We have investigated the electrochemical deposition of modulated thin films based on the CuxIn2-xSe2 system. CuInSe2 is a leading alternative to silicon for use in thin film photovoltaic solar cells due to its optical absorption and electrical characteristics. Alternating layers of two different compositions based on the CuxIn2-xSe2 system were potentiostatically deposited. These nanometer-scale layers are used to form reduced-dimensionality structures such as superlattices that can be used in concentrator solar cells. We have used X-ray diffraction, energy-dispersive spectroscopy, and scanning tunneling microscopy to characterize our as-deposited thin films. The ability of the scanning tunneling microscope to resolve the individual nanoscale layers of our multilayered thin films is shown and is used to determine modulation wavelengths.