物理化学学报 >> 2011, Vol. 27 >> Issue (10): 2303-2310.doi: 10.3866/PKU.WHXB20111013

理论与计算化学 上一篇    下一篇

二吡唑铝化合物双光子吸收性质的理论研究

刘晓婷1, 郭景富2, 安迪3, 王丹1, 任爱民1, 封继康1   

  1. 1. 吉林大学理论化学研究所, 理论化学计算国家重点实验室, 长春 130023;
    2. 东北师范大学物理学院, 长春 130024;
    3. 吉林大学电子科学与工程学院, 长春 130023
  • 收稿日期:2011-05-05 修回日期:2011-06-29 发布日期:2011-09-27
  • 通讯作者: 任爱民 E-mail:aimin_ren@yahoo.com
  • 基金资助:

    国家自然科学基金(20673045, 20973078), 留学回国人员启动基金(外交司留(2008)890 号)和国家重点基础研究发展计划项目(973)(2002CBN613406)资助

Theoretical Study on the Two-Photon Absorption Properties of Pyrazole Aluminum Compounds

LIU Xiao-Ting1, GUO Jing-Fu2, AN Di3, WANG Dan1, REN Ai-Min1, FENG Ji-Kang1   

  1. 1. State Key Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, Jilin University, Changchun 130023, P. R. China;
    2. School of Physics, Northeast Normal University, Changchun 130024, P. R. China;
    3. College of Electronic Science and Engineering, Jilin University, Changchun 130023, P. R. China
  • Received:2011-05-05 Revised:2011-06-29 Published:2011-09-27
  • Contact: REN Ai-Min E-mail:aimin_ren@yahoo.com
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20973078, 20673045), Start Found for Returned Overseas People, China ((2008)890) and National Key Basic Research Program of China (973) (2002CBN613406).

摘要: 应用密度泛函理论(DFT)和半经验的ZINDO方法对二吡唑铝化合物的单、双光子吸收(OPA、TPA)性质进行了研究. 结果表明, 铝氮烷杂环化合物具有好的双光子吸收性质, 其双光子最大吸收截面值(δmax)可达到2860.1 GM (1 GM=10-50 cm4·s·photon-1). 在中心、共轭桥和末端引入强的吸电子基团可调谐单、双光子吸收光谱, 实现在不同波长范围的双光子吸收; 利用三态公式分析了分子的双光子吸收截面变化的内在原因; 铝氮烷杂环化合物与其相应的硼化合物相比, 表现出类似的单、双光子吸收性质, 但一定程度上可增大双光子吸收截面.

关键词: 密度泛函理论, 双光子吸收, 双光子吸收截面, 二吡唑铝, 分子内电荷转移

Abstract: An extensive series of pyrazole aluminum compounds containing an Al2N4 center as a pseudoconjugated system were theoretically investigated for their one-photon absorption and two-photon absorption (OPA and TPA) properties by density functional theory (DFT) and Zerner's intermediate neglect of differential overlap (ZINDO) methods. The results indicate that pyrazole aluminum compounds are good TPA materials and that the TPA maximal absorption cross-section (δmax) can reach 2860.1 GM (1 GM=10-50 cm4·s·photon-1). By incorporating electron-acceptors in the central core, a π-conjugated bridge and terminal groups, the OPA and TPA properties can be modulated. This research provides strategies for the enhancement of molecular TPA in the target region. The origin of the large δmax of some of the studied molecules was determined using a three-level energy model. We conclude that an increase in the intramolecular charge transfer can enhance δmax. Moreover, the pyrazole aluminum compounds behave in a similar manner to pyrazabole chromophores in terms of linear optical, and TPA properties and they possess an increased δmax to some extent.

Key words: Density functional theory, Two-photon absorption, Two-photon absorption cross-section, Pyrazole aluminum, Intramolecular charge transfer

MSC2000: 

  • O641