Not sure I understand this. Is this a requirement for real-world use? What happens if the outside of the coating isn't atomically flat? What makes this hard to do?
Caveat: For older processes, built on a larger scale (>1 micron), these kinds of details may not matter, in which you are right to question this point. But if you want to implement on cutting edge manufacturing processes, these details absolutely do matter.
To put this in perspective, in cutting edge process nodes, I've seen senior engineers argue bitterly over ~1 nm in a certain critical dimension. That's (roughly) about 5 atoms across, depending on how much you trust the accuracy of the metrology.
So, if ANY layer isn't "flat" (or otherwise to spec within tolerance), the next layer in the semiconductor patterning stack will tend to translate that bumpiness upward, or cause a deformity in adjacent structure. This is (almost) always bad. These defects cause voids, bad electrical/thermal contacts and characteristics, misshapen/displaced structures, etc, etc
Crystallization in thin-film (especially conformal/gap-filling films) is a tough job which many poor PhD students have slaved over. Poly crystalline material is arguably harder to control in some key ways vs mono crystalline, since you don't have direct control the specific crystal grain orientation and growth direction. That is, some grain orientations will grow quickly, and others growing slowly. You can imagine the challenge then of getting the layer to terminate growth without ending up too jagged on the ~nm scale. After that you also get into the fun world of crystal defects, grain size, and deciding if you need to do some more post-processing (do I risk planarizing?)
Hopefully I have captured some of the pieces involved in an understandable way.
Edit: clarity