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I believe that iTunes uses DRM and you have to converyt the file and remove the DRM at the same time. Try DVD Catalyst, download the trial version and import the file you want to convert. There is a setting for the thunderbolt under android and then you can convert the file and remove the DRM at the same time. After converting all you have to do is place the video on the root of the SD card, go into the gallery and select it and it should work.
Note: I have not tried this as I do not use iTunes, but dvdCatalyst is a member on the forum and is more than willing to help. Also the trial version will only convert 25% of any given file, to convert the whole source file you will have to buy the full version for $9.95. It is well worth the investment, I already have 2 DVD's converted for use on my Tbolt.