A method (100) is provided for synthesizing a thin film electrode (350) such as an electrochromic (EC) electrode (426) or counter electrode (434) for an EC device (410), a lithiated film of transition metal oxide (616) for a battery device (600), or the like. The method (100) includes providing (140) a source material (322) within a deposition chamber (310) such as a target for sputtering, and the source material (322) includes a transition metal oxide and ionic lithium. The method (100) continues with positioning (140) an electrically conductive substrate (340) with an exposed surface within the deposition chamber (310). A thin film (350) of the transition metal oxide and the ionic lithium is deposited upon the exposed surface of the substrate (340) using physical vapor deposition with the source material (322) to form in a single deposition step a layer of lithiated transition metal oxide (350).
 The United States Government has rights in this invention under Contract No. DE-AC36-99GO10337 between the United States Department of Energy and the National Renewable Energy Laboratory, a Division of the Midwest Research Institute.