This research, part of the Experimental Physical Chemistry Program, uses laser techniques to explore the electronic structure and intermolecular interactions that determine chemical properties in prototypical organic molecules in the solid state. The data obtained, together with their interpretation using available and developing models, are utilized to understand the chemical properties, dynamics and electronic structures of polyene systems. The results of this research are useful in understanding many technologies varying from optical memories to the molecular basis for vision. Laser-based photochemical hole burning techniques will be utilized to measure 1- and 2-photon spectra and excited state dynamics for well defined polyenes substituted into mixed crystals at liquid helium temperatures. The data obtained will elucidate the fundamental mechanism by which a linear polyene isomerizes in a molecular cavity. In addition to providing new information on cis to trans isomerization, these studies will explain the connection between isomerization and nonbonded interactions between guest and host molecules.