Magic Carbon Clusters in the Chemical Vapor Deposition Growth of.pdf

ARTICLE /JACS Magic Carbon Clusters in the Chemical Vapor Deposition Growth of Graphene Qinghong Yuan,†,|| Junfeng Gao, †,§,|| Haibo Shu,†,‡,|| Jijun Zhao,* ,§ Xiaoshuang Chen,*,‡ and Feng Ding*,† †Institute of Textile and Clothing, Hong Kong Polytechnic University, Hong Kong, China ‡National Laboratory of Infrared Physics, Shanghai Institute for Technical Physics, Chinese Academy of Sciences, Yu Tian Road 500, Shanghai 200083, China §Key Laboratory of Materials Modification by Laser, Ion and Electron Beams, Dalian University of Technology, Ministry of Education, Dalian 116024, China S Supporting Information b ABSTRACT: Ground-state structures of supported C clusters, CN (N = 16, ..., 26), on four selected transition metal surfaces [Rh(111), Ru(0001), Ni(111), and Cu(111)] are systematically explored by ab initio calculations. It is found that the coreshell structured C21, which is a fraction of C60 possessing three isolated pentagons and C3v symmetry, is a very stable magic cluster on all these metal surfaces. Comparison with experimental scanning tunneling microscopy images, dI/dV curves, and cluster heights proves that C21 is the experimentally observed dominating C precursor in graphene chemical vapor deposition (CVD) growth. The exceptional stability of the C21 cluster is attributed to its high symmetry, coreshell geometry, and strong binding between edge C atoms and the metal surfaces. Besides, the high barrier of two C21 clusters’ dimerization explains its temperature- dependent behavior in graphene CVD growth. 1. INTRODUCTION