Abstract
This paper concerns electrodeposition chemistry in the Cd‐Zn‐Se system. First, the thermodynamics for the cathodic electrosynthesis of 
and 
were analyzed with the aid of Pourbaix diagrams. Strategies for modulating the Cd content and thus the photoresponse of 
alloy thin films were developed. These thin films were analyzed by cyclic photovoltammetry and photocurrent spectroscopy. X‐ray photoelectron spectroscopy provided further confirmation of the alloy composition. Finally a ramp‐hold method was developed for modulating the composition of these 
thin films to generate 
superstructures. These experiments demonstrate the feasibility of securing modulation lengths spanning the submicron regime.