论文标题

电子 - 音波相互作用对第四组半导体多晶型物的总能量的贡献:评估和含义

Electron-phonon interaction contribution to the total energy of group IV semiconductor polymorphs: evaluation and implications

论文作者

Varma, R. Arjun, Paul, Shilpa, Itale, Anup, Pable, Pranav, Tibrewala, Radhika, Dodal, Samruddhi, Yerunkar, Harshal, Bhaumik, Saurav, Shah, Vaishali, Gururajan, M. P., Prasanna, T. R. S.

论文摘要

在基于密度功能理论(DFT)的总能量研究中,包括范德华(VDW)和零点振动能(ZPVE)校正项,以获得多晶型物之间的能量差异。我们提出并计算了由于电子 - 音波相互作用(EPI)而引起的总能量的新校正项。我们依靠艾伦的一般形式主义,它超出了准谐波近似(QHA),包括由于准粒子相互作用而引起的自由能贡献。我们表明,对于半导体和绝缘子,EPI对电子和声子的自由能的贡献是相应的零点能量贡献。使用艾伦的形式主义的大约版本与EPI校正的Allen-Heine理论结合使用,我们计算了碳,硅和碳化硅的零点EPI校正的零点EPI校正。 EPI校正改变了多型型之间的能量差异。在SIC多型中,EPI校正项比VDW和ZPVE项更敏感,因此对于确定其能量差异至关重要。它清楚地表明,立方SIC-3C是亚稳定的,六边形SIC-4H是稳定的多型。我们的结果与Kleykamp的实验结果一致。我们的研究使得将EPI校正纳入自由能表达中的单独术语。通过包括EPI对所有热力学特性的贡献,这开辟了超越QHA的道路。

In density functional theory (DFT) based total energy studies, the van der Waals (vdW) and zero-point vibrational energy (ZPVE) correction terms are included to obtain energy differences between polymorphs. We propose and compute a new correction term to the total energy, due to electron-phonon interactions (EPI). We rely on Allen's general formalism, which goes beyond the Quasi-Harmonic Approximation (QHA), to include the free energy contributions due to quasiparticle interactions. We show that, for semiconductors and insulators, the EPI contributions to the free energies of electrons and phonons are the corresponding zero-point energy contributions. Using an approximate version of Allen's formalism in combination with the Allen-Heine theory for EPI corrections, we calculate the zero-point EPI corrections to the total energy for cubic and hexagonal polytypes of Carbon, Silicon and Silicon Carbide. The EPI corrections alter the energy differences between polytypes. In SiC polytypes, the EPI correction term is more sensitive to crystal structure than the vdW and ZPVE terms and is thus essential in determining their energy differences. It clearly establishes that the cubic SiC-3C is metastable and hexagonal SiC-4H is the stable polytype. Our results are consistent with the experimental results of Kleykamp. Our study enables the inclusion of EPI corrections as a separate term in the free energy expression. This opens the way to go beyond the QHA by including the contribution of EPI on all thermodynamic properties.

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