Just One Problem - The Application Can't Be Found

I've successfully moved from a Mac Pro (2,1) to a Mac Mini (6,2), running OS 10.9.5 and iTunes 12.0.1.26. There were several glitches during the move, but I finally associated my iTunes folder, now on an external HD, with the application using the option key during launch method. Everything works, iPhones, iPads, iPods all sync properly, all the playlists are there and play all songs, the App Store and iTunes Store function normally using my single Apple ID.
Just one problem.
When I try to play content from within the iTunes Music [Media] folder, either by double-clicking on a track or by control-click "Open With", I get an error message "The Application Can't be Found".
My iTunes Library goes back to iTunes 3 and contains over 350 GB media. This new behavior is worrying, because I don't understand why moving the iTunes Folder should have caused this. Any ideas will be appreciated.

Thanks for replying.
Yes, from within the iTunes app all behaviors appear normal. I should test if tracks or other media that are not inside the iTunes Library respond the same way.

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Just One Problem - The Application Can't Be Found

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