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The ability to selectively deposit thin films of lithium and remove them from surfaces is an emerging area of technology development in various fields including EUV lithography, lithium ion battery development, and in the fusion community. A lithium magnetron source was developed for lithium deposition and characterized to yield a mapping of the temperature and density of the plasma, ionization fraction, and lithium deposition. From here, a secondary plasma source was developed and studied in the same manner to also provide information on the electron density, temperature, and ionization fraction so as to accurately model and measure the deposition flux of lithium and sputter flux on the sample surface. The simultaneous process of deposition, evaporation, and sputtering of lithium is modeled and corroborated with experimental observations to develop a predictive model for the precise thickness of lithium thin films that can be engineered in any setting for any application.