General low-temperature growth of two-dimensional nanosheets from layered and nonlayered materials.

Most of the current methods for the synthesis of two-dimensional materials (2DMs) require temperatures not compatible with traditional back-end-of-line (BEOL) processes in semiconductor industry (450 °C). Here, we report a general BiOCl-assisted chemical vapor deposition (CVD) approach for the low-temperature synthesis of 27 ultrathin 2DMs. In particular, by mixing BiOCl with selected metal powders to produce volatile intermediates, we show that ultrathin 2DMs can be produced at 280-500 °C, which are ~200-300 °C lower than the temperatures required for salt-assisted CVD processes. In-depth characterizations and theoretical calculations reveal the low-temperature processes promoting 2D growth and the oxygen-inhibited synthetic mechanism ensuring the formation of ultrathin nonlayered 2DMs. We demonstrate that the resulting 2DMs exhibit electrical, magnetic and optoelectronic properties comparable to those of 2DMs grown at much higher temperatures. The general low-temperature preparation of ultrathin 2DMs defines a rich material platform for exploring exotic physics and facile BEOL integration in semiconductor industry.

Ultimate low leakage and EOT of high-κdielectric using transferred metal electrode.

The increase of gate leakage current when the gate dielectric layer is thinned is a key issue for device scalability. For scaling down the integrated circuits, a thin gate dielectric layer with a low leakage current is essential. Currently, changing the dielectric layer material or enhancing the surface contact between the gate dielectric and the channel material is the most common way to reduce gate leakage current in devices. Herein, we report a technique of enhancing the surface contact between the gate dielectric and the metal electrode, that is constructing an Au/Al2O3/Si metal-oxide-semiconductor device by replacing the typical evaporated electrode/dielectric layer contact with a transferred electrode/high-κdielectric layer contact. The contact with a mild, non-invasive interface can ensure the intrinsic insulation of the dielectric layer. By applying 2-40 nm Al2O3as the dielectric layer, the current density-electrical field (J-E) measurement reveals that the dielectric leakage generated by the transferred electrode is less than that obtained by the typical evaporated electrode with a ratio of 0.3 × 101 âˆ¼ 5 × 106atVbias = 1 V. Furthermore, atJ = 1 mA cm-2, the withstand voltage can be raised by 100-102times over that of an evaporated electrode. The capacitance-voltage (C-V) test shows that the transferred metal electrode can efficiently scale the equivalent oxide layer thickness (EOT) to 1.58 nm, which is a relatively smaller value than the overall reported Si-based device's EOT. This finding successfully illustrates that the transferred electrode/dielectric layer's mild contact can balance the scaling of the gate dielectric layer with a minimal leakage current and constantly reduce the EOT. Our enhanced electrode/dielectric contact approach provides a straightforward and effective pathway for further scaling of devices in integrated circuits and significantly decreases the overall integrated circuit's static power consumption (ICs).

Phase-Selective Synthesis of Ultrathin FeTe Nanoplates by Controllable Fe/Te Atom Ratio in the Growth Atmosphere.

Phase controllable synthesis of 2D materials is of significance for tuning related electrical, optical, and magnetic properties. Herein, the phase-controllable synthesis of tetragonal and hexagonal FeTe nanoplates has been realized by a rational control of the Fe/Te ratio in a chemical vapor deposition system. Using density functional theory calculations, it has been revealed that with the change of the Fe/Te ratio, the formation energy of active clusters changes, causing the phase-controllable synthesis of FeTe nanoplates. The thickness of the obtained FeTe nanoplates can be tuned down to the 2D limit (2.8 nm for tetragonal and 1.4 nm for hexagonal FeTe). X-ray diffraction pattern, transmission electron microscopy, and high resolution scanning transmission electron microscope analyses exhibit the high crystallinity of the as-grown FeTe nanoplates. The two kinds of FeTe nanoflakes show metallic behavior and good electrical conductivity, featuring 8.44 × 104 S m-1 for 9.8 nm-thick tetragonal FeTe and 5.45 × 104 S m-1 for 7.6 nm-thick hexagonal FeTe. The study provides an efficient and convenient route for tailoring the phases of FeTe nanoplates, which benefits to study phase-sensitive properties, and may pave the way for the synthesis of other multiphase 2D nanosheets with controllable phases.

Dual-Carbon Electrode-Based High-Energy-Density Potassium-Ion Hybrid Capacitor.

Potassium-ion hybrid capacitors (KIHCs) have attracted growing attention due to the natural abundance and low cost of potassium. However, KIHCs are still limited by sluggish redox reaction kinetics in electrodes during the accommodation of large-sized K+. Herein, a starch-derived hierarchically porous nitrogen-doped carbon (SHPNC) anode and active carbon cathode were rationally designed for dual-carbon electrode-based KIHCs with high energy density. The hierarchical structure and rich doped nitrogen in the SHPNC anode result in a distensible interlayer space to buffer volume expansion during K+ insertion/extraction, offers more electrochemical active sites to achieve high specific capacity, and has highly efficient channels for fast ion/electron transports. The in situ Raman and ex situ TEM demonstrated a reversible electrochemical behavior of the SHPNC anode. Thus, the SHPNC anode delivers superior cycling stability and a high reversible capacity (310 mA h g-1 at 50 mA g-1). In particular, the KIHCs assembled by the SHPNC anode and commercial active carbon cathode can deliver a high energy density of 165 W h kg-1 at a current density of 50 mA g-1 and an ultra-long cycle life of 10,000 cycles at 1 A g-1 (calculated based on the total mass of the anode and cathode).

Chemical vapor deposition and temperature-dependent Raman characterization of two-dimensional vanadium ditelluride.

Recently, ultrathin two-dimensional (2D) metallic vanadium dichalcogenides have attracted widespread attention because of the charge density wave (CDW) phase transition and possible ferromagnetism. Herein, we report the synthesis and temperature-dependent Raman characterization of the 2D vanadium ditelluride (VTe2). The synthesis is done by atmospheric pressure chemical vapor deposition (APCVD) using vanadium chloride (VCl3) precursor on fluorphlogopite mica, sapphire, and h-BN substrates. A large area of the thin film with thickness ∼10 nm is grown on the hexagonal boron nitride (h-BN) substrate. Temperature-dependent Raman characterization of VTe2 is conducted from room temperature to 513 K. Remarkable changes of Raman modes at around 413 K are observed, indicating the structural phase transition.

Organic charge transfer complexes on graphene with ultrahigh near infrared photogain.

Photodetectors have widespread applications in fields including telecommunications, thermal imaging and bio-medical imaging. The photogating effect, arising from charge trapping at defects and/or interfaces, can have extremely high photoelectric gain which can be a benefit to high-sensitivity room temperature photodetection. Here, we introduce thin layered organic charge transfer complexes (CPXs) integrated on graphene transistors for the development of hybrid phototransistors with ultra-high photoresponsivity of ∼106 A W-1 in the near infrared (NIR) region at room temperature. Our study has demonstrated a graphene-organic CPX with a broadband photoresponse ranging from the visible to the NIR region. The high photoelectric gain was from the photogating effect at the graphene/CPX interface. In addition, the photoresponse properties of the graphene-organic CPX can be regulated by electrical gating of graphene.

Potential 2D Materials with Phase Transitions: Structure, Synthesis, and Device Applications.

Layered materials with phase transitions, such as charge density wave (CDW) and magnetic and dipole ordering, have potential to be exfoliated into monolayers and few-layers and then become a large and important subfamily of two-dimensional (2D) materials. Benefitting from enriched physical properties from the collective interactions, long-range ordering, and related phase transitions, as well as the atomic thickness yet having nondangling bonds on the surface, 2D phase-transition materials have vast potential for use in new-concept and functional devices. Here, potential 2D phase-transition materials with CDWs and magnetic and dipole ordering, including transition metal dichalcogenides, transition metal halides, metal thio/selenophosphates, chromium silicon/germanium tellurides, and more, are introduced. The structures and experimental phase-transition properties are summarized for the bulk materials and some of the obtained monolayers. In addition, recent experimental progress on the synthesis and measurement of monolayers, such as 1T-TaS2 , CrI3 , and Cr2 Ge2 Te6 , is reviewed.

Growth of two-dimensional materials on hexagonal boron nitride (h-BN).

With its atomically smooth surface yet no dangling bond, chemical inertness and high temperature sustainability, the insulating hexagonal boron nitride (h-BN) can be an ideal substrate for two-dimensional (2D) material growth and device measurement. In this review, research progress on the chemical growth of 2D materials on h-BN has been summarized, such as chemical vapor deposition and molecular beam epitaxy of graphene and various transition metal dichalcogenides. Further, stacking of the as-grown 2D materials relative to h-BN, thermal expansion matching between the deposited materials and h-BN, electrical property of 2D materials on h-BN have been discussed in detail.