Plasma-Driven Selenization for Electrical Property Enhancement in Janus 2D Materials.

The recent emergence of Janus 2D materials like SnSSe, derived from SnS2, reveals unique electrical and optical features, such as asymmetrical electronic structure, enhanced carrier mobility, and tunable bandgap. Previous theoretical studies have discuss the electronic properties of Janus SnSSe, but experimental evidence is limited. This study presents a two-step method for synthesizing Janus SnSSe, involving hydrogen plasma treatment and in situ selenization. Optimized conditions (38 W, 1.5 min, 250 °C) are determined using Raman spectroscopy and AFM analysis. XPS confirmed SnSSe's elemental composition, while KPFM reveals a significant reduction in the work function (from 5.26 down to 5.14 eV) for the first time, indicating asymmetrically induced n-type doping. Finally, field-effect transistors (FETs) derived from SnSSe exhibited significantly enhanced mobility and on-current, as well as n-type doping, compared to SnS2-based FETs. These findings lay a crucial foundation for developing high-performance 2D electronic and optoelectronic devices.

Spectroscopic and Electrical Characterizations of Low-Damage Phosphorous-Doped Graphene via Ion Implantation.

Development of n-/p-type semiconducting graphenes is a critical route to implement in graphene-based nanoelectronics and optronics. Compared to the p-type graphene, the n-type graphene is more difficult to be prepared. Recently, phosphorous doping was reported to achieve air-stable and high mobility of n-typed graphene. The phosphorous-doped graphene (P-Gra) by ion implantation is considered as an ideal method for tailoring graphene due to its IC compatible process; however, for a conventional ion implanter, the acceleration energy is in the order of kiloelectron volts (keV), thus severely destroys the sp2 bonding of graphene owing to its high energy of accelerated ions. The introduced defects, therefore, degrade the electrical performance of graphene. Here, for the first time, we report a low-damage n-typed chemical vapor deposition (CVD) graphene by an industrial-compatible ion implanter with an energy of 20 keV where the designed protection layer (thin Au film) covered on as-grown CVD graphene is employed to efficiently reduce defect formation. The additional post-annealing is found to heal the crystal defects of graphene. Moreover, this method allows transferring ultraclean and residue-free P-Gra onto versatile target substrates directly. The doping configuration, crystallinity, and electrical properties on P-Gra were comprehensively studied. The results indicate that the low-damaged P-Gra with a controllable doping concentration of up to 4.22 at % was achieved, which is the highest concentration ever recorded. The doped graphenes with tunable work functions (4.85-4.15 eV) and stable n-type doping while keeping high-carrier mobility are realized. This work contributes to the proof-of-concept for tailoring graphene or 2D materials through doping with an exceptional low defect density by the low energy ion implantation, suggesting a great potential for unconventional doping technologies for next-generation 2D-based nanoelectronics.

Nanocatalyst-Assisted Fine Tailoring of Pore Structure in Holey-Graphene for Enhanced Performance in Energy Storage.

Nanoporous holey-graphene (HG) shows potential versatility in several technological fields, especially in biomedical, water filtration, and energy storage applications. Particularly, for ultrahigh electrochemical energy storage applications, HG has shown promise in addressing the issue of low gravimetric and volumetric energy densities by boosting of the ion-transport efficiency in a high-mass-loaded graphene electrode. However, there are no studies showing complete control over the entire pore architecture and density of HG and their effect on high-rate energy storage. Here, we report a unique and cost-effective method for obtaining well-controlled HG, where a copper nanocatalyst assists the predefined porosity tailoring of the HG and leads to an extraordinary high pore density that exceeds 1 × 103 µm-2. The pore architectures of the hierarchical and homogenous pores of HG were realized through a rationally designed nanocatalyst and the annealing procedure in this method. The HG electrode with a high mass loading results in improved supercapacitor performance that is at least 1 order of magnitude higher than conventional graphene flakes (reduced electrochemically exfoliated graphene (rECG)) in areal capacitance (∼100% retention of capacitance until 15 000 cycles), energy density, and power density. The diffusion coefficient of the HG electrode is 1.5-fold higher than that of rECG at a mass loading of 15 mg cm-2, indicating excellent ion-transport efficiency. The excellent ion-transport efficiency of HG is further proved by nearly 4-fold magnitude lowering of its Rion (the ionic resistance in the electrolyte-filled pores) value as compared with rECG when estimated for equivalent high-mass-loaded electrodes. Furthermore, the HG exhibits a packing density that is 2 orders of magnitude higher than rECG, revealing the utility of the maximum electrode mass and possessing higher volumetric capacitance. The perfect tailoring of HG with optimized porosity allows the achievement of high areal capacitance and excellent cycling stability due to the facile ion- and charge-transport at high-mass-loaded electrodes, which could open a new avenue for addressing the long-existing issue of practical application of graphene-based energy storage devices.

Ultra-large suspended graphene as a highly elastic membrane for capacitive pressure sensors.

In this work, we fabricate ultra-large suspended graphene membranes, where stacks of a few layers of graphene could be suspended over a circular hole with a diameter of up to 1.5 mm, with a diameter to thickness aspect ratio of 3 × 10(5), which is the record for free-standing graphene membranes. The process is based on large crystalline graphene (∼55 µm) obtained using a chemical vapor deposition (CVD) method, followed by a gradual solvent replacement technique. Combining a hydrogen bubbling transfer approach with thermal annealing to reduce polymer residue results in an extremely clean surface, where the ultra-large suspended graphene retains the intrinsic features of graphene, including phonon response and an enhanced carrier mobility (200% higher than that of graphene on a substrate). The highly elastic mechanical properties of the graphene membrane are demonstrated, and the Q-factor under 2 MHz stimulation is measured to be 200-300. A graphene-based capacitive pressure sensor is fabricated, where it shows a linear response and a high sensitivity of 15.15 aF Pa(-1), which is 770% higher than that of frequently used silicon-based membranes. The reported approach is universal, which could be employed to fabricate other suspended 2D materials with macro-scale sizes on versatile support substrates, such as arrays of Si nano-pillars and deep trenches.