Density Functional Theory Study on Subtriazaporphyrin Derivatives: Dipolar/Octupolar Contribution to the Second-Order Nonlinear Optical Activity

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• 作者：Lijuan Zhang ; Dongdong Qi ; Luyang Zhao ; Chao Chen ; Yongzhong Bian ; Wenjun Li
• 刊名：The Journal of Physical Chemistry A
• 出版年：2012
• 出版时间：October 18, 2012
• 年：2012
• 卷：116
• 期：41
• 页码：10249-10256
• 全文大小：475K
• 年卷期：v.116,no.41(October 18, 2012)
• ISSN：1520-5215

文摘

Density functional theory calculations have been carried out on the subtriazaporphyrin skeletons, an excellent prototype for investigating the dipolar/octupolar contribution to the second-order nonlinear optical (second-order NLO) activity, revealing the size effect and clarifying the nature of the limit when expanding the conjugated system is employed to improve the hyper-Rayleigh scattering response coefficient (尾_HRS). The octupolar and dipolar contributions are theoretically separated, rendering it possible to control the dipolar/octupolar second-order NLO contribution ratio by changing the number and orientation of the peripheral fused benzene moieties. In addition, both the dispersion and solvent effect were also revealed to lead to the enhancement of 尾_HRS.