Abstract
The strong phonon coupling to the one- photon excitonic band is well known to produce the so-called phonon-mediated optical nonlinearity (PMON) in poly-diacetylene toluene sulfonate (PTS),1-3 Indeed, the linear absorption spectrum of this onedimensional electronic structure shows strong vibronic subbands that are, in principle, forbidden unless an anharmonicity of the electronic potential induces a Frank - Condon (F-C) displacement of the one-photon excited state (Fig. 1). On the other hand, until recently little was known about the location and strength of the theoretically predicted two-photon bands of such an inherently symmetric molecular system. The latter transitions are at the origin of the very large optical Kerr response observed within the optical gap of PTS. Also, nothing is known about the phonon (vibrational) coupling to the two-photon transitions.4·5 It is therefore important to understand and properly assign such two-photon bands. Here, we intend to assign the strongest two-photon allowed transition located above the one-photon excitonic band.
© 1995 Optical Society of America
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