Search

New high-k gate dielectrics are highly necessary in facilitating the continuous down-scaling of metal–oxide–semiconductor devices to the sub-10 nm range. This study presents ultrathin organic hydrocarbon (HC) films as a novel high-k gate insulator for metal–insulator–semiconductor (MIS) devices. During inductively-coupled plasma chemical vapor deposition with CH4 and H2 gases, the growth temperature greatly affects the structure of the carbon layers and consequently their dielectric characteristics. Specifically, sp2-rich dielectric HC layers are formed below 600 °C, whereas highly-ordered sp2-hybridized graphene is formed at 950 °C. The k value of the resulting HC films increases up to a maximum value of 90 at 350 °C. Moreover, the MIS devices exhibit excellent gate-insulating properties, including almost no hysteresis in the capacitance–voltage curve, low leakage current, and high dielectric strength, which surpass those of existing high-k gate oxides. These results reveal that the organic HC films are a promising next-generation high-k gate dielectric material for sub-10 nm node Si and organic semiconductor technologies.

The growth of high-quality graphene on copper substrates has been intensively investigated using chemical vapor deposition (CVD). It, however, has been considered that the growth mechanism is different when graphene is synthesized using a plasma CVD. In this study, we demonstrate a dual role of hydrogen for the graphene growth on copper using an inductively coupled plasma (ICP) CVD. Hydrogen activates surface-bound carbon for the growth of high-quality monolayer graphene. In contrast, the role of an etchant is to manipulate the distribution of the graphene grains, which significantly depends on the plasma power. Atomic-resolution transmission electron microscopy study enables the mapping of graphene grains, which uncovers the distribution of grains and the number of graphene layers depending on the plasma power. In addition, the variation of electronic properties of the synthesized graphene relies on the plasma power.

Graphene-based two-dimensional heterostructures are of substantial interest both for fundamental studies and their various potential applications. Particularly interesting are atomically thin semiconducting oxides on graphene, which uniquely combine a wide band gap and optical transparency. Here, we report the atomic-scale investigation of a novel self-formation of a ZnO monolayer from the Zn metal on a graphene oxide substrate. The spontaneous oxidation of the ultrathin Zn metal occurs by a reaction with oxygen supplied from the graphene oxide substrate, and graphene oxide is deoxygenated by a transfer of oxygen from O-containing functional groups to the zinc metal. The ZnO monolayer formed by this spontaneous redox reaction shows a graphene-like structure and a band gap of about 4 eV. This study demonstrates a unique and straightforward synthetic route to atomically thin two-dimensional heterostructures made from a two-dimensional metal oxide and graphene, formed by the spontaneous redox reaction of a very thin metal layer directly deposited on graphene oxide.

Funder: Deutsche Forschungsgemeinschaft (German Research Foundation); doi: https://doi.org/10.13039/501100001659, Laser diodes are efficient light sources. However, state-of-the-art laser diode-based lighting systems rely on light-converting inorganic phosphor materials, which strongly limit the efficiency and lifetime, as well as achievable light output due to energy losses, saturation, thermal degradation, and low irradiance levels. Here, we demonstrate a macroscopically expanded, three-dimensional diffuser composed of interconnected hollow hexagonal boron nitride microtubes with nanoscopic wall-thickness, acting as an artificial solid fog, capable of withstanding ~10 times the irradiance level of remote phosphors. In contrast to phosphors, no light conversion is required as the diffuser relies solely on strong broadband (full visible range) lossless multiple light scattering events, enabled by a highly porous (>99.99%) non-absorbing nanoarchitecture, resulting in efficiencies of ~98%. This can unleash the potential of lasers for high-brightness lighting applications, such as automotive headlights, projection technology or lighting for large spaces.

Atomically thin semiconducting oxide on graphene carries a unique combination of wide band gap, high charge carrier mobility, and optical transparency, which can be widely applied for optoelectronics. However, study on the epitaxial formation and properties of oxide monolayer on graphene remains unexplored due to hydrophobic graphene surface and limits of conventional bulk deposition technique. Here, we report atomic scale study of heteroepitaxial growth and relationship of a single-atom-thick ZnO layer on graphene using atomic layer deposition. We demonstrate atom-by-atom growth of zinc and oxygen at the preferential zigzag edge of a ZnO monolayer on graphene through in situ observation. We experimentally determine that the thinnest ZnO monolayer has a wide band gap (up to 4.0 eV), due to quantum confinement and graphene-like structure, and high optical transparency. This study can lead to a new class of atomically thin two-dimensional heterostructures of semiconducting oxides formed by highly controlled epitaxial growth.

Over the past decade, nanostructuring has become the core of thermoelectric (TE) material research because it creates numerous internal interfaces that provide an effective way to tune the electrical and/or thermal properties of TE materials. Herein, we report a synthesis of interface-engineered BiSbTe nanostructured TE materials by introducing chemically synthesized molecular Ten2− polyanions into BiSbTe particles, from which BiSbTe nanostructured materials with high-density Te interfacial layers are prepared in thin films and sintered pellets. These Te layers form the contact potential well at the BiSbTe-Te junction to realize energy dependent carrier scattering and scatter phonons effectively, thus resulting in simultaneous improvement in the electrical and thermal properties to increase the ZT value well above 1.3 ± 0.14 that is increased by 40% compared to bulk BiSbTe. The findings of current study can open up new chemical design spaces for interface-engineered electronic and TE materials.

The polymer residue remaining on chemical-vapor-deposited graphene after its transfer to the substrate and subsequent lithographic patterning tends to cause problems such as decrease in electron mobility, and unwanted doping. In this study, by using a controllable low-energy Ar + ion beam (9.5 eV), the residue was cleaned perfectly without damaging the graphene surface. Further, a back-gate graphene field-effect transistor fabricated on the Ar + -ion-cleaned graphene surface showed about 4 times higher drain current than that showed by a similar transistor fabricated on pristine graphene. We believe that the technique used in this study can be useful in preventing the problems caused by the residue remaining on the graphene surface and can be applied not only to the processing of next-generation graphene-based electronics but also to other 2D materials-based electronic material processing.

There is an urgent need to develop metal-free, low cost, durable, and highly efficient catalysts for industrially important oxygen evolution reactions. Inspired by natural geodes, unique melamine nanogeodes are successfully synthesized using hydrothermal process. Sulfur-modified graphitic carbon nitride (S-modified g-CN x ) electrocatalysts are obtained by annealing these melamine nanogeodes in situ with sulfur. The sulfur modification in the g-CN x structure leads to excellent oxygen evolution reaction activity by lowering the overpotential. Compared with the previously reported nonmetallic systems and well-established metallic catalysts, the S-modified g-CN x nanostructures show superior performance, requiring a lower overpotential (290 mV) to achieve a current density of 10 mA cm−2 and a Tafel slope of 120 mV dec−1 with long-term durability of 91.2% retention for 18 h. These inexpensive, environmentally friendly, and easy-to-synthesize catalysts with extraordinary performance will have a high impact in the field of oxygen evolution reaction electrocatalysis.

Doping semiconductor nanocrystals with magnetic transition-metal ions has attracted fundamental interest to obtain a nanoscale dilute magnetic semiconductor, which has unique spin exchange interaction between magnetic spin and exciton. So far, the study on the doped semiconductor NCs has usually been conducted with NCs with larger than 2 nm because of synthetic challenges. Herein, we report the synthesis and characterization of Mn2+-doped (CdSe)(13) clusters, the smallest doped semiconductors. In this study, single-sized doped clusters are produced in large scale. Despite their small size, these clusters have semiconductor band structure instead of that of molecules. Surprisingly, the clusters show multiple excitonic transitions with different magneto-optical activities, which can be attributed to the fine structure splitting. Magneto-optically active states exhibit giant Zeeman splittings up to elevated temperatures (128 K) with large g-factors of 81(+/- 8) at 4 K. Our results present a new synthetic method for doped clusters and facilitate the understanding of doped semiconductor at the boundary of molecules and quantum nanostructure. Refereed/Peer-reviewed