Molecular layer deposition (MLD) offers the deposition of ultra-thin and conformal organic or hybrid films which have a wide range of applications. However, some critical potential applications require a very specific set of properties. For application as desiccant layers in water barrier films for example, the films need to exhibit water uptake, swelling and be overcoatable. For application as a backbone for a solid composite electrolyte for lithium ions on the other hand, the films need to be stable against lithium, and need to be transformable from a hybrid MLD film to a porous metal oxide film. Magnesium-based MLD films, called "magnesicone", are promising on both these 1 Page 1 of 51 ACS Paragon Plus Environment Chemistry of Materials aspects and thus an MLD process is developed using Mg(MeCp) 2 as metal source and ethylene glycol (EG) or glycerol (GL) as organic reactants. Saturated growth could be achieved at 2Å/cycle to 3Å/cycle in a wide temperature window from 100 • C to 250 • C. The resulting magnesicone films react with ambient air and exhibit water uptake, which is in the case of the GL-based films associated with swelling (up to 10%) and in the case of EG-based magnesicone with Mg(CO) 3 formation, and are overcoatable with ALD of Al 2 O 3 . Furthermore, by carefully tuning the annealing rate, the EG-grown films can be made porous at 350 • C. Hence, these functional tests demonstrate the potential of magnesicone films as reactive barrier layers and as the porous backbone of lithium ion composite solid electrolytes, making it a promising material for future applications.
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