Theoretical study on the relationship between spin multiplicity effects and nonlinear optical properties of the pyrrole radical (C4H4N.).
Theoretical study on the relationship between spin multiplicity effects and nonlinear optical properties of the pyrrole radical (C4H4N.).
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DOI：
10.1021/jp073907t
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发表时间：
2008-01
期刊：
影响因子：
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通讯作者：
Y. Qiu;H. Fan;Shiling Sun;Chun-Guan Liu;Z. Su
中科院分区：
文献类型：
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作者：
Y. Qiu;H. Fan;Shiling Sun;Chun-Guan Liu;Z. Su
中性pi共轭C_4H_4N的几何结构和稳定性。用从头算和密度泛函理论(DFT)方法研究了分子的三自旋态。此外，结合有限场方法，在同一水平上研究了薄膜的线性和非线性光学性质。计算结果表明，随自旋多重数的增加，体系的共轭程度和稳定性降低。这些可靠的UCCSD结果表明，C4H4N的极化率(α)值。四重态最大，而C4H4N最大。与二重态是最小的。Betatot值的顺序是Betaextet；betadoublet>；betaQuartet。第二个超极化率(伽马值)显示正值。伽马的变化趋势与α一致。
The geometrical structure and stability of neutral pi-conjugated C4H4N. with three spin states were investigated by using ab initio and density functional theory (DFT) methods. In addition, the linear and nonlinear optical properties were studied at the same level combined with the finite field approach. The calculated results show that conjugation and stability decreased with increasing spin multiplicity. These reliable UCCSD results show that the polarizability (alpha) values of C4H4N. with the quartet state are maximal, while those of C4H4N. with the doublet state are minimal. The order of betatot values is betasextet > betadoublet > betaquartet. The second hyperpolarizability (gamma) values exhibit positive values. The variation trends of gamma are consistent with alpha.