Hi Matt and welcome.
This sounds very much like your PC is not imaging either hard disk correctly given the large 250GB won't boot at all and the 4GB goes to a white screen. This sometimes happens on *some* PC's and my suggestion would be to try a completely different PC if possible. Another thing to try if you already have not done so is image to HDC, that is make the hard disk Master and put it on the secondary IDE port.
You will not be looking for, or needing to, unlock the hard disk as the TiVo will not lock these type of hard disks. You will know if it is locked or not anyway because your PC BIOS will report it as substantially less than what it really is, generally 9MB or thereabouts.
No you cannot boot a TiVo hard disk in anything other than a TiVo.
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