论文标题

部分可观测时空混沌系统的无模型预测

Critical role of electron-phonon interactions in determining the relative stability of Boron Nitride polymorphs

论文作者

Paul, Shilpa, Gururajan, M. P., Bhattacharya, Amrita, Prasanna, T. R. S.

论文摘要

尽管有几项第一原则研究,但BN多晶型物的相对稳定性仍然存在争议。稳定的多晶型物在三次(C-BN)和六边形(H-BN)之间变化,具体取决于使用的范德华(VDW)分散近似。这些研究无法解释主要的实验结果,C-BN是稳定的,相对稳定性顺序以及H-BN和C-BN(大于150 MEV/公式单元)之间的较大能量差。在这项研究中,我们介绍了电子 - 音波相互作用(EPI)到BN多晶型物的总能量的贡献。这清楚地确定了C-BN是稳定的多晶型物,而与VDW近似无关。仅通过包括EPI贡献才能实现Ab Insif usive匹配,这是上述主要的实验结果。 EPI对总能量的贡献对化学键合(在$ sp^2 $键入$ sp^3 $键入的多晶型物上的分层)和晶体结构非常敏感。 EPI贡献的关键作用在$ sp^2 $键入的分层BN多晶型物中可见,其中它大于VDW的贡献。鉴于H-BN是一种原型的层次材料,以散装或2D形式,我们的结果具有更广泛的相关性,即,包括EPI校正以及VDW近似值,对于分层材料中的能量学研究至关重要。

Despite several first principles studies, the relative stability of BN polymorphs remains controversial. The stable polymorph varies between the cubic (c-BN) and hexagonal (h-BN) depending on the van der Waals (vdW) dispersion approximation used. These studies are unable to explain the main experimental results, c-BN is stable, the relative stability order and the large energy difference between h-BN and c-BN (greater than 150 meV/formula unit). In this study, we introduce contributions from electron-phonon interactions (EPI) to the total energy of BN polymorphs. This clearly establishes c-BN is the stable polymorph irrespective of the vdW approximation. Only by including EPI contributions do the ab initio results match, for the first time, the main experimental results mentioned above. The EPI contribution to the total energy is strongly sensitive to chemical bonding (approximately twice in $sp^2$-bonded layered over $sp^3$-bonded polymorphs) and to crystal structure. The crucial role of EPI contributions is seen in $sp^2$-bonded layered BN polymorphs where it is greater than the vdW contribution. Given that h-BN is a prototype layered material, in bulk or 2D form, our results have a broader relevance, that is, including EPI correction, along with vdW approximation, is vital for the study of energetics in layered materials.

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