Structure-properties relations in graphene derivatives and metamaterials obtained by atomic-scale modeling

ABSTRACT

Recent findings of atomic-scale modelling studies are reviewed on graphene derivatives and metamaterials fabricated through chemical functionalization and/or defect engineering of graphene sheets. Results of molecular-statics and molecular-dynamics simulations according to a reliable bond-order potential, as well as first-principles density functional theory calculations are reviewed that have established useful structure-properties relations in two-dimensional materials, such as graphene nanomeshes (GNMs), electron-irradiated graphene, and interlayer-bonded twisted bilayer graphene. Quantitative relationships are established for the elastic moduli, mechanical properties, and thermal conductivity of GNMs as a function of the nanomesh porosity and the mechanical response of GNMs to uniaxial tensile straining is explored over the range of nanomesh porosities. The dependence of structural, mechanical, and thermal transport properties of electron-irradiated graphene sheets on the density of irradiation-induced defects is reviewed, highlighting an amorphization transition accompanied by a brittle-to-ductile transition and a transition in thermal transport mechanism beyond a critical defect concentration. The tunability of the electronic band structure, mechanical properties, and structural response to mechanical loading of graphene-diamond nanocomposite superstructures consisting of nanodiamond superlattices in interlayer-bonded twisted bilayer graphene also is demonstrated by precise control of the density and distribution of covalent interlayer C–C bonds.

KEYWORDS:

• Graphene nanomeshes
• irradiated graphene
• interlayer-bonded twisted bilayer graphene
• molecular dynamics
• density functional theory

Acknowledgements

The research efforts of our students and postdoctoral researchers, Corinne Carpenter, Lin Hu, Asanka Weerasinghe, Mengxi Chen, Alyne Machado, Augusto Christmann, Spencer Wyant, and Ioanna Fampiou, who conducted most of the computational work reviewed in this article, are gratefully acknowledged. This research was supported by Polymer-Based Materials for Harvesting Solar Energy, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences under Award No. DE-SC0001087; by the U.S. DOE, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award No. DE-FG02-07ER46407; by the National Science Foundation through the University of Massachusetts, Amherst Materials Research Science and Engineering Center (MRSEC) on Polymers under Award No. DMR-0820506; by the Army Research Laboratory under Grant Nos. W911NF-10-2-0098 (Subaward No. 14-215454-020), W911NF-11-2-0014, and W911NF-15-2-0026; and by CNPq through Grant No. 449824/2014-4 (MCTI/CNPQ/UNIVERSAL 14/2014) and by FAPERGS through travel Grant No. 11/3445-5. For the computational work reviewed here, we used the facilities of the Massachusetts Green High-Performance Computing Center (MGHPCC) and of LNCC/SDUMONT and CESUP/UFRGS.

Disclosure statement

No potential conflict of interest was reported by the authors.

ORCID

Dimitrios Maroudas http://orcid.org/0000-0001-9297-8839

Andre R. Muniz http://orcid.org/0000-0002-8784-012X

Ashwin Ramasubramaniam http://orcid.org/0000-0001-6595-7442

Additional information

Funding

This research was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences under [award number DE-SC0001087]; by the U.S. DOE, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under [award number DE-FG02-07ER46407]; by the National Science Foundation through the Materials Research Science and Engineering Center (MRSEC) on Polymers under [award number DMR-0820506]; by the Army Research Laboratory under [grant numbers W911NF-10-2-0098 (subaward number 14-215454-020), W911NF-11-2-0014, and W911NF-15-2-0026]; and by CNPq through [grant number 449824/2014-4 (MCTI/CNPQ/UNIVERSAL 14/2014)] and by FAPERGS through travel [grant number 11/3445-5].