Solvent Exfoliation of Electronic-Grade, Two-Dimensional Black Phosphorus

Abstract

Solution dispersions of two-dimensional (2D) black phosphorus (BP), often referred to as phosphorene, are achieved by solvent exfoliation. These pristine, electronic-grade BP dispersions are produced with anhydrous, organic solvents in a sealed tip ultrasonication system, which circumvents BP degradation that would otherwise occur via solvated oxygen or water. Among conventional solvents, n-methyl-pyrrolidone (NMP) is found to provide stable, highly concentrated (~0.4 mg/mL) BP dispersions. Atomic force microscopy, scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy show that the structure and chemistry of solvent-exfoliated BP nanosheets are comparable to mechanically exfoliated BP flakes. Additionally, residual NMP from the liquid-phase processing suppresses the rate of BP oxidation in ambient conditions. Solvent-exfoliated BP nanosheet field-effect transistors (FETs) exhibit ambipolar behavior with current on/off ratios and mobilities up to ~10000 and ~50 cm^2/(V*s), respectively. Overall, this study shows that stable, highly concentrated, electronic-grade 2D BP dispersions can be realized by scalable solvent exfoliation, thereby presenting opportunities for large-area, high-performance BP device applications.

6 figures, 31 pages, including supporting information

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• Spin-orbit coupling and spin relaxation in phosphorene: Intrinsic versus extrinsic effects
• Single-step exfoliation and functionalization of few-layers black phosphorus and its application for polymer composites
• Nano-imaging of the edge-dependent optical polarization anisotropy of black phosphorus
• Monolayer black phosphorus by sequential wet-chemical surface oxidation
• Field-created diverse quantizations in phosphorenes
• Novel polystyrene-based nanocomposites by phosphorene dispersion
• Growth kinetics and atomistic mechanisms of native oxidation of ZrS${}_x$Se${}_{2-x}$ and MoS${}_2$ crystals
• Multiorbital edge and corner states in black phosphorene
• Electron spin dynamics of two-dimensional layered materials
• Lattice dynamics and elastic properties of black phosphorus
• H2 O incorporation in the phosphorene/a-SiO2 interface: A first-principles study