iTunes does have a cache folder, but I think it's only related to the iTunes Store - a bit like a web browser's cache. I wouldn't have thought it's anything to do with the actual media files, but you could try removing this folder and see if that helps....
Home > Library > Caches > com.apple.iTunes (folder)
(NB: if running 10.7 Lion or 10.8 Mountain Lion, the user Library folder is hidden by default - hold down the Alt key and use the "Go" menu to open the Library folder)
Or you could try running OnyX (or similar tool) on your Mac to clear all caches (system and user) - in fact try all the options under the "Automate" tab. OnyX is here...
http://www.titanium.free.fr/download.php(make sure you download the correct edition to match your OS)