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Proceedings Paper

Third-order optical nonlinearities and femtosecond responses in metallophthalocyanine thin films made by vacuum deposition, molecular beam epitaxy, and spin coating
Author(s): Tatsuo Wada; Masahiro Hosoda; Anthony F. Garito; Hiroyuki Sasabe; A. Terasaki; Takayoshi Kobayashi; Hiroaki Tada; Atsushi Koma
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Paper Abstract

The molecular design and assembly of metallophthalocyanine systems that have the enhanced macroscopic third-order nonlinear susceptibility (chi) (3)ijkl(-(omega) 4; (omega) 1, (omega) 2, (omega) 3) and show ultrafast responses are described. Enhancement of the third harmonic susceptibility (chi) (3)1111(-3(omega) ; (omega) , (omega) , (omega) ) was observed in vanadyl phthalocyanine vacuum-deposited film with the staggered stacking arrangement induced by thermal treatment. Processable polymeric system based on tert-butyl mono-substituted rich vanadyl phthalocyanine was developed and the favorable staggered stacking arrangement was induced in a polymer matrix to enhance (chi) (3)1111(- 3(omega) ;(omega) ,(omega) ,(omega) ). Femtosecond-time-resolved spectroscopy was performed on vanadyl phthalocyanine thin films with different morphological forms in order to elucidate the exciton dynamics. The exciton decay kinetics consists of three processes: exciton-exciton annihilation, exciton-phonon coupling, and much slower triplet state formation. The decay rate of the exciton population via exciton-exciton annihilation was found to have a time dependence of t-1/2. The vacuum-deposited film and spin-coated film of vanadyl phthalocyanine derivatives showed similar decay behavior, whereas molecular beam epitaxy film showed a faster decay with a time constant of several hundreds of femtoseconds.

Paper Details

Date Published: 1 December 1991
PDF: 10 pages
Proc. SPIE 1560, Nonlinear Optical Properties of Organic Materials IV, (1 December 1991); doi: 10.1117/12.50715
Show Author Affiliations
Tatsuo Wada, RIKEN--The Institute of Physical and Chemical Research (Japan)
Masahiro Hosoda, RIKEN--The Institute of Physical and Chemical Research (Japan)
Anthony F. Garito, RIKEN--The Institute of Physical and Chemical Research (Japan)
Hiroyuki Sasabe, RIKEN--The Institute of Physical and Chemical Research (Japan)
A. Terasaki, Univ. of Tokyo (Japan)
Takayoshi Kobayashi, Univ. of Tokyo (Japan)
Hiroaki Tada, Univ. of Tokyo (Japan)
Atsushi Koma, Univ. of Tokyo (Japan)

Published in SPIE Proceedings Vol. 1560:
Nonlinear Optical Properties of Organic Materials IV
Kenneth D. Singer, Editor(s)

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