We investigated the validity of noninteracting molecular chain theories for fully polymerized polydiacetylene crystals by measuring the two photon absorption spectrum of poly[4,6-dodecadiyn-1,10-diol-bis(n-butoxycarbonylmethylurethane)] chains isolated in their monomer matrix and comparing the results to those obtained previously from polydiacetylene single crystals. Data were taken over 800-940 nm using Z-scan and the measurements were found to be consistent with previously measured results in polydiacetylene single crystal poly[bis(p-toluene sulfonate) of 2,4-hexadiyne-1,6-diol], indicating the validity of the isolated molecule theoretical approach. We also report a low photo-induced polymerization threshold. (C) 2003 American Institute of Physics.