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High-density semiconducting aligned carbon nanotube (A-CNT) arrays have been demonstrated with wafer-scale preparation of materials and have shown high performance in P-type field-effect transistors (FETs) and great potential for applications in future digital integrated circuits (ICs). However, high-performance N-type FETs (N-FETs) have not yet been implemented with A-CNTs, making development of complementary metal-oxide-semiconductor (CMOS) technology, a necessary component for modern digital ICs, impossible. In this work, we reveal the mechanism hindering the realization of A-CNT N-FETs contacted by low-work-function metals and develop corresponding solutions to promote the performance of N-FETs to that of P-type FETs (P-FETs). The fabricated scandium (Sc)-contacted A-CNT N-FET with a 100 nm gate length exhibits an on-state current (

A mechanistic understanding of interactions between atomically thin two-dimensional (2D) transition-metal dichalcogenides (TMDs) and their growth substrates is important for achieving the unidirectional alignment of nuclei and seamless stitching of 2D TMD domains and thus 2D wafers. In this work, we conduct a cross-sectional scanning transmission electron microscopy (STEM) study to investigate the atomic-scale nucleation and early stage growth behaviors of chemical vapor deposited monolayer (ML-) MoS

An in-depth understanding and precise controlling of grain boundary (GB) motion at the atomic scale are crucial for grain growth and recrystallization in polycrystalline materials. So far, the reported studies mainly focus on the GB motion in the ideal bicrystal system, while the atomic mechanisms of GB motion in polycrystals remain poorly understood. Herein, taking two-dimensional (2D) hexagonal boron nitride (h-BN) as a model system, we experimentally investigated the atomic-scale mechanisms of the GB motion in 2D polycrystals. Since GB motion is directly related to the GB structures, this article is organized following the configurations of GBs, which can be divided into straight (including symmetric and asymmetric GBs) and curved GBs. We revealed that (I) for symmetric GBs, the shear-coupled motion alone is insufficient to drive the continuous GB motion in polycrystalline materials, and GB sliding is also needed. (II) For asymmetric GBs, GB motion follows a defaceting-faceting process, in which dislocation reactions are crucial. (III) For curved GBs, shear-coupled GB motion (during grain shrinking) leads to grain rotation, and the rotation direction highly depends on the misorientation angles. (IV) Finally, we will discuss the characteristics of binary lattice h-BN and find that partial dislocations participate in the GB motion at high misorientation angles (>38°). Our results build up the framework of the atomic-scale mechanisms of the GB motion in 2D polycrystalline materials and will be instructive for technological applications such as grain growth and GB engineering.

A mechanistic understanding of the growth of multiply twinned nanoparticles (MTPs), such as decahedra (Dh) and icosahedra (Ih), is crucial for precisely controlled syntheses and applications. Despite previous successes, no consensus has been reached regarding the multiple competing growth pathways for MTPs proposed thus far, in part due to the lack of information about their nucleation and growth dynamics. Here, we used decahedral and icosahedral gold nanoparticles as a model system in conjunction with in situ liquid cell transmission electron microscopy (LCTEM) to investigate the nucleation and growth dynamics of MTPs in aqueous solution; two growth pathways were successfully identified: (A) nucleation-based layer-by-layer growth from a rounded multiply twinned seed and (B) the successive twinning and growth of tetrahedra. The LCTEM results enabled us to directly and conclusively identify the growth behaviors of intermediate products. The internal strain relaxation mechanisms and growth kinetics differ for the two pathways: in pathway A, a MTP grew by the opening and closing of re-entrant grooves at the twin boundaries, which was not found in pathway B. We also analyzed different MTP growth pathways from an energetic perspective and discussed how the preferred pathway (A or B) is related to factors, such as the initial seed yield and the size- and morphology-dependent formation of MTPs. Our results contextualize the current understanding of MTP formation mechanisms and provide insightful guidance for the precisely controlled synthesis of MTPs for practical applications.

In this work, the interlayer coupling dependent lithium intercalation induced phase transition in bilayer MoS2 (BL-MoS2) was investigated using an atomic-resolution annual dark-field scanning transmission electron microscope (ADF-STEM). It was revealed that the lithiation induced H → T' phase transition in BL-MoS2 strongly depended on the interlayer twist angle; i.e., the H → T' phase transition occurred in well-stacked H phase BL-MoS2 (with a twist angle of θt = 0°) but not for θt ≠ 0° BL-MoS2. The lithiated BL-MoS2 appeared in homophase stacking, either T'/T' or H/H (locally, no phase transformation) stacking, without any heterophase stacking such as H/T' or T'/H observed. This finding indicated the H → T' phase transition occurred via a domain-by-domain mode rather than layer-by-layer. Up to 15 types of stacking orders were experimentally identified locally in lithiated bilayer T'-MoS2, and the formation mechanism was attributed to the discrete interlayer translation with a unit step of (m/6a, n/6b) (m, n = 0, 1, 2, 3), where a and b were the primitive lattice vectors of T'-MoS2. Our experimental results were further corroborated by ab initio density functional theory (DFT) calculations, where the occurrence of different stacking orders can be quantitatively correlated with the variation of intercalated lithium contents into the BL-MoS2. The present study aids in the understanding of the phase transition mechanisms in atomically thin 2D transition metal dichalcogenides (TMDCs) and will also shed light on the precisely controlled phase engineering of 2D materials for memory applications.

We propose and fabricate solid-state nanopore devices that monolithically integrate solution-gated, vertical thin-film transistors (TFTs) inside the nanopores for charge-based sensing of translocating biomolecules. The TFTs consist of zinc oxide semiconductor channels and aluminum oxide gate dielectrics, which are both conformally deposited along the inner surfaces of the nanopores via atomic layer deposition. The resultant TFT channel lengths and nanopore diameters both reach the ∼10 nm range. In translocation experiments using λ-DNAs or bovine serum antibody (BSA) proteins, the TFT-nanopore devices demonstrate concurrent detection of the ion conductance blockade signals and modulation signals in the TFT electrical current. The TFT signals show opposite signs for the negatively charged DNAs and positively charged BSAs as well as staircase signal shapes that correspond to the folding and knotting of λ-DNAs. Further experiments under various electrical biases and solution ionic strengths show that the ion blockade signals and the TFT signals have different dependence upon these experimental conditions. The TFT signals are analyzed to be consistent with the field effect sensing of the biomolecular charge, and the induced mirror charge is estimated from the signal amplitudes. This study could be a step forward to achieve charge-based single-biomolecular technology for basic research as well as for biosensing applications. It may also stimulate the development of TFT technologies for conformal integration of semiconductor electronics at the front end of nanostructures.

A mechanistic understanding of the growth of multiply twinned nanoparticles (MTPs), such as decahedra (Dh) and icosahedra (Ih), is crucial for precisely controlled syntheses and applications. Despite previous successes, no consensus has been reached regarding the multiple competing growth pathways for MTPs proposed thus far, in part due to the lack of information about their nucleation and growth dynamics. Here, we used decahedral and icosahedral gold nanoparticles as a model system in conjunction with

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS2/WS2 bilayer with various stacking configurations, by optical two-color ultrafast pump–probe spectroscopy. Surprisingly, we found that the charge transfer is robust against varying interlayer twist angles and interlayer coupling strength, in time scale of ∼90 fs. Our observat...

Stacked transition-metal dichalcogenides on hexagonal boron nitride (h-BN) are platforms for high-performance electronic devices. However, such vertical stacks are usually constructed by the layer-by-layer polymer-assisted transfer of mechanically exfoliated layers. This inevitably causes interfacial contamination and device performance degradation. Herein, we develop a two-step, low-pressure chemical vapor deposition synthetic strategy incorporating the direct growth of monolayer h-BN on Au foil with the subsequent growth of MoS2. In such vertical stacks, the interactions between MoS2 and Au are diminished by the intervening h-BN layer, as evidenced by the appearance of photoluminescence in MoS2. The weakened interfacial interactions facilitate the transfer of the MoS2/h-BN stacks from Au to arbitrary substrates by an electrochemical bubbling method. Scanning tunneling microscope/spectroscopy characterization shows that the central h-BN layer partially blocks the metal-induced gap states in MoS2/h-BN/Au ...

Localized surface plasmon resonance (LSPR) of doped Si nanocrystals (NCs) is critical to the development of Si-based plasmonics. We now experimentally show that LSPR can be obtained from both B- and P-doped Si NCs in the mid-infrared region. Both experiments and calculations demonstrate that the Drude model can be used to describe the LSPR of Si NCs if the dielectric screening and carrier effective mass of Si NCs are considered. When the doping levels of B and P are similar, the LSPR energy of B-doped Si NCs is higher than that of P-doped Si NCs because B is more efficiently activated to produce free carriers than P in Si NCs. We find that the plasmonic coupling between Si NCs is effectively blocked by oxide at the NC surface. The LSPR quality factors of B- and P-doped Si NCs approach those of traditional noble metal NCs. We demonstrate that LSPR is an effective means to gain physical insights on the electronic properties of doped Si NCs. The current work on the model semiconductor NCs, i.e., Si NCs has important implication for the physical understanding and practical use of semiconductor NC plasmonics.

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS

Stacked transition-metal dichalcogenides on hexagonal boron nitride (h-BN) are platforms for high-performance electronic devices. However, such vertical stacks are usually constructed by the layer-by-layer polymer-assisted transfer of mechanically exfoliated layers. This inevitably causes interfacial contamination and device performance degradation. Herein, we develop a two-step, low-pressure chemical vapor deposition synthetic strategy incorporating the direct growth of monolayer h-BN on Au foil with the subsequent growth of MoS

Semiconducting single-walled carbon nanotubes (s-SWNTs) with diameters of 1.0–1.5 nm (with similar bandgap to crystalline silicon) are highly desired for nanoelectronics. Up to date, the highest reported content of s-SWNTs as-grown is ∼97%, which is still far below the daunting requirements of high-end applications. Herein, we report a feasible and green pathway to use H2O vapor to modulate the structure of the intermetallic W6Co7 nanocrystals. By using the resultant W6Co7 nanocatalysts with a high percentage of (1 0 10) planes as structural templates, we realized the direct growth of s-SWNT with the purity of ∼99%, in which ∼97% is (14,4) tubes (diameter 1.29 nm). H2O can also act as an environmentally friendly and facile etchant for eliminating metallic SWNTs, and the content of s-SWNTs was further improved to 99.8% and (14,4) tubes to 98.6%. High purity s-SWNTs with even bandgap determined by their uniform structure can be used for the exquisite applications in different fields.

Two-dimensional transition-metal dichalcogenide alloys have attracted intense attention due to their tunable band gaps. In the present work, photoluminescence, Raman scattering, and electrical transport properties of monolayer and few-layer molybdenum tungsten diselenide alloys (Mo1-xWxSe2, 0 ≤ x ≤ 1) are systematically investigated. The strong photoluminescence emissions from Mo1-xWxSe2 monolayers indicate composition-tunable direct band gaps (from 1.56 to 1.65 eV), while weak and broad emissions from the bilayers indicate indirect band gaps. The first-order Raman modes are assigned by polarized Raman spectroscopy. Second-order Raman modes are assigned according to its frequencies. As composition changes in Mo1-xWxSe2 monolayers and few layers, the out-of-plane A1g mode showed one-mode behavior, while B2g(1) (only observed in few layers), in-plane E2g(1), and all observed second-order Raman modes showed two-mode behaviors. Electrical transport measurement revealed n-type semiconducting transport behavior with a high on/off ratio (>10(5)) for Mo1-xWxSe2 monolayers.

We present the controlled synthesis of high-quality two-dimensional (2D) GaSe crystals on flexible transparent mica substrates via a facile van der Waals epitaxy method. Single- and few-layer GaSe nanoplates with the lateral size of up to tens of micrometers were produced. The orientation and nucleation sites of GaSe nanoplates were well-controlled. The 2D GaSe crystal-based photodetectors were demonstrated on both mechanically rigid SiO2/Si and flexible mica substrates. Efficient photoresponse was observed in 2D GaSe crystal devices on transparent flexible mica substrates, regardless of repeated bending with different radii. The controlled growth of 2D GaSe crystals with efficient photoresponsivity opens up opportunities for both fundamental aspects and new applications in photodetectors.

Fabrication of large-area clean graphene sheets is the first step toward the development of high-performance applications in surface chemistry and biotechnology as well as in high-mobility electronics. Here we demonstrate the clean transfer of graphene grown by chemical vapor deposition on Cu foil, with surface cleanness defined by transmission electron microscopy (TEM) in combination with Raman scattering on the same position of suspended graphene sheets. For clean graphene, the Raman spectra exhibit distinctive features that can explicitly discriminate from that of graphene covered with a thin layer of amorphous carbon such as residual poly(methyl methacrylate) (PMMA). By applying this technique to graphene sheets with various degrees of surface cleanness, we show that the quantitative characterization of the thickness of surface contaminants is possible based on multiple reflections and interference of light in samples.

Catalyst-free inner growth of single-wall carbon nanotubes has been directly realized and monitored by means of in situ high-resolution transmission electron microscopy, with particular attention paid to the evolution of the cap shape. The cap of a carbon nanotube is surprisingly found to be kept closed during the growing/shrinking process, and the cap shape evolves inhomogeneously with a few particular sites growing faster during the growth, while the cap of a carbon nanotube keeps a round shape during the shrinkage process. The closed cap should be specific for noncatalytic growth of carbon nanotubes. We infer, from the results above, the possible atomistic mechanism and how the carbon network can accommodate or release the carbon atoms during the growth/shrinkage of carbon nanotubes.