General principles to high-throughput constructing two-dimensional carbon allotropes

doi:10.1088/1674-1056/ab6c4b

中国物理B ›› 2020, Vol. 29 ›› Issue (3): 37306-037306.doi: 10.1088/1674-1056/ab6c4b

• CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES • 上一篇下一篇

General principles to high-throughput constructing two-dimensional carbon allotropes

Qing Xie(谢庆), Lei Wang(王磊), Jiangxu Li(李江旭), Ronghan Li(李荣汉), Xing-Qiu Chen(陈星秋)

1 Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China;
2 University of Chinese Academy of Sciences, Beijing 100049, China;
3 School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China

收稿日期:2019-12-11 修回日期:2020-01-12 出版日期:2020-03-05 发布日期:2020-03-05
通讯作者: Xing-Qiu Chen E-mail:xingqiu.chen@imr.ac.cn
基金资助:
Project supported by the National Science Fund for Distinguished Young Scholars, China (Grant No. 51725103) and the National Natural Science Foundation of China (Grant No. 51671193). All calculations have been performed on the high-performance computational cluster in the Shenyang National University Science and Technology Park.

General principles to high-throughput constructing two-dimensional carbon allotropes

Qing Xie(谢庆)^1,2, Lei Wang(王磊)^1,3, Jiangxu Li(李江旭)^1,3, Ronghan Li(李荣汉)^1,3, Xing-Qiu Chen(陈星秋)¹

1 Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China;
2 University of Chinese Academy of Sciences, Beijing 100049, China;
3 School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China

Received:2019-12-11 Revised:2020-01-12 Online:2020-03-05 Published:2020-03-05
Contact: Xing-Qiu Chen E-mail:xingqiu.chen@imr.ac.cn
Supported by:
Project supported by the National Science Fund for Distinguished Young Scholars, China (Grant No. 51725103) and the National Natural Science Foundation of China (Grant No. 51671193). All calculations have been performed on the high-performance computational cluster in the Shenyang National University Science and Technology Park.

摘要/Abstract

摘要： We propose general principles to construct two-dimensional (2D) single-atom-thick carbon allotropes. They can be viewed as the generalization of patterning Stone-Walse defects (SWDs) by manipulating bond rotation and of patterning inverse SWDs by adding (or removing) carbon pairs on the pristine graphene, respectively. With these principles, numerous 2D allotropes of carbon can be systematically constructed. Using 20 constructed 2D allotropes as prototypical and benchmark examples, besides nicely reproducing all well-known ones, such as pentaheptites, T-graphene, OPGs, etc, we still discover 13 new allotropes. Their structural, thermodynamic, dynamical, and electronic properties are calculated by means of first-principles calculations. All these allotropes are metastable in energy compared with that of graphene and, except for OPG-A and C3-10-H allotropes, the other phonon spectra of 18 selected allotropes are dynamically stable. In particular, the proposed C3-11 allotrope is energetically favorable than graphene when the temperature is increased up to 1043 K according to the derived free energies. The electronic band structures demonstrate that (i) the C3-8 allotrope is a semiconductor with an indirect DFT band gap of 1.04 eV, (ii) another unusual allotrope is C3-12 which exhibits a highly flat band just crossing the Fermi level, (iii) four allotropes are Dirac semimetals with the appearance of Dirac cones at the Fermi level in the lattices without hexagonal symmetry, and (vi) without the spin-orbit coupling (SOC) effect, the hexagonal C3-11 allotrope exhibits two Dirac cones at K and K' points in its Brillouin zone in similarity with graphene.

关键词: graphene allotropes, phonon spectra, semimetal, dirac Fermions, modeling

Abstract: We propose general principles to construct two-dimensional (2D) single-atom-thick carbon allotropes. They can be viewed as the generalization of patterning Stone-Walse defects (SWDs) by manipulating bond rotation and of patterning inverse SWDs by adding (or removing) carbon pairs on the pristine graphene, respectively. With these principles, numerous 2D allotropes of carbon can be systematically constructed. Using 20 constructed 2D allotropes as prototypical and benchmark examples, besides nicely reproducing all well-known ones, such as pentaheptites, T-graphene, OPGs, etc, we still discover 13 new allotropes. Their structural, thermodynamic, dynamical, and electronic properties are calculated by means of first-principles calculations. All these allotropes are metastable in energy compared with that of graphene and, except for OPG-A and C3-10-H allotropes, the other phonon spectra of 18 selected allotropes are dynamically stable. In particular, the proposed C3-11 allotrope is energetically favorable than graphene when the temperature is increased up to 1043 K according to the derived free energies. The electronic band structures demonstrate that (i) the C3-8 allotrope is a semiconductor with an indirect DFT band gap of 1.04 eV, (ii) another unusual allotrope is C3-12 which exhibits a highly flat band just crossing the Fermi level, (iii) four allotropes are Dirac semimetals with the appearance of Dirac cones at the Fermi level in the lattices without hexagonal symmetry, and (vi) without the spin-orbit coupling (SOC) effect, the hexagonal C3-11 allotrope exhibits two Dirac cones at K and K' points in its Brillouin zone in similarity with graphene.

Key words: graphene allotropes, phonon spectra, semimetal, dirac Fermions, modeling

中图分类号: (Surface states, band structure, electron density of states)

73.20.At

63.22.Np (Layered systems) 73.22.Pr (Electronic structure of graphene)

谢庆, 王磊, 李江旭, 李荣汉, 陈星秋. General principles to high-throughput constructing two-dimensional carbon allotropes[J]. 中国物理B, 2020, 29(3): 37306-037306.

Qing Xie(谢庆), Lei Wang(王磊), Jiangxu Li(李江旭), Ronghan Li(李荣汉), Xing-Qiu Chen(陈星秋). General principles to high-throughput constructing two-dimensional carbon allotropes[J]. Chin. Phys. B, 2020, 29(3): 37306-037306.

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General principles to high-throughput constructing two-dimensional carbon allotropes

General principles to high-throughput constructing two-dimensional carbon allotropes

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