Acta Phys. -Chim. Sin. ›› 2011, Vol. 27 ›› Issue (10): 2303-2310.doi: 10.3866/PKU.WHXB20111013

• THEORETICAL AND COMPUTATIONAL CHEMISTRY • Previous Articles     Next Articles

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).

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