Silicon oxide nanoparticles grown on graphite by co-deposition of the atomic constituents†

IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL
Steffen Friis Holleufer, Alfred T. Hopkinson, Duncan S. Sutherland, Zheshen Li, Jeppe V. Lauritsen, Liv Hornekaer and Andrew Cassidy
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Abstract

Nanoscale silicate dust particles are the most abundant refractory component observed in the interstellar medium and are thought to play a key role in catalysing the formation of complex organic molecules in the star forming regions of space. We present a method to synthesise a laboratory analogue of nanoscale silicate dust particles on highly oriented pyrolytic graphite (HOPG) substrates by co-deposition of the atomic constituents. The resulting nanoparticulate films are sufficiently thin and conducting to allow for surface science investigations, and are characterised here, in situ under UHV, using X-ray photoelectron spectroscopy, near-edge X-ray absorption atomic fine spectroscopy and scanning tunnelling microscopy, and, ex situ, using scanning electron microscopy. We compare SiOx film growth with and without the use of atomic O beams during synthesis and conclude that exposure of the sample to atomic O leads to homogeneous films of interconnected nanoparticle networks. The networks cover the graphite substrate and demonstrate superior thermal stability, up to 1073 K, when compared to oxides produced without exposure to atomic O. In addition, control over the flux of atomic O during growth allows for control of the average oxidation state of the film produced. Photoelectron spectroscopy measurements demonstrate that fully oxidised films have an SiO2 stoichiometry very close to bulk SiO2 and scanning tunnelling microscopy images show the basic cluster building unit to have a radius of approximately 2.5 nm. The synthesis of SiOx films with adjustable stoichiometry and suitable for surface science experiments that require conducting substrates will be of great interest to the astrochemistry community, and will allow for nanoscale-investigation of the chemical processes thought to be catalysed at the surface of dust grains in space.

Abstract Image

通过原子组分的共沉积在石墨上生长氧化硅纳米颗粒
纳米级硅酸盐尘埃颗粒是在星际介质中观测到的最丰富的难熔成分,被认为在催化空间恒星形成区域复杂有机分子的形成中起着关键作用。我们提出了一种通过原子成分共沉积在高取向热解石墨(HOPG)衬底上合成纳米级硅酸盐粉尘颗粒的实验室模拟方法。由此产生的纳米颗粒薄膜足够薄,并且导电,可以进行表面科学研究,并在这里进行表征,在特高压下,使用x射线光电子能谱,近边缘x射线吸收原子精细光谱和扫描隧道显微镜,并在非原位使用扫描电子显微镜。我们比较了在合成过程中使用原子O束和不使用原子O束的情况下SiOx薄膜的生长,并得出结论,将样品暴露于原子O会导致相互连接的纳米颗粒网络的均匀薄膜。该网络覆盖在石墨衬底上,与不暴露于O原子的氧化物相比,表现出优异的热稳定性,高达1073 K。此外,在生长过程中控制O原子的通量可以控制所生成薄膜的平均氧化状态。光电子能谱测量表明,完全氧化膜的SiO2化学计量学非常接近体SiO2,扫描隧道显微镜图像显示,基本团簇构建单元的半径约为2.5 nm。SiOx薄膜的合成具有可调节的化学计量,适合于需要导电衬底的表面科学实验,这将引起天体化学界的极大兴趣,并将允许对被认为是在太空尘埃颗粒表面催化的化学过程进行纳米级研究。
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来源期刊
Physical Chemistry Chemical Physics
Physical Chemistry Chemical Physics 化学-物理:原子、分子和化学物理
CiteScore
5.50
自引率
9.10%
发文量
2675
审稿时长
2.0 months
期刊介绍: Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.
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