The effect of the extent of electron conjugation on the primary photophysics in semiconducting polymers is reported. A rapid depolarization of photoluminescence and transient absorption, which indicates a reorientation of the transition dipole moment by ϳ30°on a sub-100 fs time scale, is observed in the fully conjugated polymer poly͓2-͑2'-ethylhexyloxy͒-5-methoxy-1,4-phenylenevinylene͔ ͑MEH-PPV͒. In contrast, partially conjugated polymers exhibit a much slower depolarization. The results reveal rapid changes of exciton delocalization in the fully conjugated MEH-PPV driven by structural relaxation.

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