The structure of indium phosphide surfaces and interfaces has been investigated during the growth of nanomaterials by metalorganic chemical vapor deposition. In the phosphorus-rich environment of the MOCVD process, the InP (001) surface forms a (2x1) reconstruction that is terminated with a monolayer of phosphorus dimers. Each of these dimers is stabilized by the adsorption of hydrogen onto one of the dangling bonds. Upon switching from the growth of InP to InGaAs or InSb, the surface can change dramatically depending on the interactions among the group V elements. When InP is exposed to tertiarybutylarsine above 500 °C, arsenic atoms diffuse into the bulk, creating strained InAsP films with a roughness exceeding 1.0 nm. By contrast, when InP is exposed to trimethylantimony between 450 and 600 °C, a thin layer of InSb, ~6.8 Å thick, is deposited. This layer is strained in only one direction, and forms an interesting one-dimensional, ridge-shaped structure.