Computational Investigation of an All-sp(3) Hybridized Superstable Carbon Allotrope with Large Band Gap

对具有大带隙的全sp(3)杂化超稳碳同素异形体的计算研究

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Abstract

Carbon is one of nature's basic elements, hosting a tremendous number of allotropes benefiting from its capacity to generate sp, sp2, and sp3 hybridized carbon-carbon bonds. The exploration of novel carbon architectures has remained a pivotal focus in the fields of condensed matter physics and materials science for an extended period. In this paper, we, by using first-principles calculation, carry on a detailed investigation an an all-sp3 hybridized carbon structure in a 20-atom tetragonal unit cell with P43212 symmetry (D48, space group No. 96), and call it T20 carbon. The equilibrium energy of T20 carbon is -8.881 eV/atom, only 0.137 eV/atom higher than that of diamond, indicating that T20 is a superstable carbon structure. T20 is also a superhard carbon structure with a large Vicker's hardness about 83.5 GPa. The dynamical stability of T20 was verified by means of phonon band spectrum calculations. Meanwhile, its thermal stability up to 1000 K was verified via ab initio molecular dynamics simulations. T20 is an indirect band-gap insulator with approximately 5.80 eV of a band gap. This value is obviously greater than the value in the diamond (5.36 eV). Moreover, the simulated X-ray diffraction pattern of T20 displays a remarkable match with the experimental data found in the milled fullerene soot, evidencing that T20 may be a potential modification discovered in this experimental work. Our work has given a systematical understanding on an all-sp3 hybridized superstable and superhard carbon allotrope with large band gap and provided a very competitive explanation for previous experimental data, which will also provide guidance for upcoming studies in theory and experiment.

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