The ability to synthesize high-quality samples over large areas and at low cost is one of the biggest challenges during the developmental stage of any novel material. While chemical vapor deposition (CVD) methods provide a promising low-cost route for CMOS compatible, large-scale growth of materials, it often falls short of the high-quality demands in nanoelectronics and optoelectronics. We present large-scale CVD synthesis of single- and few-layered MoS2 using direct vapor-phase sulfurization of MoO2, which enables us to obtain extremely high-quality single-crystal monolayer MoS2 samples with field-effect mobility exceeding 30 cm(2)/(V s) in monolayers. These samples can be readily synthesized on a variety of substrates, and demonstrate a high-degree of optoelectronic uniformity in Raman and photoluminescence mapping over entire crystals with areas exceeding hundreds of square micrometers. Because of their high crystalline quality, Raman spectroscopy on these samples reveal a range of multiphonon processes through peaks with equal or better clarity compared to past reports on mechanically exfoliated samples. This enables us to investigate the layer thickness and substrate dependence of the extremely weak phonon processes at 285 and 487 cm(-1) in 2D-MoS2. The ultrahigh, optoelectronic-grade crystalline quality of these samples could be further established through photocurrent spectroscopy, which clearly reveal excitonic states at room temperature, a feat that has been previously demonstrated only on samples which were fabricated by micro-mechanical exfoliation and then artificially suspended across trenches. Our method reflects a big step in the development of atomically thin, 2D-MoS2 for scalable, high-quality optoelectronics.

Heterocrystals: rotationally oriented stacks of incommensurate 2D materials with tunable and laser-reconfigurable properties.

Bismuth selenide (Bi2Se3) is a 3D topological insulator, its strong spin-orbit coupling resulting in the well-known topologically protected coexistence of gapless metallic surface states and semiconducting bulk states with a band gap, Eg ≃ 300 meV. A fundamental question of considerable importance is how the electronic properties of this material evolve under nanoscale confinement. We report on catalyst-free, high-quality single-crystalline Bi2Se3 with controlled lateral sizes and layer thicknesses that could be tailored down to a few nanometers and a few quintuple layers (QLs), respectively. Energy-resolved photoabsorption spectroscopy (1.5 eV < E(photon) < 6 eV) of these samples reveals a dramatic evolution of the photon absorption spectra as a function of size, transitioning from a featureless metal-like spectrum in the bulk (corresponding to a visually gray color), to one with a remarkably large band gap (Eg ≥ 2.5 eV) and a spectral shape that correspond to orange-red colorations in the smallest samples, similar to those seen in semiconductor nanostructures. We analyze this colorful transition using ab initio density functional theory and tight-binding calculations which corroborate our experimental findings and further suggest that while purely 2D sheets of few QL-thick Bi2Se3 do exhibit small band gaps that are consistent with previous ARPES results, the presently observed large gaps of a few electronvolts can only result from a combined effect of confinement in all three directions.

Atomically thin quaternary alloy of boron, nitrogen, carbon and oxygen, 2D-BNCO with tunable composition.

Bi2Se3 is a well-known room temperature topological insulator with a gapless surface state and ∼300 meV bulk band-gap, and as such has never been proposed to possess light-emitting properties. Here, we report prominent light emission in the visible region via photoluminescence (PL) measurements of chemical vapor deposition grown Bi2Se3 nanoplates with an average thickness and effective diameter of tens of nanometers. When excited using 488 nm (2.54 eV) laser light, these nanoscale Bi2Se3 platelets show a strong photoluminescence response in the Eph ∼ 2.1–2.3 eV region, with significant enhancement of light emission compared to bulk level emission. After annealing samples at 200 °C for 4 h, PL intensity increased by a factor of 2.4 to 3 for nanoscale Bi2Se3.