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The exclamation mark next to a title in iTunes means that iTunes cannot locate the song associated with that title (original file cannot be found). The cause for this is an incorrect setting of iTunes preferences when copying iPod songs.
Before copying your iPod songs, setup your iTunes preferences as follows:
Then close down iTunes and start up TouchCopy. Connect your iPod when instructed to do so, select your songs and click on Copy to iTunes.
For more details on how to use TouchCopy please see TouchCopy User Guide.
Also, ensure that you are using the latest version of TouchCopy. You can download this from the TouchCopy download page.