title: Effect of cage charges on multiphoton absorptions: first-principles study on metallofullerenes Sc(2)C(2)@C(68) and Sc(3)N@C(68).
abstract: A combined method of the time-dependent density functional theory (TDDFT) and sum-overstate (SOS) formula was implemented to model multiphoton absorption spectra, including two-photon absorption (2PA) and three-photon absorption (3PA), of Sc(2)C(2)@C(68) and Sc(3)N@C(68) endohedral metallofullerenes (EMFs). This method has been proved to be effective by comparisons between the calculated and experimental results of trans-4,4'-bis[diphenylamino]stilbene. It was found that the multiphoton absorption cross sections were larger for Sc(2)C(2)@C(68) than that of Sc(3)N@C(68). The electronic origin of multiphoton absorption has been identified with respect to the molecular orbitals involved in charge transfer process. It shows that the increase of pi-charges on the cage of C(68) results in a large multiphoton absorption cross section in EMFs.
authors.affiliation: State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, People's Republic of China.
authors.forename: W-D
authors.initials: WD
authors.lastname: Cheng
authors.forename: H
authors.initials: H
authors.lastname: Hu
authors.forename: D-S
authors.initials: DS
authors.lastname: Wu
authors.forename: J-Y
authors.initials: JY
authors.lastname: Wang
authors.forename: S-P
authors.initials: SP
authors.lastname: Huang
authors.forename: Z
authors.initials: Z
authors.lastname: Xe
authors.forename: H
authors.initials: H
authors.lastname: Zhang
mesh_terms: D000042:Absorption; D004583:Electrons; D037741:Fullerenes / Q000737:chemistry*; D008670:Metals / Q000737:chemistry*; D008958:Models, Molecular; D008968:Molecular Conformation; D017785:Photons; D011789:Quantum Theory; D012680:Sensitivity and Specificity; D012984:Software; D013997:Time Factors
chemical_list: D037741:Fullerenes; D008670:Metals