Controlled Fabrication of Metallic MoO2 Nanosheets towards High-Performance p-Type 2D Transistors.

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDCs) are extensively employed as channel materials in advanced electronic devices. The electrical contacts between electrodes and 2D semiconductors play a crucial role in the development of high-performance transistors. While numerous strategies for electrode interface engineering have been proposed to enhance the performance of n-type 2D transistors, upgrading p-type ones in a similar manner remains a challenge. In this work, significant improvements in a p-type WSe2 transistor are demonstrated by utilizing metallic MoO2 nanosheets as the electrode contact, which are controllably fabricated through physical vapor deposition and subsequent annealing. The MoO2 nanosheets exhibit an exceptional electrical conductivity of 8.4 × 104 S m‒1 and a breakdown current density of 3.3 × 106 A cm‒2. The work function of MoO2 nanosheets is determined to be ≈5.1 eV, making them suitable for contacting p-type 2D semiconductors. Employing MoO2 nanosheets as the electrode contact in WSe2 transistors results in a notable increase in the field-effect mobility to 92.0 cm2 V‒1 s‒1, which is one order of magnitude higher than the counterpart devices with conventional electrodes. This study not only introduces an intriguing 2D metal oxide to improve the electrical contact in p-type 2D transistors, but also offers an effective approach to fabricating all-2D devices.

Nucleation and Growth of Nanocrystals Investigated by In Situ Transmission Electron Microscopy.

Nanocrystals play a key role in the modern energy, catalysis, semiconductor, and biology industries due to their unique structures and performances. However, controllable fabrication of ideal nanocrystals with the desired structures and properties is still challenging, which needs a deep understanding of their nucleation and growth process. Here, the research on nucleation and growth of nanocrystals studied by in situ transmission electron microscopy (TEM) is reviewed, mainly focusing on the atomic migration dynamics, interface evolution, and structure transformation. In addition, the challenges in the study of nanocrystal growth by TEM are discussed and the perspective on the future development of advanced in situ TEM techniques is provided. It is hoped that the review can give a deep insight into the nanocrystal nucleation and growth process, and further contribute to the rational design and precise fabrication of high-performance functional nanocrystals.

Construction of the Heterostructure of NiPt Truncated Octahedral Nanoparticle/MoS2 and Its Interfacial Structure Evolution.

Interfacial atomic configuration plays a vital role in the structural stability and functionality of nanocomposites composed of metal nanoparticles (NPs) and two-dimensional semiconductors. In situ transmission electron microscope (TEM) provides a real-time technique to observe the interface structure at atomic resolution. Herein, we loaded bimetallic NiPt truncated octahedral NPs (TONPs) on MoS2 nanosheets and constructed a NiPt TONPs/MoS2 heterostructure. The interfacial structure evolution of NiPt TONPs on MoS2 was in situ investigated using aberration-corrected TEM. It was observed that some NiPt TONPs exhibited lattice matching with MoS2 and displayed remarkable stability under electron beam irradiation. Intriguingly, the rotation of an individual NiPt TONP can be triggered by the electron beam to match the MoS2 lattice underneath. Furthermore, the coalescence kinetics of NiPt TONPs can be quantitatively described by the relationship between neck radius (r) and time (t), expressed as rn = Kt. Our work offers a detailed analysis of the lattice alignment relationship of NiPt TONPs on MoS2, which may enlighten the design and preparation of stable bimetallic metal NPs/MoS2 heterostructures.

Atomic-Scale Structure Dynamics of Nanocrystals Revealed By In Situ and Environmental Transmission Electron Microscopy.

Nanocrystals are of great importance in material sciences and industry. Engineering nanocrystals with desired structures and properties is no doubt one of the most important challenges in the field, which requires deep insight into atomic-scale dynamics of nanocrystals during the process. The rapid developments of in situ transmission electron microscopy (TEM), especially environmental TEM, reveal insights into nanocrystals to digest. According to the considerable progress based on in situ electron microscopy, a comprehensive review on nanocrystal dynamics from three aspects: nucleation and growth, structure evolution, and dynamics in reaction conditions are given. In the nucleation and growth part, existing nucleation theories and growth pathways are organized based on liquid and gas-solid phases. In the structure evolution part, the focus is on in-depth mechanistic understanding of the evolution, including defects, phase, and disorder/order transitions. In the part of dynamics in reaction conditions, solid-solid and gas-solid interfaces of nanocrystals in atmosphere are discussed and the structure-property relationship is correlated. Even though impressive progress is made, additional efforts are required to develop the integrated and operando TEM methodologies for unveiling nanocrystal dynamics with high spatial, energy, and temporal resolutions.

Growth of few-layer WTe2 by a salt-assisted double-tube chemical vapor deposition method with high infrared photosensitivity.

WTe2, as a member of Weyl semimetals, is a vital candidate for the development of broad-wavelength-range photodetectors. At present, the preparation of WTe2 films mainly depends on the chemical vapor deposition (CVD) method. However, the chemical reactivity between W and Te is low, and the controllable synthesis of large-sized layered WTe2 in a stoichiometric ratio is the main challenge for further research. Here, we propose a salt-assisted double-tube CVD method for the one-step preparation of high-quality and large-size WTe2 crystals with a monolayer and few layers. The thickness and lateral dimension of WTe2 crystals can be effectively tuned by the growth temperature and hydrogen concentration, and the dynamic growth mechanism is understood by the combination of surface reaction and mass transport. Furthermore, a high-performance photodetector based on WTe2 is fabricated, which has high responsivity of 118 mA W-1 (1550 nm) and 408 mA W-1 (2700 nm) at room temperature, indicating its great potential for application in infrared optoelectronic devices. The results provide a reference for the preparation of 2D materials by CVD and lay the foundation for the fabrication of next-generation optoelectronic devices with a wide-wavelength-range response.

Atom-Resolved Investigation on Dynamic Nucleation and Growth of Platinum Nanocrystals.

Understanding the mechanism of nucleation and growth of nanocrystals is crucial for designing and regulating the structure and properties of nanocrystals. However, the process from molecules to nanocrystals remains unclear because of the rapid and complicated dynamics of evolution under reaction conditions. Here, the complete evolution process of solid-phase chloroplatinic acid during the electron beam irradiation triggered reduction and nucleation of platinum nanocrystals is recorded. Aberration-corrected environmental transmission electron microscopy is used for direct visualization of the dynamic evolution from H2 PtCl6 to Pt nanocrystals at the atomic scale, including the formation and growth of amorphous clusters, crystallization, and growth of clusters, and the ripening of Pt nanocrystals. At the first two stages, there exists a critical size of ≈2.0 nm, which represents the start of crystallization. Crystallization from the center and density fluctuation are observed in the second stage of the crystallization of a few clusters with a size obviously larger than the critical size. The work provides valuable information to understand the kinetics of the early stage of nanocrystal nucleation and crystallization at atomic scale.

Planar Fully Stretchable Lithium-Ion Batteries Based on a Lamellar Conductive Elastomer.

Stretchable lithium-ion batteries (LIBs) have attracted great attention as a promising power source in the emerging field of wearable electronics. Despite the recent advances in stretchable electrodes, separators, and sealing materials, building stretchable full batteries remains a big challenge. Herein, a simple strategy to prepare stretchable electrodes and separators at the full battery scale is reported. Then, electrostatic spraying is used to make the anode and cathode on an elastic current collector. Finally, a polyvinylidene fluoride/thermoplastic polyurethane nanofiber separator is hot-sandwiched between the cathode and anode. The fabricated battery shows stable electrochemical performance during repeatable release-stretch cycles. In particular, a stable capacity of 6 mA•h/cm2 at the current rate of 0.5 C can be achieved for the fully stretchable LIB. More importantly, over 70% of the initial capacity can be maintained after 100 cycles with ∼150% stretch.

Probing Evolution of Local Strain at MoS2-Metal Boundaries by Surface-Enhanced Raman Scattering.

Strain usually exists in two-dimensional (2D) materials and devices, and its presence drastically modulates their properties. When 2D materials interface with noble metals, local strain and surface plasmon can couple at the metal-2D material boundaries, delivering a lot of intriguing phenomena. Current studies are mostly focused on the explanations of these strain-related phenomena based on a static point of view. Although strain can typically be relaxed in many environments, the time evolution of strain at metal-2D material interfaces remains largely unknown. In this work, we investigate the evolution of local strain at Ag-MoS2 boundaries by surface-enhanced Raman scattering. With the split of MoS2 Raman peaks as an indicator of local strain, it is found that the originally localized strain at Ag-MoS2 boundaries evolves and relaxes with time into a delocalized strain in MoS2 plane. The time to start the strain relaxation depends on the number of layers of MoS2 flakes, suggesting that the relaxation may result from the mechanical instability of the interface between the topmost MoS2 layer and the underlying materials. The relaxation occurs in a certain period of time, i.e., ∼70 days for 1L and ∼30 days for 3L. Accompanying the strain relaxation, surface sulfurization of Ag also occurs, a process that reduces the strength of locally enhanced electric field. Our results not only provide a deep understanding of strain evolution at metal-MoS2 interfaces but also shed light on the optimization of MoS2-based device fabrications.