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We report pressure-dependent transient picosecond and continuous-wavephotomodulation studies of disordered and ordered films of2-methoxy-5-(2-ethylhexyloxy) poly(para-phenylenevinylene). Photoinducedabsorption (PA) bands in the disordered film exhibit very weak pressuredependence and are assigned to intrachain excitons and polarons. In contrast,the ordered film exhibits two additional transient PA bands in the midinfraredthat blueshift dramatically with pressure. Based on high-order configurationinteraction calculations we ascribe the PA bands in the ordered film toexcimers. Our work brings insight to the exciton binding energy in orderedfilms versus disordered films and solutions. The reduced exciton binding energyin ordered films is due to new energy states appearing below the continuum bandthreshold of the single strand.

Evidence for Excimer Photoexcitations in an Ordered {\pi}-Conjugated Polymer Film