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Published October 7, 2010 | Supplemental Material + Published
Journal Article Open

Quantum mechanics based force field for carbon (QMFF-Cx) validated to reproduce the mechanical and thermodynamics properties of graphite

Abstract

As assemblies of graphene sheets, carbon nanotubes, and fullerenes become components of new nanotechnologies, it is important to be able to predict the structures and properties of these systems. A problem has been that the level of quantum mechanics practical for such systems (density functional theory at the PBE level) cannot describe the London dispersion forces responsible for interaction of the graphene planes (thus graphite falls apart into graphene sheets). To provide a basis for describing these London interactions, we derive the quantum mechanics based force field for carbon (QMFF-Cx) by fitting to results from density functional theory calculations at the M06-2X level, which demonstrates accuracies for a broad class of molecules at short and medium range intermolecular distances. We carried out calculations on the dehydrogenated coronene (C24) dimer, emphasizing two geometries: parallel-displaced X (close to the observed structure in graphite crystal) and PD-Y (the lowest energy transition state for sliding graphene sheets with respect to each other). A third, eclipsed geometry is calculated to be much higher in energy. The QMFF-Cx force field leads to accurate predictions of available experimental mechanical and thermodynamics data of graphite (lattice vibrations, elastic constants, Poisson ratios, lattice modes, phonon dispersion curves, specific heat, and thermal expansion). This validates the use of M06-2X as a practical method for development of new first principles based generations of QMFF force fields.

Additional Information

© 2010 American Institute of Physics. Received 5 April 2010; accepted 2 June 2010; published online 6 October 2010. This research was partially supported by the Functional Engineered Nano Architects (FENA) via the Microelectronics Advanced Research Corporation (MARCO) with the prime award (2009–NT-2048) at UCLA (PI Kang Wang). T.A.P. thanks the National Science Foundation and the U.S. Department of Energy (CSGF) for graduate fellowships. W. A. G. acknowledges the WCU program at the Korea Advanced Institute of Science and Technology (KAIST) for additional support.

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Published - Pascal2010p11717J_Chem_Phys.pdf

Supplemental Material - qmff-cx_sm.pdf

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