Multicomponent Covalent Chemical Patterning of Graphene.

The chemical patterning of graphene is being pursued tenaciously due to exciting possibilities in electronics, catalysis, sensing, and photonics. Despite the intense efforts, spatially controlled, multifunctional covalent patterning of graphene has not been achieved. The lack of control originates from the inherently poor reactivity of the basal plane of graphene, which necessitates the use of harsh chemistries. Here, we demonstrate spatially resolved multicomponent covalent chemical patterning of single layer graphene using a facile and efficient method. Three different functional groups could be covalently attached to the basal plane in dense, well-defined patterns using a combination of lithography and a self-limiting variant of diazonium chemistry requiring no need for graphene activation. The layer thickness of the covalent films could be controlled down to 1 nm. This work provides a solid foundation for the fabrication of chemically patterned multifunctional graphene interfaces for device applications.

Understanding ambipolar transport in MoS2 field effect transistors: the substrate is the key.

2D materials offer a pathway for further scaling of CMOS technology. However, for this to become a reality, both n-MOS and p-MOS should be realized, ideally with the same (standard) material. In the specific case of MoS2 field effect transistors (FETs), ambipolar transport is seldom reported, primarily due to the phenomenon of Fermi level pinning (FLP). In this study we identify the possible sources of FLP in MoS2 FETs and resolve them individually. A novel contact transfer technique is used to transfer contacts on top of MoS2 flake devices that results in a significant increase in the hole branch of the transfer characteristics as compared to conventionally fabricated contacts. We hypothesize that the pinning not only comes from the contact-MoS2 interface, but also from the MoS2-substrate interface. We confirm this by shifting to an hBN substrate which leads to a 10 fold increase in the hole current compared to the SiO2 substrate. Furthermore, we analyse MoS2 FETs of different channel thickness on three different substrates, SiO2, hBN and Al2O3, by correlating the p-branch I ON/I OFF to the position of oxide defect band in these substrates. FLP from the oxide is reduced in the case of Al2O3 which enables us to observe ambipolar transport in a bilayer MoS2 FET. These results highlight that MoS2 is indeed an ambipolar material, and the absence of ambipolar transport in MoS2 FETs is strongly correlated to its dielectric environment and processing conditions.

Material-Selective Doping of 2D TMDC through AlxOy Encapsulation.

For the integration of two-dimensional (2D) transition metal dichalcogenides (TMDC) with high-performance electronic systems, one of the greatest challenges is the realization of doping and comprehension of its mechanisms. Low-temperature atomic layer deposition of aluminum oxide is found to n-dope MoS2 and ReS2 but not WS2. Based on electrical, optical, and chemical analyses, we propose and validate a hypothesis to explain the doping mechanism. Doping is ascribed to donor states in the band gap of AlxOy, which donate electrons or not, based on the alignment of the electronic bands of the 2D TMDC. Through systematic experimental characterization, incorporation of impurities (e.g., carbon) is identified as the likely cause of such states. By modulating the carbon concentration in the capping oxide, doping can be controlled. Through systematic and comprehensive experimental analysis, this study correlates, for the first time, 2D TMDC doping to the carbon incorporation on dielectric encapsulation layers. We highlight the possibility to engineer dopant layers to control the material selectivity and doping concentration in 2D TMDC.

Layer-controlled epitaxy of 2D semiconductors: bridging nanoscale phenomena to wafer-scale uniformity.

The rapid cadence of MOSFET scaling is stimulating the development of new technologies and accelerating the introduction of new semiconducting materials as silicon alternative. In this context, 2D materials with a unique layered structure have attracted tremendous interest in recent years, mainly motivated by their ultra-thin body nature and unique optoelectronic and mechanical properties. The development of scalable synthesis techniques is obviously a fundamental step towards the development of a manufacturable technology. Metal-organic chemical vapor deposition has recently been used for the synthesis of large area TMDs, however, an important milestone still needs to be achieved: the ability to precisely control the number of layers and surface uniformity at the nano-to micro-length scale to obtain an atomically flat, self-passivated surface. In this work, we explore various fundamental aspects involved in the chemical vapor deposition process and we provide important insights on the layer-dependence of epitaxial MoS2 film's structural properties. Based on these observations, we propose an original method to achieve a layer-controlled epitaxy of wafer-scale TMDs.