xvi, 145 p. : ill. (some col.) / The structures of several compounds in the [(PbSe)0.99]m[WSe2]n, [(PbSe)1.00]1[MoSe2]1, and [(SnSe)1.03]1[MoSe2]1 systems were determined using x-ray data. The structural determination using Rietveld methods was complicated by the strong preferred orientation of the samples, which resulted in x-ray diffraction scans with either 00l or hk0 reflections depending on the orientation of the sample in the diffractometer. Rietveld refinements of the [(PbSe)0.99]1[WSe2]1, [(PbSe)1.00]1[MoSe2]1, and [(SnSe)1.03]1[MoSe2]1 samples were compared to single crystal sample refinement results for [(MX)1+d]1[TX2]1, where M is a metal, T is a transition, X is a chalcogen, and d is the misfit parameter. The structural refinement yielded rock salt layer puckering values of 25 pm, 23 pm, and 36 pm for [(PbSe)0.99]1[WSe2]1, [(PbSe)1.00]1[MoSe2]1, and [(SnSe)1.03]1[MoSe2]1, respectively, which are all within the established literature range of 20 pm to 60 pm. The refinement of the hk0 reflections confirmed that the in plane structures were consistent with the dichalcogenide (P63mmc) and rock salt (Fm3m) structure types. Structures for the [(PbSe)0.99]m[WSe2]m isomer series where m = 1 to 5 were determined, and a systematic trend in structure as a function of the thickness of the constituent layers was discovered. The structure of the rock salt constituent was found to distort into pairs, forming alternating long and short distances along the c axis. This distortion decreases as the number of rock salt planes increases from 4 to 6 to 8 and is either absent or nearly so in compounds with a larger number of rock salt planes. The puckering distortion at the interface between the rock salt and the dichalcogenide is also observed in the inner rock salt layers but decreases in magnitude moving away from the rock salt – dichalcogenide interface. Structures of [(PbSe)0.99]m[WSe2]n where m = 1 or 2 and n = 1 or 2 were also determined. The degree of structural distortion is a function of the ratio of rock salt to dichalcogenide layers. This dissertation includes unpublished co-authored material. / Committee in charge: Dr. Thomas R. Dyke, Ph.D., Chairperson; Dr. David C. Johnson, Ph.D., Advisor; Dr. Catherine J. Page, Ph.D., Member; Dr. Andrew H. Marcus, Ph.D., Member; Dr. John L. Hardwick, Ph.D., Member; Dr. Richard Taylor, Ph.D., Outside Member