Abstract

We report that the stimulated Raman gain signals of a single-crystal polydiacetylene with the side groups 2,5-bis-trifluoromethyl-phenyl, PDA-DFMP, exhibit an optical Stark shift of ≈50 cm⁻¹. Using an ultrashort, near-resonant high-intensity laser, we find that the intensity-dependent signal shifts to higher probe photon energies for both the C=C- and C≡C-stretching modes. Semiquantitative agreement between the data and a three-level-system density-matrix calculation is achieved with a nonlinear-optical mechanism in which a pump-laser field is optically coupled to both the exciton ← zero-phonon ground-state and the exciton ← one-phonon ground-state transitions.

© 1994 Optical Society of America

Relaxation dynamics of photoexcitations in polydiacetylenes and polythiophene

Takayoshi Kobayashi, Masayuki Yoshizawa, Uwe Stamm, Makoto Taiji, and Masamitsu Hasegawa
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Ac Stark shifts in a two-zone Raman interaction

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Tahira Nasreen
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Gary M. Carter
J. Opt. Soc. Am. B 4(6) 1018-1024 (1987)