Molybdenum disulfide is considered as one of the most promising two-dimensional semiconductors for electronic and optoelectronic device applications. So far, the charge transport in monolayer molybdenum disulfide is dominated by extrinsic factors such as charged impurities, structural defects and traps, leading to much lower mobility than the intrinsic limit. Here we develop a facile low-temperature thiol chemistry route to repair the sulfur vacancies and improve the interface, resulting in significant reduction of the charged impurities and traps. High mobility 480 cm 2 V À 1 s À 1 is achieved in backgated monolayer molybdenum disulfide field-effect transistors at room temperature. Furthermore, we develop a theoretical model to quantitatively extract the key microscopic quantities that control the transistor performances, including the density of charged impurities, short-range defects and traps. Our combined experimental and theoretical study provides a clear path towards intrinsic charge transport in two-dimensional dichalcogenides for future high-performance device applications.

Doping of low-dimensional graphitic materials, including graphene, graphene quantum dots and single-wall carbon nanotubes with nitrogen, sulfur or boron can significantly change their properties. We report that simple fluorination followed by annealing in a dopant source can superdope low-dimensional graphitic materials with a high level of N, S or B. The superdoping results in the following doping levels: (i) for graphene, 29.82, 17.55 and 10.79 at% for N-, S- and B-doping, respectively; (ii) for graphene quantum dots, 36.38 at% for N-doping; and (iii) for single-wall carbon nanotubes, 7.79 and 10.66 at% for N- and S-doping, respectively. As an example, the N-superdoping of graphene can greatly increase the capacitive energy storage, increase the efficiency of the oxygen reduction reaction and induce ferromagnetism. Furthermore, by changing the degree of fluorination, the doping level can be tuned over a wide range, which is important for optimizing the performance of doped low-dimensional graphitic materials.

The electrical performance of two dimensional transitional metal dichalcogenides (TMDs) is strongly influenced by the amount of structural defects inside. In this work, we provide an optical spectroscopic characterization approach to correlate the amount of structural defects and the electrical performance of WSe 2 devices. Low temperature photoluminescence (PL) spectra of electron beam lithography (EBL) processed WSe 2 presents a clear defect-induced PL emission due to excitons bound to defects, which would strongly degrade the electrical performance. By adopting an e-beam-free transfer-electrode technique, we are able to prepare backgated WSe 2 device with limited amount of defects. A maximum hole-mobility of about 200 cm 2 /Vs was achieved due to reduced scattering sources, which is the highest reported value among its type.This work would not only provide a versatile and nondestructive method to monitor the defects in TMDs, but also a new route to approach the room temperature phonon-limited mobility in high performance TMDs devices.

The widely used photodetector design based on atomically thin transition metal dichalcogenides (TMDs) has a lateral metal-TMD-metal junction with a fairly small, line shape photoresponsive active area at the TMD-electrode interface. Here, we report a highly efficient photodetector with extremely large photoresponsive active area based on a lateral junction of monolayer-bilayer WSe 2 . Impressively, the separation of the electron-hole pairs (excitons) extends onto the whole 1L-2L WSe 2 junction surface. The responsivity of the WSe 2 junction photodetector is over 3200 times higher than that of a monolayer WSe 2 device and leads to a highest external quantum efficiency of 256% due to the efficient carrier extraction. Unlike the TMD p-n junctions modulated by dual gates or localized doping, which require complex fabrication procedures, our study establishes a simple, controllable, and scalable method to improve the photodetection performance by maximizing the active area for current generation.

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Currently, the fundamental factors that control the oxygen reduction reaction (ORR) activity of graphene itself, in particular the dependence of the ORR activity on the number of exposed edge sites remain elusive, mainly due to limited synthesis routes of achieving small size graphene. In this work, the synthesis of low oxygen content (< 2.5±0.2 at %), few layer graphene nanosheets with lateral dimensions smaller than a few hundred nm was achieved using a combination of ionic liquid assisted grinding of high purity graphite coupled with sequential centrifugation. We show for the first time, that the graphene nanosheets possessing a plethora of edges exhibited considerably higher electron transfer numbers compared to the thicker graphene nanoplatelets. This enhanced ORR activity was accomplished by successfully exploiting the plethora of edges of the nanosized graphene as well as the efficient electron communication between the active edge sites and the electrode substrate. The graphene nanosheets were characterized by an onset potential of-0.13 V vs. Ag/AgCl and a current density of-3.85 mA/cm 2 at-1 V, which represent the best ORR performance ever achieved from an undoped carbon based catalyst. This work demonstrates how low oxygen content nanosized graphene synthesized by a simple route can considerably impact the ORR catalytic activity and hence it is of significance in designing and optimizing advanced metal-free ORR electrocatalysts.

Molybdenum disulfide (MoS ) and bismuth telluride (Bi Te ) are the two most common types of structures adopted by 2D chalcogenides. In view of their unique physical properties and structure, 2D chalcogenides have potential applications in various fields. However, the excellent properties of these 2D crystals depend critically on their crystal structures, where defects, cracks, holes, or even greater damage can be inevitably introduced during the preparation and transferring processes. Such defects adversely impact the performance of devices made from 2D chalcogenides and, hence, it is important to develop ways to intuitively and precisely repair these 2D crystals on the atomic scale, so as to realize high-reliability devices from these structures. Here, an in situ study of the repair of the nanopores in MoS and Bi Te is carried out under electron beam irradiation by transmission electron microscopy. The experimental conditions allow visualization of the structural dynamics of MoS and Bi Te crystals with unprecedented resolution. Real-time observation of the healing of defects at atomic resolution can potentially help to reproducibly fabricate and simultaneously image single-crystalline free-standing 2D chalcogenides. Thus, these findings demonstrate the viability of using an electron beam as an effective tool to precisely engineer materials to suit desired applications in the future.

Nanodiamonds are interesting materials from the point of view of their biocompatibility and their chemical, spectroscopic, and mechanical properties. Current synthetic methods for nanodiamonds involve harsh environments, which are potentially hazardous in addition to being expensive. We report a low-temperature (423 K) hydrothermal approach to form nanodiamonds by using graphene-oxide or nitrated polycyclic aromatic hydrocarbons (naphthalene, anthracene, phenanthrene, or pyrene) as a starting material. The reaction products contain single-crystalline or twinned nanodiamonds with average diameters in the 2–3 nm range. Theoretical calculations prove that, at the nanoscale, sub-4 nm nanodiamonds may adopt a structure that is more stable than graphene-oxide and nitrated polycyclic aromatic hydrocarbons. Our findings show that sp 2 carbon in the polycyclic aromatic precursor can be converted to sp 3 carbon under unexpectedly moderate temperature conditions by using nanoscale precursors and thus offer a low-temperature approach for the synthesis of sub-4 nm nanodiamonds.