title: Theoretical study of the structures and first hyperpolarizabilities of C60Cl n and Li@C60Cl n (n = 4, 6, 8, 10).
abstract: We recently reported (Song Y-D et al., 2016, J Mol Model 22:50) that doping with Li greatly affects the static first hyperpolarizability of C60Cl2. In this work, with a view to creating nonlinear optical materials with high thermodynamic stability and wide transparent regions, a series of Li@C60Cl n (n = 4, 6, 8, 10) were designed. The structures, electrostatic potentials, electronic structures, absorption spectra, and linear and nonlinear optical properties of C60Cl n and Li@C60Cl n were systematically investigated using density functional theory (DFT) methods. The results of our calculations indicated that the stability of these molecules decreases in the order Li@C60Cl10 > Li@C60Cl8 > Li@C60Cl6 > Li@C60Cl4. It is clear that the number of Cl atoms greatly influences the stability of Li@C60Cl n . Li@C60Cl n showed greater thermodynamic stability than Li@C60Cl2. We also investigated the first hyperpolarizabilities of Li@C60Cl n and found them to be 2973, 3640, 4307, and 2627 au for n = 4, 6, 8, and 10, respectively-higher than that of Li@C60Cl2. Finally, we noted that the transparent region could be modulated by increasing the number of Cl atoms: Li@C60Cl n possess wider transparent regions than that of Li@C60Cl2. We therefore believe that this study has highlighted an effective method for designing nonlinear optical materials with high thermodynamic stability and wide transparent regions.
authors.affiliation: College of Mathematics and Physics, Fujian University of Technology, Fuzhou, Fujian, 350118, People's Republic of China. yaodong909@163.com.cn.
authors.forename: Yao-Dong
authors.initials: YD
authors.lastname: Song
authors.affiliation: School of Humanities, Fujian University of Technology, Fuzhou, Fujian, 350118, People's Republic of China.
authors.forename: Liang
authors.initials: L
authors.lastname: Wang
authors.affiliation: Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, People's Republic of China. liming_wu@fjirsm.ac.cn.
authors.forename: Li-Ming
authors.initials: LM
authors.lastname: Wu
keywords: Absorption spectra; Electronic structures; First hyperpolarizability; Fullerene derivatives