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- 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.
- 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.
- ItemLocal Structure Investigation of Cu Precipitates in Modified 18CrNiMo7-6 Steels by Synchrotron X-ray Absorption Spectroscopy(Tōkyō : ISIJ, 2022) Suwanpinij, Piyada; Bambach, Margarita; Bootchanont, Atipong; Sailuam, WutthigraiThis paper studied the copper precipitation in an 18CrNiMo7-6 martensitic steel (0.19 mass% C) with copper addition and its resulting improved mechanical behavior. The development of nano-precipitates in two modified alloys with 1.0 and 1.5 mass% copper addition was investigated by means of synchrotron X-ray absorption spectroscopy. The first-principles calculation has enabled the modeling of the unavailable copper standards: solid solution, B2, BCC, 2H, 9R and 3R, for calculating the XAS spectra and successfully identified the unknown phases after aging for the first time in this steel group. The samples alloyed with 1.5 mass% copper yielded the semi-coherent 9R structure when aged at 500°C between 166 to 360 minutes. The ones containing 1 mass% copper formed the B2 ordered structure after aging at 480°C for 50 minutes and revealed the co-existence of the 9R after 240 minutes. The analysis reveals the precipitation kinetics of copper in low carbon martensitic steel and helps determine the optimum tempering parameters to adjust peak strength.
- 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.
- ItemHeat accumulation during femtosecond laser treatment at high repetition rate – A morphological, chemical and crystallographic characterization of self-organized structures on Ti6Al4V(Amsterdam : Elsevier, 2021) Schnell, Georg; Lund, Henrik; Bartling, Stephan; Polley, Christian; Riaz, Abdullah; Senz, Volkmar; Springer, Armin; Seitz, HermannThis study presents a detailed characterization of self-organized nano- and microstructures on Ti6Al4V evoked by different scanning strategies and fluences with a 300 fs laser operating at a laser wavelength of 1030 nm. The resulting surface morphology was visualized via field emission scanning electron microscopy (FEG-SEM) images of the surface and cross-sections. X-ray diffraction (XRD)-analysis was performed to analyse changes in crystal structures. The chemical surface composition of the near-surface layer was determined by X-ray photoelectron spectroscopy (XPS). Results show a significant influence of heat accumulation while processing with high laser repetition rates on the formation, crystallinity and chemical composition of self-organized structures depending on the scanning strategy. The ablation with different laser scanning strategies led to varying dynamics of growth-mechanisms of self-organized structures, formation of intermetallic phases (Ti3Al), sub-oxides and oxides (Ti6O, TiO) as well as ions (Ti3+, Ti4+) in surface layer reliant on applied fluence. Furthermore, investigations revealed a heat-affected zone up to several micrometers in non-ablated material. © 2021 The Authors
- ItemSelf-organized formation of unidirectional and quasi-one-dimensional metallic Tb silicide nanowires on Si(110)(Amsterdam [u.a.] : Elsevier, 2022) Appelfeller, Stephan; Franz, Martin; Karadag, Murat; Kubicki, Milan; Zielinski, Robert; Krivenkov, Maxim; Varykhalov, Andrei; Preobrajenski, Alexei; Dähne, MarioTerbium induced nanostructures on Si(110) and their growth are thoroughly characterized by low energy electron diffraction, scanning tunneling microscopy and spectroscopy, core-level and valence band photoelectron spectroscopy, and angle-resolved photoelectron spectroscopy. For low Tb coverage, a wetting layer forms with its surface fraction continuously decreasing with increasing Tb coverage in favor of the formation of unidirectional Tb silicide nanowires. These nanowires show high aspect ratios for high annealing temperatures or on substrates already containing Tb in the bulk. Both wetting layer and nanowires are stable for temperatures up to 750°C. In contrast to the nanowires, the wetting layer is characterized by a band gap. Thus, the metallic nanowires, which show a quasi-one-dimensional electronic band structure, are embedded in a semiconducting surrounding of wetting layer and substrate, insulating the nanowires from each other.
- ItemSelf-stabilization of the equilibrium state in ferroelectric thin films(Amsterdam : Elsevier, 2022) Gaal, Peter; Schmidt, Daniel; Khosla, Mallika; Richter, Carsten; Boesecke, Peter; Novikov, Dmitri; Schmidbauer, Martin; Schwarzkopf, Jutta(K,Na)NbO3 is a lead-free and sustainable ferroelectric material with electromechanical parameters comparable to Pb(Zr,Ti)O3 (PZT) and other lead-based solid solutions. It is therefore a promising candidate for caloric cooling and energy harvesting applications. Specifically, the structural transition from the low-temperature Mc- to the high-temperature c-phase displays a rich hierarchical order of domains and superdomains, that forms at specific strain conditions. The relevant length scales are few tens of nanometers for the domain and few micrometers for the superdomain size, respectively. Phase-field calculations show that this hierarchical order adds to the total free energy of the solid. Thus, domains and their formation has a strong impact on the functional properties relevant for electrocaloric cooling or energy harvesting applications. However, monitoring the formation of domains and superdomains is difficult and requires both, high spatial and high temporal resolution of the experiment. Synchrotron-based time-resolved X-ray diffraction methods in combination with scanning imaging X-ray microscopy is applied to resolve the local dynamics of the domain morphology with sub-micrometer spatial and nanosecond temporal resolution. In this regime, the material displays a novel self-stabilization mechanism of the domain morphology, which may be a general property of first-order phase transitions.