From structure to surface tension of small silicon clusters by Quantum Monte Carlo simulations

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-05-10 DOI:10.1016/j.susc.2024.122507
B.G.A. Brito , G.-Q. Hai , L. Cândido
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Abstract

We investigate the structural, surface and electronic properties of small silicon clusters Sin (for n=2 to 15) using HF, DFT and FN-DMC calculations. We analyze the atomic configurations, surface properties and electronic structures and show that the radius and average surface area of the clusters can be modeled by a Jellium-type model. We found that the surface tension σ of the clusters decreases with increasing cluster size in the range of the clusters under investigation. An estimate of the surface tension for bulk silicon yields σbulk=0.88(3) J/m2 in agreement with recent experiments. The average bond length of the clusters shows a non-monotonic behavior. Smaller clusters exhibit a high spin state influenced by electron correlation, especially during the 2D to 3D structural transition, which occurs at n=4 to n=5. We also find that the Si4, Si10 and Si12 clusters exhibit enhanced stability due to electron correlation. Our results are consistent with the experiments on bond length, binding energy and dissociation energy.

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通过量子蒙特卡洛模拟研究小硅团簇的结构和表面张力
我们利用高频、DFT 和 FN-DMC 计算研究了小硅团簇 Sin(n=2 至 15)的结构、表面和电子特性。我们分析了原子构型、表面性质和电子结构,结果表明硅团簇的半径和平均表面积可以用 Jellium 型模型来模拟。我们发现,在所研究的团簇范围内,团簇的表面张力 σ 随着团簇尺寸的增大而减小。根据对硅块表面张力的估算,σbulk=0.88(3) J/m2,这与最近的实验结果一致。硅簇的平均键长显示出一种非单调行为。较小的硅簇表现出受电子相关性影响的高自旋状态,尤其是在 n=4 到 n=5 的二维到三维结构转变期间。我们还发现,由于电子相关,Si4、Si10 和 Si12 簇表现出更高的稳定性。我们的结果与有关键长、结合能和解离能的实验结果一致。
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来源期刊
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
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