Multi-radical ground state and magnetism of neutral, charged and chemically modified zigzag edged graphene nanopatches

Michael R Philpott
Center for Computational Materials Science, Institute of Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, 980-8577 Sendai, Japan
Visiting Scholar, Pitzer Theory Center, Department of Chemistry, UC Berkeley, CA 94720-1460, USA

Lundi 20 septembre 2010,
11h00 Salle RAPHAEL 2&3
site d Ivry-sur-Seine


All valence electron density functional theory (DFT) calculations of large compact polycyclic aromatic hydrocarbon (PAH) molecules predict an interior that approximates graphene (single sheet of graphite) [1-6]. In high symmetry molecules the graphene core relegates spin and edge vs. interior geometry changes to the outer (about 2) carbon rows. For example, the ground state of the zigzag edged hexagonal shaped PAH with formula C600H60 (hex 10-zzg) is predicted to be a singlet hexa-radical with one spin associated with each of six sectors. Evidence comes from: (i) singlet ground state, triplet and higher spin states of the series C6m**2H6m (m = 2, 3, 4, .. 10; hex m-zzg); (ii) charged and/or chemically modified hex 9-zzg and 10-zzg systems; (iii) comparisons with the linear acenes C4m+2H2m+4 (m = 9, 10) that have similar edges but no graphene interior. The spin patterns, calculated for these hex m-zzg molecules, provide guidance in predicting the magnetism of arbitrary graphene nanopatches. Calculations were performed on the CCMS-IMR Supercomputer.

References:
1) M.R.Philpott, F.Cimpoesu,Y.Kawazoe, Mat.Trans. (Jpn) 49, 2448(2008)
2) M.R.Philpott, F.Cimpoesu, Y.Kawazoe, Chem. Phys.354, 1(2008)
3) M.R.Philpott, Y.Kawazoe, Chem.Phys.358, 85(2009)
4) M.R.Philpott, Y.Kawazoe, Phys. Rev. B 79, 233303(2009)
5) M.R.Philpott, Y. Kawazoe, J.Chem.Phys.131,0214706(2009)
6) M.R.Philpott, S.Vukovic,Y.Kawazoe, W.A.Lester Jr, J.Chem.Phys.133,044708(2010)