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- ItemHigh-Quality Graphene Using Boudouard Reaction(Weinheim : Wiley-VCH, 2022) Grebenko, Artem K.; Krasnikov, Dmitry V.; Bubis, Anton V.; Stolyarov, Vasily S.; Vyalikh, Denis V.; Makarova, Anna A.; Fedorov, Alexander; Aitkulova, Aisuluu; Alekseeva, Alena A.; Gilshtein, Evgeniia; Bedran, Zakhar; Shmakov, Alexander N.; Alyabyeva, Liudmila; Mozhchil, Rais N.; Ionov, Andrey M.; Gorshunov, Boris P.; Laasonen, Kari; Podzorov, Vitaly; Nasibulin, Albert G.Following the game-changing high-pressure CO (HiPco) process that established the first facile route toward large-scale production of single-walled carbon nanotubes, CO synthesis of cm-sized graphene crystals of ultra-high purity grown during tens of minutes is proposed. The Boudouard reaction serves for the first time to produce individual monolayer structures on the surface of a metal catalyst, thereby providing a chemical vapor deposition technique free from molecular and atomic hydrogen as well as vacuum conditions. This approach facilitates inhibition of the graphene nucleation from the CO/CO2 mixture and maintains a high growth rate of graphene seeds reaching large-scale monocrystals. Unique features of the Boudouard reaction coupled with CO-driven catalyst engineering ensure not only suppression of the second layer growth but also provide a simple and reliable technique for surface cleaning. Aside from being a novel carbon source, carbon monoxide ensures peculiar modification of catalyst and in general opens avenues for breakthrough graphene-catalyst composite production.
- ItemTowards the Growth of Hexagonal Boron Nitride on Ge(001)/Si Substrates by Chemical Vapor Deposition(Basel : MDPI, 2022) Franck, Max; Dabrowski, Jaroslaw; Schubert, Markus Andreas; Wenger, Christian; Lukosius, MindaugasThe growth of hexagonal boron nitride (hBN) on epitaxial Ge(001)/Si substrates via high-vacuum chemical vapor deposition from borazine is investigated for the first time in a systematic manner. The influences of the process pressure and growth temperature in the range of 10−7–10−3 mbar and 900–980 °C, respectively, are evaluated with respect to morphology, growth rate, and crystalline quality of the hBN films. At 900 °C, nanocrystalline hBN films with a lateral crystallite size of ~2–3 nm are obtained and confirmed by high-resolution transmission electron microscopy images. X-ray photoelectron spectroscopy confirms an atomic N:B ratio of 1 ± 0.1. A three-dimensional growth mode is observed by atomic force microscopy. Increasing the process pressure in the reactor mainly affects the growth rate, with only slight effects on crystalline quality and none on the principle growth mode. Growth of hBN at 980 °C increases the average crystallite size and leads to the formation of 3–10 well-oriented, vertically stacked layers of hBN on the Ge surface. Exploratory ab initio density functional theory simulations indicate that hBN edges are saturated by hydrogen, and it is proposed that partial de-saturation by H radicals produced on hot parts of the set-up is responsible for the growth.
- ItemHeteroepitaxy of group IV materials for future device application(Bristol : IOP Publ., 2023) Yamamoto, Yuji; Wen, Wei-Chen; Tillack, BerndHeteroepitxy of group IV materials (Si, SiGe, and Ge) has great potential for boosting Si-based novel device performance because of the possibility for strain, band gap/Fermi-level engineering, and applying emerging artificial materials such as a superlattice (SL) and nanodots. In order to control group IV heteroepitaxy processes, strain, interface, and surface energies are very essential parameters. They affect dislocation formation, interface steepness, reflow of deposited layers, and also surface reaction itself during the growth. Therefore, process control and crystallinity management of SiGe heteroepitaxy are difficult especially in the case of high Ge concentrations. In this paper, we review our results of abrupt SiGe/Si interface fabrication by introducing C-delta layers and the influence of strain on the surface reaction of SiGe. Three-dimensional self-ordered SiGe and Ge nanodot fabrication by proactively using strain and surface energies by depositing SiGe/Si and Ge/SiGe SL are also reviewed.
- ItemVertical alignment control of self-ordered multilayered Ge nanodots on SiGe(Bristol : IOP Publ., 2023) Wen, Wei-Chen; Schubert, Markus Andreas; Tillack, Bernd; Yamamoto, YujiSelf-ordered multilayered Ge nanodots with SiGe spacers on a Si0.4Ge0.6 virtual substrate are fabricated using reduced-pressure chemical vapor deposition, and the mechanism of vertical ordering is investigated. The process conditions of Ge and SiGe layer deposition are H2-GeH4 at 550 °C and H2-SiH4-GeH4 at 500 °C-550 °C, respectively. By depositing the SiGe at 550 °C or increasing Ge content, the SiGe surface becomes smooth, resulting in vertically aligned Ge nanodots to reduce strain energy. Ge nanodots prefer to grow on the nanodot where the SiGe is relatively tensile strained due to the buried Ge nanodot underneath. By depositing at 500 °C and lowering Ge content, checkerboard-like surface forms, and the following Ge nanodots grow at staggered positions to reduce surface energy. The Ge nanodots are laterally aligned along the elastically soft 〈100〉 direction without pre-structuring resulting from the strain distribution.
- ItemEngineering grain boundaries at the 2D limit for the hydrogen evolution reaction([London] : Nature Publishing Group UK, 2020) He, Yongmin; Tang, Pengyi; Hu, Zhili; He, Qiyuan; Zhu, Chao; Wang, Luqing; Zeng, Qingsheng; Golani, Prafful; Gao, Guanhui; Fu, Wei; Huang, Zhiqi; Gao, Caitian; Xia, Juan; Wang, Xingli; Wang, Xuewen; Zhu, Chao; Ramasse, Quentin M.; Zhang, Ao; An, Boxing; Zhang, Yongzhe; Martí-Sánchez, Sara; Morante, Joan Ramon; Wang, Liang; Tay, Beng Kang; Yakobson, Boris I.; Trampert, Achim; Zhang, Hua; Wu, Minghong; Wang, Qi Jie; Arbiol, Jordi; Liu, ZhengAtom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~1012 cm−2. We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec−1), thus indicating an intrinsically high activation of the TMD GBs.
- ItemHigh-performance electronics and optoelectronics of monolayer tungsten diselenide full film from pre-seeding strategy(Weinheim : Wiley, 2021) Zhang, Shu; Pang, Jinbo; Cheng, Qilin; Yang, Feng; Chen, Yu; Liu, Yu; Li, Yufen; Gemming, Thomas; Liu, Xiaoyan; Ibarlucea, Bergoi; Yang, Jiali; Liu, Hong; Zhou, Weijia; Cuniberti, Gianaurelio; Rümmeli, Mark H.Tungsten diselenide (WSe2) possesses extraordinary electronic properties for applications in electronics, optoelectronics, and emerging exciton physics. The synthesis of monolayer WSe2 film is of topmost for device arrays and integrated circuits. The monolayer WSe2 film has yet been reported by thermal chemical vapor deposition (CVD) approach, and the nucleation mechanism remains unclear. Here, we report a pre-seeding strategy for finely regulating the nuclei density at an early stage and achieving a fully covered film after chemical vapor deposition growth. The underlying mechanism is heterogeneous nucleation from the pre-seeding tungsten oxide nanoparticles. At first, we optimized the precursor concentration for pre-seeding. Besides, we confirmed the superiority of the pre-seeding method, compared with three types of substrate pretreatments, including nontreatment, sonication in an organic solvent, and oxygen plasma. Eventually, the high-quality synthetic WSe2 monolayer film exhibits excellent device performance in field-effect transistors and photodetectors. We extracted thermodynamic activation energy from the nucleation and growth data. Our results may shed light on the wafer-scale production of homogeneous monolayer films of WSe2, other 2D materials, and their van der Waals heterostructures.
- ItemSubstrate Developments for the Chemical Vapor Deposition Synthesis of Graphene(Weinheim : Wiley-VCH Verlag, 2020) Shi, Q.; Tokarska, K.; Ta, H.Q.; Yang, X.; Liu, Y.; Ullah, S.; Liu, L.; Trzebicka, B.; Bachmatiuk, A.; Sun, J.; Fu, L.; Liu, Z.; Rümmeli, M.H.Since the isolation of graphene and numerous demonstrations of its unique properties, the expectations for this material to be implemented in many future commercial applications have been enormous. However, to date, challenges still remain. One of the key challenges is the fabrication of graphene in a manner that satisfies processing requirements. While transfer of graphene can be used, this tends to damage or contaminate it, which degrades its performance. Hence, there is an important drive to grow graphene directly over a number of technologically important materials, viz., different substrate materials, so as to avoid the need for transfer. One of the more successful approaches to synthesis graphene is chemical vapor deposition (CVD), which is well established. Historically, transition metal substrates are used due to their catalytic properties. However, in recent years this has developed to include many nonmetal substrate systems. Moreover, both solid and molten substrate forms have also been demonstrated. In addition, the current trend to progress flexible devices has spurred interest in graphene growth directly over flexible materials surfaces. All these aspects are presented in this review which presents the developments in available substrates for graphene fabrication by CVD, with a focus primarily on large area graphene.