SIMS probes the first 2 - 3 nm of surfaces and is very effective at characterizing polymer substrates. When combined with X-ray photoelectron spectroscopy you can have a really good idea of what's present on the surface.
I used both approaches a lot in my graduate studies to confirm whether a reaction occur on the surfaces I was studying, albeit, I was mostly looking at inorganic substrates with organic coatings.
However, other graduate students in the group did look at polymeric substrates. As a reference here is a paper (let me know if you need a copy of it):
http://onlinelibrary.wiley.com/doi/10.1002/sia.5352/abstract
Here is another paper that may be useful:
http://surrey.ac.uk/mes/files/Shimizu_paper.pdf
Polymer coatings are first characterized by a) FTIR and then by ToF-SIMS. As the probing for ToF-SIMS is only few nm, sample preparation and atmospheric contamination avoidance is very important. Besides, sims has quantification issues but good for fingerprinting.
The question is, what kind of information you want to get from the polymeric films? What are their thickness? For surface analysis as already discusses TOF SiMS is a good method for characterizing the surface of polyer films. In principle it should also be possible to make depth profiling and follow special elements or molecule fragments as a function of depth. This has already been done e.b. for organic LED and organic electronic devices.
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