Monolithic
device integration of crystalline complex oxide thin
films can open for smarter and more sustainable devices in electronics
and energy technology. However, the facile integration of such compounds
has so far been incompatible with the present production lines for
electronics. Atomic layer deposition (ALD) is already well-integrated
for the production of amorphous binary oxides in electronics, but
extending the technique to crystalline complex compounds has proved
challenging. Herein, we show how the subcycle arrangement (i.e., the overall order of binary subcycles) plays a crucial
role in the formation and quality of crystalline complex oxides by
ALD, exemplified by the growth of LaNiO3. We show that
an approach somewhere in between the traditional homogeneous and multilayer
approaches provides the best platform for crystalline growth. Based
on these results, we hypothesize that choosing multilayer unit slab
thicknesses close to the interlayer distances in the target crystalline
structure, while still maintaining the correct cation composition,
enhances as-deposited crystallinity and in turn the functional properties.
We believe this approach can be used to extend the toolbox of attainable
crystalline complex oxides by ALD and establish utilization of the
technique for monolithic integration of functional thin films.