There are unsynced songs in my library, how do I get them on my device?

We had a problem with this library and had to delete it and open it in a new location.  It works great now, all of the songs appear in the library, they all play on the computer, but they will not sync to an iphone or ipad.  None of them have exclamation points, like before.  I have checked "entire music library" when syncing.  There is plenty of room on both devices.  The sync appears to go fine.  About 70 songs just never move over.  Many of these were itunes downloads, some were uploaded directly into iTunes from a CD.  There is no point in re-downloading them, they appear in the library, just not on a device.
What is going on?
Home computer is Windows 7 professional, always has been.  This is a new problem. iPhone is a 3, but has always synced fine in the past.  iPad is 2nd generation, but same thing, always worked before.

Hold down the option (or alt) key key and launch iPhoto. How many libraries are listed in the resulting window?

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