Quantum nuclear motion in silicene: Assessing structural and vibrational properties through path-integral simulations

IF 4.3 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY
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Abstract

This paper explores the interplay between quantum nuclear motion and anharmonicity, which causes nontrivial effects on the structural and dynamical characteristics of silicene, a two-dimensional (2D) allotrope of silicon with interesting electronic and mechanical properties. Employing path-integral molecular dynamics (PIMD) simulations, we investigate the quantum delocalization of nuclei, unraveling its impact on the behavior of silicene at the atomic scale. Our study reveals that this delocalization induces significant deviations in the structural parameters of silicene, influencing in-plane surface area, bond lengths, angles, compressibility, and overall lattice dynamics. Through extensive simulations, we delve into the temperature-dependent behavior between 25 and 1200 K, unveiling the role of quantum nuclear fluctuations in dictating thermal expansion and phonon spectra. The extent of nuclear quantum effects is assessed by comparing results of PIMD simulations using an efficient tight-binding Hamiltonian, with those obtained from classical molecular dynamics simulations. The observed quantum effects showcase non-negligible deviations from classical predictions, emphasizing the need for accurate quantum treatments in understanding the material’s behavior at finite temperatures. At low T, the 2D compression modulus of silicene decreases by a 14% due to quantum nuclear motion. We compare the magnitude of quantum effects in this material with those in other related 2D crystalline solids, such as graphene and SiC monolayers.

Abstract Image

硅烯中的量子核运动:通过路径积分模拟评估结构和振动特性
硅烯是硅的二维(2D)异构体,具有有趣的电子和机械特性,本文探讨了量子核运动和非谐波之间的相互作用,这种相互作用对硅烯的结构和动力学特性产生了非同寻常的影响。利用路径积分分子动力学(PIMD)模拟,我们研究了原子核的量子外迁,揭示了它在原子尺度上对硅烯行为的影响。我们的研究发现,这种脱域会导致硅烯的结构参数发生显著偏差,影响面内表面积、键长、角度、可压缩性和整体晶格动力学。通过大量模拟,我们深入研究了 25 至 1200 K 之间随温度变化的行为,揭示了量子核波动在决定热膨胀和声子谱方面的作用。通过比较使用高效紧密结合哈密顿的 PIMD 模拟结果和经典分子动力学模拟结果,我们评估了核量子效应的程度。观察到的量子效应显示出与经典预测的不可忽略的偏差,强调了在有限温度下理解材料行为时精确量子处理的必要性。在低温下,由于量子核运动,硅烯的二维压缩模量降低了 14%。我们将这种材料的量子效应大小与其他相关二维晶体固体(如石墨烯和碳化硅单层)的量子效应大小进行了比较。
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来源期刊
Journal of Physics and Chemistry of Solids
Journal of Physics and Chemistry of Solids 工程技术-化学综合
CiteScore
7.80
自引率
2.50%
发文量
605
审稿时长
40 days
期刊介绍: The Journal of Physics and Chemistry of Solids is a well-established international medium for publication of archival research in condensed matter and materials sciences. Areas of interest broadly include experimental and theoretical research on electronic, magnetic, spectroscopic and structural properties as well as the statistical mechanics and thermodynamics of materials. The focus is on gaining physical and chemical insight into the properties and potential applications of condensed matter systems. Within the broad scope of the journal, beyond regular contributions, the editors have identified submissions in the following areas of physics and chemistry of solids to be of special current interest to the journal: Low-dimensional systems Exotic states of quantum electron matter including topological phases Energy conversion and storage Interfaces, nanoparticles and catalysts.
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