Three-dimensional acetylenic modified graphene for high-performance optoelectronics and topological materials

Yan Gao,Kai Liu,Shengyuan A. Yang,Chengyong Zhong,Zhong-Yi Lu

doi:10.1038/s41524-021-00579-5

Abstract

Seeking carbon phases with versatile properties is one of the fundamental goals in physics, chemistry, and materials science. Here, based on the first-principles calculations, a family of three-dimensional (3D) graphene networks with abundant and fabulous electronic properties, including rarely reported dipole-allowed truly direct band gap semiconductors with suitable band gaps (1.07–1.87 eV) as optoelectronic/photovoltaic materials and topological nodal-ring semimetals, are proposed through stitching different graphene layers with acetylenic linkages. Remarkably, the optical absorption coefficients in some of those semiconducting carbon allotropes express possibly the highest performance among all of the semiconducting carbon phases known to date. On the other hand, the topological states in those topological nodal-ring semimetals are protected by the time-reversal and spatial symmetry and present nodal rings and nodal helical loops topological patterns. Those newly revealed carbon phases possess low formation energies and excellent thermodynamic stabilities; thus, they not only host a great potential in the application of optoelectronics, photovoltaics, and quantum topological materials etc., but also can be utilized as catalysis, molecule sieves or Li-ion anode materials and so on. Moreover, the approach used here to design novel carbon allotropes may also give more enlightenments to create various carbon phases with different applications.

Highlights

Carbon is one of the central and essential elements in the current scientific research and industrial applications due to its novel properties, i.e., superhardness, exceptional toughness, and the highest thermal conductivity[1,2,3,4,5,6,7]
Elemental carbon exists in two natural allotropes, i.e., diamond and graphite, there are many novel carbon phases that have been manufactured in experiments over the past decades, such as fullerenes, carbon nanotubes, graphene, and so on[8,9]
We propose a new strategy to tailor graphene through stitching graphene layers with acetylenic linkage, as shown in Fig. 1a, b, which here is termed as 3D acetylenic modified graphene (3D-AMG)

Summary

INTRODUCTION

Carbon is one of the central and essential elements in the current scientific research and industrial applications due to its novel properties, i.e., superhardness, exceptional toughness, and the highest thermal conductivity[1,2,3,4,5,6,7]. The family of 3D-AMGs present very abundant and fabulous electronic properties, some of which are dipole-allowed truly direct band gap semiconductors with band gaps in the range of 1.0–1.5 eV, which are located in the optimal band gap value range for photovoltaic application, and possess probably the highest optical absorption strength amongst all of the semiconducting carbon allotropes known to date, between two acetylenic connected carbon dimer (i.e., the cyan atoms). Our soft mode throughout the entire Brillion zone (BZ), implying they work discovers some semiconducting carbon allotropes with are dynamically stable (see Fig. 2a, b) Their AIMD simulations excellent optical absorption strength and some topological nodalring semimetals, the approach used here to design manifest that they can be stable under at least 1000 K (see Fig. 2c–f), showing very excellent thermodynamic stability as well. Novel carbon allotropes through connecting graphene with acetylenic linkage may give more thoughts to create various The electronic and optical properties of 3D-AMGs carbon phases with different applications

Method

DISCUSSION

Findings

METHODS