Structural transformations of graphene exposed to nitrogen plasma: quantum chemical molecular dynamics simulations

Abstract

Non-equilbrium quantum chemical molecular dynamics simulations of graphene nitrogenation in plasma reveal the importance of cooperative nitrogen rearrangements.

Exploring reactivity and product formation in N(4S) collisions with pristine and defected graphene with direct dynamics simulations

“…Some of the motifs have been reported in a recent simulation of N collisions with graphene. 27 These surface species underscore the wide range of bonding the nitrogen can have with the carbon surface. The ultimate fate of these species was not explored in the current study because of the long simulation time required.…”

“…PLEASE CITE THIS ARTICLE AS DOI:10.1063/5.0028253 a graphene surface. 27 In our calculations, the third-order correction 31,32 was utilized with the 3ob-3-1 Slater-Koster parameter set 33 and the Lennard-Jones (LJ) dispersion model. 34 Because of the semi-empirical nature of the SCC-DFTB method, it is important to assess its accuracy and reliability in describing the systems of our interest.…”

“…The only exception was a recent direct dynamics simulation, in which up to 100 N atoms were directed to a pristine graphene sheet in order to understand nitrogen doping resulting from nitrogen plasma exposure. 27 With incident energies of 23, 46, and 92 kcal/mol, atomic nitrogen was found to react with the graphene sheet and release various molecular species including N2, CN, CN2, and C2N2. These incident energies are higher than desired for modeling TPS chemistry.…”

Direct Dynamics Simulations of Hyperthermal O(3P) Collisions with Pristine, Defected, Oxygenated, and Nitridated Graphene Surfaces

“…In the DD approach, the energies and forces are computed on the fly, thus avoiding the construction of analytical PESs. This is particularly advantageous for high-dimensional reactive systems, as the development of an analytical PES with multiple reactive channels can be challenging. − This DD approach has been successfully used in many chemical dynamics studies, including atom scattering from graphene/graphite surfaces. ,,,,, In our recent publication, this method was applied to the scattering of hyperthermal N­( 4 S) on pristine and modified model graphene surfaces . As in previous studies, , the HOPG surface was modeled as periacene (5 a ,6 z ), as shown in Figure .…”

Elucidating the Mechanism of Nitrogen Doping in Graphene Oxide: Structural Evolution of Dopants and the Role of Oxygen

“…Degradation steps can be predicted, but the absorption of these dopants into graphene is not known. Defects and oxygen functionalities are predicted to play a significant role, and certain DFT studies have tried to uncover reaction dynamics on particular carbon defects and oxygen functionalities using ammonia as a source. − Although some insight is shown in these studies, DFT studies are limited due to high computational costs. These cannot provide a dynamics of the binding process, and complicated systems like GO cannot be studied.…”