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- ItemGiant persistent photoconductivity in monolayer MoS2 field-effect transistors(London : Nature Publishing Group, 2021) George, A.; Fistul, M.V.; Gruenewald, M.; Kaiser, D.; Lehnert, T.; Mupparapu, R.; Neumann, C.; Hübner, U.; Schaal, M.; Masurkar, N.; Arava, L.M.R.; Staude, I.; Kaiser, U.; Fritz, T.; Turchanin, A.Monolayer transition metal dichalcogenides (TMD) have numerous potential applications in ultrathin electronics and photonics. The exposure of TMD-based devices to light generates photo-carriers resulting in an enhanced conductivity, which can be effectively used, e.g., in photodetectors. If the photo-enhanced conductivity persists after removal of the irradiation, the effect is known as persistent photoconductivity (PPC). Here we show that ultraviolet light (λ = 365 nm) exposure induces an extremely long-living giant PPC (GPPC) in monolayer MoS2 (ML-MoS2) field-effect transistors (FET) with a time constant of ~30 days. Furthermore, this effect leads to a large enhancement of the conductivity up to a factor of 107. In contrast to previous studies in which the origin of the PPC was attributed to extrinsic reasons such as trapped charges in the substrate or adsorbates, we show that the GPPC arises mainly from the intrinsic properties of ML-MoS2 such as lattice defects that induce a large number of localized states in the forbidden gap. This finding is supported by a detailed experimental and theoretical study of the electric transport in TMD based FETs as well as by characterization of ML-MoS2 with scanning tunneling spectroscopy, high-resolution transmission electron microscopy, and photoluminescence measurements. The obtained results provide a basis for the defect-based engineering of the electronic and optical properties of TMDs for device applications.
- ItemSelective control of molecule charge state on graphene using tip-induced electric field and nitrogen doping(London : Nature Publishing Group, 2019) Pham, Van Dong; Ghosh, Sukanya; Joucken, Frédéric; Pelaez-Fernandez, Mario; Repain, Vincent; Chacon, Cyril; Bellec, Amandine; Girard, Yann; Sporken, Robert; Rousset, Sylvie; Dappe, Yannick J.; Narasimhan, Shobhana; Lagoute, JérômeThe combination of graphene with molecules offers promising opportunities to achieve new functionalities. In these hybrid structures, interfacial charge transfer plays a key role in the electronic properties and thus has to be understood and mastered. Using scanning tunneling microscopy and ab initio density functional theory calculations, we show that combining nitrogen doping of graphene with an electric field allows for a selective control of the charge state in a molecular layer on graphene. On pristine graphene, the local gating applied by the tip induces a shift of the molecular levels of adsorbed molecules and can be used to control their charge state. Ab initio calculations show that under the application of an electric field, the hybrid molecule/graphene system behaves like an electrostatic dipole with opposite charges in the molecule and graphene sub-units that are found to be proportional to the electric field amplitude, which thereby controls the charge transfer. When local gating is combined with nitrogen doping of graphene, the charging voltage of molecules on nitrogen is greatly lowered. Consequently, applying the proper electric field allows one to obtain a molecular layer with a mixed charge state, where a selective reduction is performed on single molecules at nitrogen sites. © 2019, The Author(s).
- ItemReactive plasma cleaning and restoration of transition metal dichalcogenide monolayers(London : Nature Publishing Group, 2021) Marinov, Daniil; de Marneffe, Jean-François; Smets, Quentin; Arutchelvan, Goutham; Bal, Kristof M.; Voronina, Ekaterina; Rakhimova, Tatyana; Mankelevich, Yuri; El Kazzi, Salim; Nalin Mehta, Ankit; Wyndaele, Pieter-Jan; Heyne, Markus Hartmut; Zhang, Jianran; With, Patrick C.; Banerjee, Sreetama; Neyts, Erik C.; Asselberghs, Inge; Lin, Dennis; De Gendt, StefanThe cleaning of two-dimensional (2D) materials is an essential step in the fabrication of future devices, leveraging their unique physical, optical, and chemical properties. Part of these emerging 2D materials are transition metal dichalcogenides (TMDs). So far there is limited understanding of the cleaning of “monolayer” TMD materials. In this study, we report on the use of downstream H2 plasma to clean the surface of monolayer WS2 grown by MOCVD. We demonstrate that high-temperature processing is essential, allowing to maximize the removal rate of polymers and to mitigate damage caused to the WS2 in the form of sulfur vacancies. We show that low temperature in situ carbonyl sulfide (OCS) soak is an efficient way to resulfurize the material, besides high-temperature H2S annealing. The cleaning processes and mechanisms elucidated in this work are tested on back-gated field-effect transistors, confirming that transport properties of WS2 devices can be maintained by the combination of H2 plasma cleaning and OCS restoration. The low-damage plasma cleaning based on H2 and OCS is very reproducible, fast (completed in a few minutes) and uses a 300 mm industrial plasma etch system qualified for standard semiconductor pilot production. This process is, therefore, expected to enable the industrial scale-up of 2D-based devices, co-integrated with silicon technology.
- ItemSingle-atom catalytic growth of crystals using graphene as a case study(London : Nature Publishing Group, 2021) Yang, Xiaoqin; Liu, Yu; Ta, Huy Q.; Rezvani, Ehsan; Zhang, Yue; Zeng, Mengqi; Fu, Lei; Bachmatiuk, Alicja; Luo, Jinping; Liu, Lijun; Rümmeli, Mark H.Anchored Single-atom catalysts have emerged as a cutting-edge research field holding tremendous appeal for applications in the fields of chemicals, energy and the environment. However, single-atom-catalysts for crystal growth is a nascent field. Of the few studies available, all of them are based on state-of-the-art in situ microscopy investigations and computational studies, and they all look at the growth of monolayer graphene from a single-atom catalyst. Despite the limited number of studies, they do, collectively, represent a new sub-field of single-atom catalysis, namely single-atom catalytic growth of crystalline solids. In this review, we examine them on substrate-supported and as freestanding graphene fabrication, as well as rolled-up graphene, viz., single-walled carbon nanotubes (SWCNT), grown from a single atom. We also briefly discuss the catalytic etching of graphene and SWCNT’s and conclude by outlining the future directions we envision this nascent field to take.
- ItemSpatially controlled epitaxial growth of 2D heterostructures via defect engineering using a focused He ion beam(London : Nature Publishing Group, 2021) Heilmann, Martin; Deinhart, Victor; Tahraoui, Abbes; Höflich, Katja; Lopes, J. Marcelo J.The combination of two-dimensional (2D) materials into heterostructures enables the formation of atomically thin devices with designed properties. To achieve a high-density, bottom-up integration, the growth of these 2D heterostructures via van der Waals epitaxy (vdWE) is an attractive alternative to the currently mostly employed mechanical transfer, which is problematic in terms of scaling and reproducibility. Controlling the location of the nuclei formation remains a key challenge in vdWE. Here, a focused He ion beam is used to deterministically place defects in graphene substrates, which serve as preferential nucleation sites for the growth of insulating, 2D hexagonal boron nitride (h-BN). Therewith a mask-free, selective-area vdWE (SAvdWE) is demonstrated, in which nucleation yield and crystal quality of h-BN are controlled by the ion beam parameters used for defect formation. Moreover, h-BN grown via SAvdWE is shown to exhibit electron tunneling characteristics comparable to those of mechanically transferred layers, thereby lying the foundation for a reliable, high-density array fabrication of 2D heterostructures for device integration via defect engineering in 2D substrates.