利用密度泛函理论(DFT)方法研究了[Mo6O19]2-修饰的单壁碳纳米管的非线性光学(NLO)性质.结果表明,[ Mo6O19]2-修饰的单壁碳纳米管作为特殊的有机-无机杂化体系,具有显著的二阶非线性光学响应.通过调整[ Mo6O19]2-与纳米管之间的角度,体系的稳定性显示出规律性的变化趋势,且二阶NLO响应发生了变化.对静场二阶极化率(βvec)有主要贡献的电子跃迁特征表明,[ Mo6O19]2-与碳纳米管之间角度的改变影响了分子内的给受体特征.当角度达到30°时,化合物显示出最大的βvec值,此时杂多阴离子簇为电子受体,而碳纳米管为电子给体.此外,在碳纳米管的端位连接电子给体(如氨基)可有效地增大βvec值.%The nonlinear optical ( NLO ) properties of [ Mo6 019 ] 2- decorated single wall carbon nanotubes ( SWCNT) were investigated by density functional theory( DFT). These special organic-inorganic hybrids possess a large second-order NLO response. It is noteworthy that the second-order NLO behavior can be switched by the variable angle between [ Mo6019 ]2- and CNT and the stability of systems shows the regular trends. The characteristic of the charge-transfer transition corresponding to the dominant contributions to the static second-order polarizibility(βvec) values indicates that the variable anchoring angles of [ Mo6019]2- can influence the intramolecular donor or acceptor character. When the anchoring angle of [Mo6O19]2- becomes 30 , the complex exhibits the largest βvec value; besides, the polyoxometalate(POM) cluster acts as the acceptor and the CNT as the donor. Furthermore, the incorporation of an electron donor(the amido group) leads to a larger βvec value at the end of the CNT segment.
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