Enhancement of Carrier Mobility in Multilayer InSe Transistors by van der Waals Integration.

Two-dimensional material indium selenide (InSe) holds great promise for applications in electronics and optoelectronics by virtue of its fascinating properties. However, most multilayer InSe-based transistors suffer from extrinsic scattering effects from interface disorders and the environment, which cause carrier mobility and density fluctuations and hinder their practical application. In this work, we employ the non-destructive method of van der Waals (vdW) integration to improve the electron mobility of back-gated multilayer InSe FETs. After introducing the hexagonal boron nitride (h-BN) as both an encapsulation layer and back-gate dielectric with the vdW interface, as well as graphene serving as a buffer contact layer, the electron mobilities of InSe FETs are substantially enhanced. The vdW-integrated devices exhibit a high electron mobility exceeding 103 cm2 V-1 s-1 and current on/off ratios of ~108 at room temperature. Meanwhile, the electron densities are found to exceed 1012 cm-2. In addition, the fabricated devices show an excellent stability with a negligible electrical degradation after storage in ambient conditions for one month. Electrical transport measurements on InSe FETs in different configurations suggest that a performance enhancement with vdW integration should arise from a sufficient screening effect on the interface impurities and an effective passivation of the air-sensitive surface.

Selective Chemical Vapor Deposition Growth of WS2/MoS2 Vertical and Lateral Heterostructures on Gold Foils.

Vertical and lateral heterostructures consisting of atomically layered two-dimensional (2D) materials exhibit intriguing properties, such as efficient charge/energy transfer, high photoresponsivity, and enhanced photocatalytic activities. However, the controlled fabrication of vertical or lateral heterojunctions on metal substrates remains challenging. Herein, we report a facile and controllable method for selective growth of WS2/MoS2 vertical or lateral heterojunctions on polycrystalline gold (Au) foil by tuning the gas flow rate of hydrogen (H2). We find that lateral growth is favored without H2, whereas vertical growth mode can be switched on by introducing 8-10 sccm H2. In addition, the areal coverage of the WS2/MoS2 vertical heterostructures is tunable in the range of 12-25%. Transmission electron microscopy (TEM) and selected area electron diffraction (SAED) results demonstrate the quality and absence of cross-contamination of the as-grown heterostructures. Furthermore, we investigate the effects of the H2 flow rate on the morphology of the heterostructures. These pave the way to develop unprecedented 2D heterostructures towards applications in (opto)electronic devices.

1T-Phase Dirac Semimetal PdTe2 Nanoparticles for Efficient Photothermal Therapy in the NIR-II Biowindow.

1T-phase transition-metal dichalcogenides (TMDs) nanomaterials are one type of emerging and promising near-infrared II (NIR-II) photothermal agents (PTAs) derived from their distinct metallic electronic structure, but it is still challenging to synthesize these nanomaterials. Herein, PdTe2 nanoparticles (PTNs) with a 1T crystal symmetry and around 50 nm in size are prepared by an electrochemical exfoliation method, and the corresponding photothermal performances irradiated under a NIR-II laser have been explored. The encapsulation of 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-poly(ethylene glycol) (DSPE-PEG) endows PTNs with water solubility, enhanced photothermal stability, and high biocompatibility. Notably, PTN/DSPE-PEG displays a potent absorbance through the NIR-II zone and considerable photothermal conversion efficiency, which is up to 68% when irradiated with a 1060 nm laser. With these unique photothermal properties, excellent in vitro and in vivo tumor inhibition effects of PTN/DSPE-PEG have been achieved under the irradiation of a NIR-II (1060 nm) laser without visible toxicity to normal tissues, suggesting that it is an efficient NIR-II photothermal nanoagent.

Ultrathin Single-Crystalline 2D Perovskite Photoconductor for High-Performance Narrowband and Wide Linear Dynamic Range Photodetection.

For next-generation Internet-of-Everything applications, for example, artificial-neural-network image sensors, artificial retina, visible light communication, on-chip light interconnection, and flexible devices, etc., high-performance microscale photodetectors are in urgent demands. 2D material (2DM) photodetectors have been researched and demonstrated impressive performances. However, they have not met the demands in filterless narrowband photoresponse, wide linear dynamic range (LDR), ultralow dark current, and large on/off ratio, which are key performances for these applications. 2D Ruddlesden-Popper perovskites (2D-RPPs) are recently highlighted photovoltaic and optoelectronic materials. Embedding ultrathin 2D-RPPs into 2DM photodetectors holds potentials to improve these performances. Herein, a single-crystalline ultrathin (PEA)2 PbI4 is integrated into a vertical-stacked graphene-(PEA)2 PbI4 -graphene micro photoconductor (V-PEPI-PC). V-PEPI-PC exhibits narrowband photoresponses at 517 nm with a full-width-at-half-maximum of 15 nm and a wide LDR of 122 dB. Due to the multiple quantum wells in (PEA)2 PbI4 , V-PEPI-PC demonstrates an ultralow dark current of 1.1 × 10-14 A (44 pA mm-2 ), a high specific detectivity of 1.2 × 1013 Jones, and a high on/off ratio of 1.6 × 106 . Owing to the short vertical channel, V-PEPI-PC shows a fast response rise time of 486 µs. Therefore, the vertical-stacked photodetectors based on hybrid 2D-RPPs and 2DMs may have great potentials in future optoelectronics.

Visible to near-infrared photodetector with novel optoelectronic performance based on graphene/S-doped InSe heterostructure on h-BN substrate.

van der Waals heterostructures of two-dimensional (2D) materials have attracted considerable attention due to their flexibility in the design of new functional devices. Despite numerous studies on graphene/2D semiconductor heterostructures, their optoelectronic applications are significantly hindered because of several disadvantages, such as large band gaps and chemical instability. In this work, we demonstrate the fabrication of graphene/S-doped InSe heterostructure photodetectors with excellent photoresponse performance, and this is attributed to the moderate band gap and band gap engineering by element doping of InSe as well as the high carrier mobility of graphene. In particular, the graphene/InSe0.9S0.1 device achieves an ultrahigh photoresponsivity of ∼4.9 × 106 A W-1 at 700 nm and an EQE of 8.7 × 108%, and it exhibits broadband photodetection (visible to near-infrared). More importantly, by virtue of the interaction between n-type graphene arising from the influence of h-BN as a dielectric layer and S-doped InSe with a high work-function, our devices always exhibited positive photocurrent when the polarity of the gate voltage is adjusted, and is different from that the previously reported graphene/2D semiconductor photodetectors. This work not only provides a promising platform for highly efficient broadband photodetectors but also sheds light on tuning the optoelectronic performance through band gap engineering and designing novel heterostructures-based various 2D materials.

Surface-Modified Ultrathin InSe Nanosheets with Enhanced Stability and Photoluminescence for High-Performance Optoelectronics.

Indium selenide (InSe) has become a research hotspot because of its favorable carrier mobility and thickness-tunable band gap, showing great application potential in high-performance optoelectronic devices. The trend of miniaturization in optoelectronics has forced the feature sizes of the electronic components to shrink accordingly. Therefore, atomically thin InSe crystals may play an important role in future optoelectronics. Given the instability and ultralow photoluminescent (PL) emission of mechanically exfoliated ultrathin InSe, synthesis of highly stable mono- and few-layer InSe nanosheets with high PL efficiency has become crucial. Herein, ultrathin InSe nanosheets were prepared via thermal annealing of electrochemically intercalated products from bulk InSe. The size and yield of the as-prepared nanosheets were up to ∼160 µm and ∼70%, respectively, and ∼80% of the nanosheets were less than five layer. Impressively, the as-prepared nanosheets showed greatly enhanced stability and PL emission because of surface modification by carbon species. Efficient photoresponsivity of 2 A/W was achieved in the as-prepared nanosheet-based devices. These nanosheets were further assembled into large-area thin films with photoresponsivity of 16 A/W and an average Hall mobility of about 5 cm2 V-1 s-1. Finally, one-dimensional (1D) InSe nanoscrolls with a length up to 90 µm were constructed by solvent-assisted self-assembly of the exfoliated nanosheets.

Synthesis of large-area uniform Si2Te3 thin films for p-type electronic devices.

Two-dimensional (2D) p-n junctions are basic components of various functional devices. However, the shortage of natural p-type 2D semiconductors makes it difficult to achieve both p-type and n-type transport in high-performance multifunctional devices. Here, continuous and uniform p-type Si2Te3 thin films are grown on SiO2/Si substrates, which are simultaneously used as an in situ Si source. Large-size 2D films with dimensions of ∼8 × 2 cm2 are prepared for the first time using a reliable and simple chemical vapor deposition (CVD) technique. Film growth occurs via the vapor-liquid-solid mechanism, allowing the film thickness to be controlled by the substrate temperature. As the Si2Te3 film thickness increases from 3 to 8 nm, the bandgap decreases from 2.07 to 1.65 eV. Moreover, the directly grown thin films possess high crystallinity, showing electronic properties that are comparable to those of MoTe2 crystals and MoS2 films. Therefore, this large-area growth of p-type Si2Te3 enriches the 2D semiconductor library and opens up a new platform for the study of p-type Si2Te3, which has potential for application in p-n junctions.

High-Yield Electrochemical Production of Large-Sized and Thinly Layered NiPS3 Flakes for Overall Water Splitting.

Achieving large-sized and thinly layered 2D metal phosphorus trichalcogenides with high quality and yield has been an urgent quest due to extraordinary physical/chemical characteristics for multiple applications. Nevertheless, current preparation methodologies suffer from uncontrolled thicknesses, uneven morphologies and area distributions, long processing times, and inferior quality. Here, a sonication-free and fast (in minutes) electrochemical cathodic exfoliation approach is reported that can prepare large-sized (typically ≈150 µm2 ) and thinly layered (≈70% monolayer) NiPS3 flakes with high crystallinity and pure phase structure with a yield ≈80%. During the electrochemical exfoliation process, the tetra-n-butylammonium salt with a large ionic diameter is decomposed into gaseous species after the intercalation and efficiently expands the tightly stratified bulk NiPS3 crystals, as revealed by in situ and ex situ characterizations. Atomically thin NiPS3 flakes can be obtained by slight manual shaking rather than sonication, which largely preserves in-plane structural integrity with large size and minimum damage. The obtained high quality NiPS3 offers a new and ideal model for overall water splitting due to its inherent fully exposed S and P atoms that are often the active sites for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Consequently, the bifunctional NiPS3 exhibits outstanding performance for overall water splitting.

Phase Identification and Strong Second Harmonic Generation in Pure ε-InSe and Its Alloys.

Two-dimensional material indium selenide (InSe) has offered a new platform for fundamental research in virtue of its emerging fascinating properties. Unlike 2H-phase transition-metal dichalcogenides (TMDs), ε phase InSe with a hexagonal unit cell possesses broken inversion symmetry in all the layer numbers, and predicted to have a strong second harmonic generation (SHG) effect. In this work, we find that the as-prepared pure InSe, alloyed InSe1- xTe x and InSe1- xS x ( x = 0.1 and 0.2) are ε phase structures and exhibit excellent SHG performance from few-layer to bulk-like dimension. This high SHG efficiency is attributed to the noncentrosymmetric crystal structure of the ε-InSe system, which has been clearly verified by aberration-corrected scanning transmission electron microscopy (STEM) images. The experimental results show that the SHG intensities from multilayer pure ε-InSe and alloyed InSe0.9Te0.1 and InSe1- xS x ( x = 0.1 and 0.2) are around 1-2 orders of magnitude higher than that of the monolayer TMD systems and even superior to that of GaSe with the same thickness. The estimated nonlinear susceptibility χ(2) of ε-InSe is larger than that of ε-GaSe and monolayer TMDs. Our study provides first-hand information about the phase identification of ε-InSe and indicates an excellent candidate for nonlinear optical (NLO) applications as well as the possibility of engineering SHG response by alloying.

Toward Exploring the Structure of Monolayer to Few-layer TaS2 by Efficient Ultrasound-free Exfoliation.

Tantalum disulfide nanosheets have attracted great interest due to its electronic properties and device applications. Traditional solution-ased ultrasonic process is limited by ultrasound which may cause the disintegration into submicron-sized flake. Here, an efficient multi-step intercalation and ultrasound-free process has been successfully used to exfoliate 1T-TaS2. The obtained TaS2 nanosheets reveal an average thickness of 3 nm and several micrometers in size. The formation of few-layer TaS2 nanosheets as well as monolayer TaS2 sheets is further confirmed by atomic force microscopy images. The few-layer TaS2 nanosheets remain the 1T structure, whereas monolayer TaS2 sheets show lattice distortion and may adopt the 1H-like structure with trigonal prism coordination.

One-Step Synthesis of Titanium Oxyhydroxy-Fluoride Rods and Research on the Electrochemical Performance for Lithium-ion Batteries and Sodium-ion Batteries.

Titanium oxyhydroxy-fluoride, TiO0.9(OH)0.9F1.2 · 0.59H2O rods with a hexagonal tungsten bronze (HTB) structure, was synthesized via a facile one-step solvothermal method. The structure, morphology, and component of the products were characterized by X-ray powder diffraction (XRD), thermogravimetry (TG), scanning electron microscopy (SEM), transmission electron microscopy (TEM), high-resolution TEM (HRTEM), inductively coupled plasma optical emission spectroscopy (ICP-OES), ion chromatograph, energy-dispersive X-ray (EDX) analyses, and so on. Different rod morphologies which ranged from nanoscale to submicron scale were simply obtained by adjusting reaction conditions. With one-dimension channels for Li/Na intercalation/de-intercalation, the electrochemical performance of titanium oxyhydroxy-fluoride for both lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) was also studied. Electrochemical tests revealed that, for LIBs, titanium oxyhydroxy-fluoride exhibited a stabilized reversible capacity of 200 mAh g(-1) at 25 mA g(-1) up to 120 cycles in the electrode potential range of 3.0-1.2 V and 140 mAh g(-1) at 250 mA g(-1) up to 500 cycles, especially; for SIBs, a high capacity of 100 mAh g(-1) was maintained at 25 mA g(-1) after 115 cycles in the potential range of 2.9-0.5 V.

Facile one-pot synthesis of polytypic CuGaS2 nanoplates.

CuGaS2 (CGS) nanoplates were successfully synthesized by one-pot thermolysis of a mixture solution of CuCl, GaCl3, and 1-dodecanethiol in noncoordinating solvent 1-octadecene. Their morphology, crystalline phase, and composition were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), powder X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), respectively. Crystalline structure analysis showed that the as-prepared CGS nanoplates were polytypic, in which the wurtzite phase was interfaced with zincblende domains. The growth process of CGS nanoplates was investigated. It was found that copper sulfide nanoplates were firstly formed and then the as-formed copper sulfide nanoplates gradually transformed to CGS nanoplates with proceeding of the reaction. The optical absorption of the as-synthesized CGS nanoplates was also measured and the direct optical bandgap was determined to be 2.24 eV.

Facile synthesis of AgInS2 hierarchical flowerlike nanoarchitectures composed of ultrathin nanowires.

In this work, AgInS(2) hierarchical flowerlike nanoarchitectures, which are composed of ultrathin nanowires, were synthesized by thermolysis of a mixed solution of AgNO(3), InCl(3)·4H(2)O and n-dodecanethiol at elevated temperature. The average diameter and length of the nanowires composing the nanoarchitectures can reach 5 nm and ∼300 nm, respectively. We investigated the growth process of the nanoarchitectures and the effects of reaction parameters by XRD, SEM and TEM. In particular, the use of InCl(3)·4H(2)O played a decisive role in the synthesis of the nanoarchitectures. Moreover, it was found that polyhedra formed in the initial reaction time, and then the nanowires grew on the facets of these polyhedra, which resulted in the nanoarchitectures. The reaction temperature and the concentration of metal salts could influence the size of the nanowires.