Development of a reactor for the <i>in situ</i> monitoring of 2D materials growth on liquid metal catalysts, using synchrotron x-ray scattering, Raman spectroscopy, and optical microscopy

Saedi, Mehdi; Voogd, Jan; Sjardin, A; Manikas, Anastasios C.; Galiotis, Costas; Jankowski, Maciej; Renaud, Gilles; Porta, Francesco La; Konovalov, Oleg; Baarle, G. J. C. van; Groot, Irene M. N.

doi:10.1063/1.5110656

Cited by 25 publications

(43 citation statements)

References 34 publications

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“…The growth can be monitored in situ using X-ray-based techniques (Grazing-incidence X-ray diffraction (GIXD) and X-ray reflectivity (XRR)), Raman spectroscopy, and optical microscopy. 63 The reactor has a cylindrical shape with a wall consisting of X-ray-transparent beryllium. A quartz window is placed on top of the reactor providing optical access for the Raman spectroscopy and optical microscopy measurements (see below).…”

Section: Methodsmentioning

confidence: 99%

Real-Time Multiscale Monitoring and Tailoring of Graphene Growth on Liquid Copper

et al. 2021

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The synthesis of large, defect-free two-dimensional materials (2DMs) such as graphene is a major challenge toward industrial applications. Chemical vapor deposition (CVD) on liquid metal catalysts (LMCats) is a recently developed process for the fast synthesis of high-quality single crystals of 2DMs. However, up to now, the lack of in situ techniques enabling direct feedback on the growth has limited our understanding of the process dynamics and primarily led to empirical growth recipes. Thus, an in situ multiscale monitoring of the 2DMs structure, coupled with a real-time control of the growth parameters, is necessary for efficient synthesis. Here we report real-time monitoring of graphene growth on liquid copper (at 1370 K under atmospheric pressure CVD conditions) via four complementary in situ methods: synchrotron X-ray diffraction and reflectivity, Raman spectroscopy, and radiation-mode optical microscopy. This has allowed us to control graphene growth parameters such as shape, dispersion, and the hexagonal supra-organization with very high accuracy. Furthermore, the switch from continuous polycrystalline film to the growth of millimeter-sized defect-free single crystals could also be accomplished. The presented results have far-reaching consequences for studying and tailoring 2D material formation processes on LMCats under CVD growth conditions. Finally, the experimental observations are supported by multiscale modeling that has thrown light into the underlying mechanisms of graphene growth.

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Section: Methodsmentioning

confidence: 99%

Real-Time Multiscale Monitoring and Tailoring of Graphene Growth on Liquid Copper

et al. 2021

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“…We believe that the embedded structural motif is unique to liquid Cu graphene growth and speculate that it is key to understanding the special growth observed experimentally, where both high growth speeds and low defect densities can be obtained simultaneously. 7,19 A thorough analysis of this is a topic of our ongoing work. For example, we expect that barriers of the C precursor species to diffuse over the flake edge (Ehrlich-Schwöbel barrier) would be lowered in the embedded state.…”

Section: Discussionmentioning

confidence: 99%

Interface between graphene and liquid Cu from molecular dynamics simulations

Cingolani

Deimel

Köcher

et al. 2020

The Journal of Chemical Physics

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Controllable synthesis of defect-free graphene is crucial for applications since the properties of graphene are highly sensitive to any deviations from the crystalline lattice. We focus here on the emerging use of liquid Cu catalysts, which has high potential for fast and efficient industrial-scale production of high-quality graphene. The interface between graphene and liquid Cu is studied using force field and ab initio molecular dynamics, revealing a complete or partial embedding of finite-sized flakes. By analyzing flakes of different sizes we find that the size-dependence of the embedding can be rationalized based on the energy cost of embedding versus bending the graphene flake. The embedding itself is driven by the formation of covalent bonds between the under-coordinated edge C atoms and the liquid Cu surface, which is accompanied by a significant charge transfer. In contrast, the central flake atoms are located around or slightly above 3 Å from the liquid Cu surface and exhibit weak vdW-bonding and much lower charge transfer. The structural and electronic properties of the embedded state revealed in our work provides the atomicscale information needed to develop effective models to explain the special growth observed in experiments where various interesting phenomena such as flake self-assembly and rotational alignment, high growth speeds and low defect densities in the final graphene product have been observed.

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“…Specifically, the development of in situ characterization tools should allow better handling of graphene growth and consolidation that will undoubtedly lead to 2D films of better quality. 25 To tackle this substantial challenge, considerable efforts have been made towards the development of in situ metrology that provides direct atomicscale insights into reaction procedures under real time conditions.…”

Section: In Situ Characterization Of Graphene Growth On Liquid Metalsmentioning

confidence: 99%

“…However, in order to develop standard in situ characterization tools important changes to the design of the commercial reactors are required so as to accommodate satellite characterization equipment. One notable example of such an endeavour is the recent development of a CVD reactor for the specific purpose of investigating 2DMs on LMCat 25 that integrates a number of characterization tools such as Raman microscopy, X-rays and optical microscopy. All these techniques can operate simultaneously with the growth process (Fig.…”

Section: Reactor Design For the In Situ Characterization Of 2dm Growth On Lmcatmentioning

confidence: 99%

“…It is evident that in order to be able to intervene during 2DM CVD growth, real-time characterization techniques must be developed so as to become standard tools for every CVD reactor. [25][26][27][28] This review aims to shed light on the process-structure-property relationship that governs the fabrication of tailored 2DMs by liquid catalytic CVD. The term "process" describes the substrate preparation, catalytic activation and growth mechanisms of 2DM growth by CVD.…”

Section: Introductionmentioning

confidence: 99%

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Growth andin situcharacterization of 2D materials by chemical vapour deposition on liquid metal catalysts: a review

et al. 2021

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Development of a reactor for the in situ monitoring of 2D materials growth on liquid metal catalysts, using synchrotron x-ray scattering, Raman spectroscopy, and optical microscopy

Cited by 25 publications

References 34 publications

Real-Time Multiscale Monitoring and Tailoring of Graphene Growth on Liquid Copper

Real-Time Multiscale Monitoring and Tailoring of Graphene Growth on Liquid Copper

Interface between graphene and liquid Cu from molecular dynamics simulations

Growth andin situcharacterization of 2D materials by chemical vapour deposition on liquid metal catalysts: a review

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