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The application of neutron interferometry to the measurement of the atom density of polymer thin films (≪1 μm thick) supported on silicon substrates is described. Polymer films were chosen primarily for their fixed, well-defined stoichiometry; however, the technique is applicable to films of any elemental composition. The wavelength-independent phase shift of a beam of thermal neutrons passing through the sample gives a measure of the product of the film atom density, the film thickness, the lattice spacing of the silicon interferometer, and the scattering lengths of the constituent elements of the film. The film thickness was found by x-ray reflectivity while the other two parameters are well-defined quantities. The technique does not rely on complex mathematical modeling of physical processes nor on thin film standards for data interpretation. With some refinements, neutron interferometry is envisioned as an important tool in the creation of thin films having well-defined densities which will be useful in the calibration of many analysis techniques. © 1999 American Institute of Physics.