title: Exploration of the origin of large first hyperpolarizabilities of trisaza-bridged (36) fulleroids.
abstract: We investigate theoretically the structures and second-order nonlinear optical (NLO) responses (first hyperpolarizabilities) of 15 trisaza-bridged (36) fulleroids (series-A) and 15 triborane-bridged (36) fulleroids (series-B). 3A has smaller transition energy and smaller ground state dipole moment, resulting in relatively larger static first hyperpolarizability (10647 au). Most trisaza-bridged (36) fulleroids have larger β values than the corresponding triborane-bridged (36) fulleroids. The f(0) and Δμ remain stable values when substituents R change for series-A except 2A and 5A (for series-B except 5B and 10B) and β values are proportional to ΔE(-3), which implies that the β values for series-A and series-B follow the two-level model. Results demonstrate that a proper bridge and lower transition energy ΔE are more favorable to enlarging first hyperpolarizabilities of series-A and series-B. In addition, the frequency-dependent SHG and EOPE are also estimated and discussed. The current work can stimulate experimentalists to synthesize novel NLO materials designed in this work.
authors.affiliation: State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China.
authors.forename: Lizhi
authors.initials: L
authors.lastname: Jiang
authors.forename: Jingyang
authors.initials: J
authors.lastname: Gu
authors.forename: Xiaolei
authors.initials: X
authors.lastname: Zhu
mesh_terms: D001896:Boron Compounds / Q000737:chemistry*; D002244:Carbon / Q000737:chemistry*; D004583:Electrons; D004735:Energy Transfer; D037741:Fullerenes / Q000737:chemistry*; D008956:Models, Chemical; D008958:Models, Molecular; D036103:Nanotechnology; D055095:Optics and Photonics; D013816:Thermodynamics
chemical_list: D001896:Boron Compounds; D037741:Fullerenes; D002244:Carbon