Near-Unity Quantum Yields for Intersystem Crossing and Singlet Oxygen Generation in Polymethine-like Molecules: Design and Experimental Realization

作者：Webster Scott^*; Peceli Davorin; Hu Honghua; Padilha Lazaro A; Przhonska Olga V; Masunov Artem E; Gerasov Andriy O; Kachkovski Alexey D; Slominsky Yurii L; Tolmachev Alexey I; Kurdyukov Vladimir V; Viniychuk Olexander O; Barrasso Emma; Lepkowicz Richard; Hagan David J; Van Stryland Eric W

来源：Journal of Physical Chemistry Letters, 2010, 1(15): 2354-2360.

DOI：10.1021/jz100381v

The photophysical properties of two pairs of squaraine molecules where two oxygen atoms in a squaraine bridge are replaced with sulfur atoms are investigated. This substitution leads to an inversion of the lowest singlet pi-pi* electronic transition by an n-pi* transition, effectively reducing the energy difference between singlet and triplet states and significantly increasing the intersystem crossing efficiency without the use of "heavy atoms". Experimental results, in agreement with quantum chemical calculations, show near-unity values for triplet quantum yield and singlet oxygen generation quantum yield for sulfur-containing squaraines, which are potentially useful for two-photon photodynamic therapy.

• 出版日期2010-8-5