dimensional (3D) materials. Instead, they form a novel class of 3D solids with an unparalleled atomic arrangement, featuring a distribution of lattice constants, which is tunable. A map to identify further material combinations with similar characteristic is given. It opens the way for the design of a novel class of artificial solids with unexplored properties.     

New Frontiers on van der Waals Layered Metal Phosphorous Trichalcogenides

The exponentially growing works on 2D materials have resulted in both high scientific interest and huge potential applications in nanocatalysis, optoelectronics, and spintronics. Of especial note is that the newly emerged and promising family of metal phosphorus trichalcogenides (MPX₃) contains semiconductors, metals, and insulators with intriguing layered structures and architectures. The bandgaps of the members in this family range from 1.3 to 3.5 eV, significantly enriching the application of 2D materials in the broad wavelength spectrum. In this review, emphasizing their remarkable structural, physicochemical, and magnetic properties, as well as the numerous applications in various fields, the innovative progress on layered MPX₃ crystals is summarized. Different from other layered materials, these crystals will advance a fascinating frontier in magnetism and spintronic devices with their especially featured atomic layered nanosheets. Thus, their crystal and electronic structures, along with some related researches in magnetism, are discussed in detail. The assortments of growth methods are then summarized. Considering their potential applications, the prominent utilization of these 2D MPX₃ nanoscrystals in catalysis, batteries, and optoelectronics is also discussed. Finally, the outlook of these kinds of layered nanomaterials is provided.     

Demonstration of enhanced the photocatalytic effect with PtSe2 and TiO2 treated large area graphene obtained by CVD method

Here, we report our method on enhancing the photocatalytic effect with PtSe₂ and TiO₂ treated large area graphene (LAG). The LAG was growth on copper foil at a low temperature (500 °C) under atmospheric pressure by chemical vapor deposition (CVD) method. A facile, fast ultrasonic method was then used to successfully synthesize PtSe₂-LAG/TiO₂ nanocomposites. The composites that were obtained were characterized using X-ray diffraction (XRD) spectroscopy, scanning electron microscopy (SEM) with energy dispersive X-ray (EDX) spectroscopy, transmission electron microscopy (TEM), Raman spectroscopic analysis, and X-ray photoelectron spectroscopy (XPS). UV–vis diffuse reflectance spectra (DRS) analyses were also performed, and the catalytic behavior was investigated by the decomposition of methylene blue (MB).The as-prepared LAG with a Raman D band was obtained, and graphene layers can be clearly seen in High-Resolution Transmission Electron Microscopy (HRTEM) images. The degradation performance of the MB solution was determined via UV–vis spectrophotometry. This improved photocatalytic activity is a result of the positive synergetic effect between PtSe₂ and LAG in the heterogeneous photocatalyst. In this study, the LAG behaves as an electron transfer agent, contributor, collector, and source of active adsorption sites. The optical properties were also observed to be affected by the different weight ratios of the LAG in the composites by observing their respective band gaps from diffuse reflectance spectra.     

微波光子异质/异构集成技术

微波光子芯片是支撑微波光子学发展的基石。针对微波光子芯片材料体系多样、难以多功能集成等问题,异质/ 异构集成技术提供了一种有效途径。该技术可将不同材料体系的最优性能器件集成到同一芯片上,大大扩展微波光子芯片的功能,降低微波光子功能模块的体积、重量,并提高其性能稳定性。本文介绍了目前主流的微波光子异质/ 异构集成技术和光电混合集成方面的主要研究进展,并对未来发展趋势进行展望。     

High Crystal Quality 2D Manganese Phosphorus Trichalcogenide Nanosheets and their Photocatalytic Activity

Transition metal phosphorus trichalcogenides (MPX₃, X = S, Se) are layered materials possessing high chemical diversity and wide range of applications in a broad wave length spectrum. Theoretical studies reveal that auspicious activity of photocatalytic water splitting can be realized from them. However, experimental efforts have so far been challenged with the synthesis bottleneck. Described herein is the general chemical vapor deposition (CVD) growth method and photocatalytic activity of these materials. A novel route to systematically grow MnPX₃ nanosheets on flexible carbon fiber substrate is reported. The temperature profile of the CVD process is carefully optimized that confer a facile and successful conversion of oxide precursor to phospho‐trichalcogenide with high crystallinity. Moreover, the obtained manganese‐based phosphorus trichalcogenide nanosheets demonstrate promising activity in sacrificial agent‐free photocatalytic water splitting under simulated solar light (AM 1.5G). This study provides a significant stepping stone in exploring the fascinating world of functional 2D materials and pursuing performance enhancement.     

Atomically Smooth Graphene-Based Hybrid Template for the Epitaxial Growth of Organic Semiconductor Crystals

Atomically thin 2D materials are good templates to grow organic semiconductor thin films with desirable features. However, the 2D materials typically exhibit surface roughness and spatial charge inhomogeneity due to nonuniform doping, which can affect the uniform assembly of organic thin films on the 2D materials. A hybrid template is presented for preparation of highly crystalline small-molecule organic semiconductor thin film that is fabricated by transferring graphene onto a highly ordered self-assembled monolayer. This hybrid graphene template has low surface roughness and spatially uniform doping, and it yields highly crystalline fullerene thin films with grain sizes >300 nm, which is the largest reported grain size for C₆₀ thin films on 2D materials. A graphene/fullerene/pentacene phototransistor fabricated directly on the hybrid template has five times higher photoresponsivity than a phototransistor fabricated on a conventional graphene template supported by a SiO₂ wafer.     

Large‐Area Chemical Vapor Deposited MoS2 with Transparent Conducting Oxide Contacts toward Fully Transparent 2D Electronics

2D semiconductors are poised to revolutionize the future of electronics and photonics, much like transparent oxide conductors and semiconductors have revolutionized the display industry. Herein, these two types of materials are combined to realize fully transparent 2D electronic devices and circuits. Specifically, a large‐area chemical vapor deposition process is developed to grow monolayer MoS₂ continuous films, which are, for the first time, combined with transparent conducting oxide (TCO) contacts. Transparent conducting aluminum doped zinc oxide contacts are deposited by atomic layer deposition, with composition tuning to achieve optimal conductivity and band‐offsets with MoS₂. The optimized process gives fully transparent TCO/MoS₂ 2D electronics with average visible‐range transmittance of 85%. The transistors show high mobility (4.2 cm² V^?1 s^?1), fast switching speed (0.114 V dec^?1), very low threshold voltage (0.69 V), and large switching ratio (4 × 10⁸). To our knowledge, these are the lowest threshold voltage and subthreshold swing values reported for monolayer chemical vapor deposition MoS₂ transistors. The transparent inverters show fast switching properties with a gain of 155 at a supply voltage of 10 V. The results demonstrate that transparent conducting oxides can be used as contact materials for 2D semiconductors, which opens new possibilities in 2D electronic and photonic applications.